Photoelectric device, preparation method, power utilization device and power generation device

Abstract

The invention relates to a photoelectric device, a preparation method, a power utilization device and a power generation device. The photoelectric device comprises a perovskite layer, wherein the perovskite layer comprises a Pb element and an I element; the perovskite layer is provided with a first surface and a second surface which are deviated from each other in the thickness direction; the perovskite layer comprises a first area located near the first surface and a second area located at the bulk phase part of the perovskite layer, the first area is located between the first surface and the second area, the binding energy of Pb < 2 + > 4f orbital electrons in the first area is recorded as J1, and the binding energy of Pb < 2 + > 4f orbital electrons in the second area is recorded as J2; the binding energy of the I-3d orbital electrons in the first region is recorded as J3, and the binding energy of the I-3d orbital electrons in the second region is recorded as J4; wherein the perovskite layer meets the conditions that J1-J2 is greater than or equal to 0.15 eV and J4-J3 is greater than or equal to 0.15 eV. The photoelectric device has relatively high photoelectric conversion efficiency.

Description

Technical Field

[0001] This application relates to the field of optoelectronic device technology, and further to optoelectronic devices, preparation methods, electrical devices, and power generation devices. Background Technology

[0002] Optoelectronic devices are a class of devices that utilize photoelectric conversion mechanisms to perform photoelectric conversion. They can convert light energy into electrical energy for use in photovoltaics, or electrical energy into light energy for use in displays, lighting, and other fields. Accordingly, optoelectronic devices can be either photovoltaic devices or light-emitting devices. Taking photovoltaic devices as an example, as a highly efficient device that directly converts solar energy into electrical energy, they have been widely used in many fields. For instance, they are widely used on the rooftops of residential, commercial, and industrial buildings to form distributed photovoltaic power generation systems, or combined with energy storage devices for off-grid power systems, or integrated into portable electronic devices to provide power support for outdoor scenarios.

[0003] The core functional layer for photoelectric conversion in photovoltaic devices is the light-absorbing layer. Representative photovoltaic devices include crystalline silicon solar cells and perovskite solar cells. In perovskite solar cells, the light-absorbing layer is a perovskite layer containing perovskite material. Due to their high conversion efficiency and the ability to be fabricated using low-cost solution methods, perovskite solar cells have attracted widespread attention from the industry. Photoelectric conversion efficiency is crucial for the practical application of perovskite solar cells. Therefore, researching ways to improve the energy conversion efficiency of photovoltaic devices is of great significance. Summary of the Invention

[0004] According to various embodiments and examples of this application, this application provides an optoelectronic device, a fabrication method, an electrical device, and a power generation device. The optoelectronic device exhibits high energy conversion efficiency.

[0005] In some embodiments of the first aspect of this application, an optoelectronic device is provided, including a perovskite layer comprising a first perovskite material containing lead and iodine; the thickness direction of the perovskite layer is denoted as the Z direction; the perovskite layer has a first surface and a second surface that are opposite to each other in the Z direction;

[0006] There exists a first region with a thickness of 5nm to 10nm extending 20nm from the first surface along the Z direction toward the interior of the perovskite layer;

[0007] The thickness of the perovskite layer is denoted as H0; a second region with a thickness of 5nm to 10nm exists within a range extending (1 / 2)·H0 from the perovskite layer toward the first surface and the second surface, respectively, by (1 / 40)·H0; the first region is located between the first surface and the second region;

[0008] Pb of lead in the first region 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+ The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region - The binding energy of the 3d orbital electrons is denoted as J3, and the I of the iodine element in the second region is... - The binding energy of 3d orbital electrons is denoted as J4;

[0009] The perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

[0010] The perovskite material (denoted as the first perovskite material) in the perovskite layer of this optoelectronic device contains lead (Pb) and iodine (I) elements. Furthermore, the perovskite layer includes a first region located near one side of the surface and a second region located in the bulk phase of the perovskite layer, further controlling the Pb content of the lead element within the first region. 2+ The binding energy of the 4f orbital electrons shifts to a higher binding energy direction relative to the second region by a certain amount (e.g., J1-J2≥0.15eV), while the I-energy of iodine in the first region... - The binding energy of 3d orbital electrons shifts to a lower binding energy direction relative to the second region by a certain margin (e.g., J4-J3≥0.15eV). At this time, the valence state of lead in the first region is relatively closer to +2, and the valence state of iodine is relatively closer to -1. This is more conducive to the formation of a more stable crystal structure in the first region of the perovskite layer, reducing the distortion of the crystal structure caused by the binding energy shift of Pb or I elements in the perovskite material, and reducing lead or iodine vacancy defects. This alleviates the defects in the first region caused by excessive dangling bonds and uneven crystallization near the surface of the perovskite layer, thereby reducing the probability of nonradiative recombination of charge carriers in the first region and thus improving the overall energy conversion efficiency of optoelectronic devices.

[0011] It's understandable that I don't want to be limited to the above theories.

[0012] In some embodiments of this application, the perovskite layer satisfies one or more of the following characteristics:

[0013] (t1) 0.15 eV ≤ J1-J2 ≤ 0.3 eV, optionally, 0.16 eV ≤ J1-J2 ≤ 0.28 eV, further optionally, 0.20 eV ≤ J1-J2 ≤ 0.25 eV;

[0014] (t2) 0.15 eV ≤ J4-J3 ≤ 0.45 eV, optionally, 0.20 eV ≤ J4-J3 ≤ 0.45 eV, further optionally, 0.35 eV ≤ J4-J3 ≤ 0.42 eV.

[0015] By controlling J1-J2 within the aforementioned range, it is possible to regulate the formation of a more stable lattice structure in the first region, thereby reducing the defects of lead vacancies in the perovskite layer. It is also beneficial to better avoid excessive electron cloud shift of Pb elements, thereby reducing the significant distortion caused by excessive changes in charge distribution in the perovskite lattice and the resulting introduction of lattice stress suppression.

[0016] By controlling J4-J3 within the aforementioned range, it is possible to regulate the formation of a more stable lattice structure in the first region, thereby reducing the defects of iodine vacancies in the perovskite layer. It is also beneficial to better avoid excessive electron cloud shift of element I, thereby reducing the significant distortion caused by excessive changes in charge distribution in the perovskite lattice and the resulting introduction of lattice stress.

[0017] In some embodiments of this application, the perovskite layer satisfies one or more of the following characteristics: within the domain:

[0018] (z1) J2 is 138 eV~139 eV;

[0019] (z2)J4 is 619 eV~620 eV.

[0020] At this point, by controlling the Pb content of lead in the second region... 2+ The binding energy of the 4f orbital electrons and / or the I of iodine - The binding energy of 3d orbital electrons can regulate the valence distribution of lead and iodine in the perovskite bulk phase, placing them near +2 and -1 valences. This allows for overall regulation of the perovskite crystal structure within the perovskite layer, resulting in a more stable lattice structure and improving the long-term stability of optoelectronic devices.

[0021] In some embodiments of this application, the first perovskite material further includes bromine; the Br content of bromine in the first region... - Let J5 be the binding energy of the 3d orbital electrons, and let Br be the Br of bromine in the second region. - The binding energy of 3d orbital electrons is denoted as J6; where J6-J5>0eV.

[0022] When the perovskite layer includes lead, iodine and bromine, it can leverage the advantages of high crystallinity and high device efficiency of lead-containing perovskite, as well as the advantages of bromine in regulating crystallization and improving band gap.

[0023] Furthermore, by using the Br element of bromine in the first region... - The binding energy of 3d orbital electrons shifts towards lower binding energy relative to the second region, which helps to bring the valence state of bromine in the first region closer to -1, making the lattice structure of bromine-containing perovskite crystals more stable and helping to reduce defects such as halogen vacancies.

[0024] In some of these embodiments, 0.2 eV ≤ J6-J5 ≤ 0.5 eV. In this case, the Br₂ of bromine in the first region is... - The shift of the binding energy of 3d orbital electrons relative to the second region towards lower binding energy is beneficial for bringing the valence state of bromine in the first region closer to -1, making the lattice structure of bromine-containing perovskite crystals more stable, reducing defects such as halogen vacancies, further controlling the shift range within the aforementioned range, and also helping to better avoid significant lattice distortion and the introduction of lattice stress.

[0025] In some embodiments of this application, 0.28 eV ≤ J6-J5 ≤ 0.5 eV, and optionally, 0.35 eV ≤ J6-J5 ≤ 0.46 eV. In this case, by using the Br₂ of bromine in the first region... - The movement of the binding energy of 3d orbital electrons relative to the second region is within the aforementioned range, which is beneficial not only for effectively reducing defects such as halogen vacancies, but also for avoiding significant lattice distortion and the resulting introduction of lattice stress.

[0026] In some embodiments of this application, the thickness of the perovskite layer is 200 nm to 1500 nm, and optionally 400 nm to 1000 nm. The aforementioned modulation of the binding energy of Pb and I can effectively avoid interface defects and the resulting energy level pinning even when the perovskite layer has a large thickness, achieving effective interface charge transport and thus improving the energy conversion efficiency of optoelectronic devices with thicker perovskite layers.

[0027] In some embodiments of this application, the perovskite layer satisfies one or more of the following characteristics in a direction perpendicular to the thickness of the perovskite layer:

[0028] (a1) The Moran index of J1-J2 is less than or equal to 0.2, and optionally less than or equal to 0.15;

[0029] (a2) The Moran index of J4-J3 is less than or equal to 0.2, and optionally less than or equal to 0.15;

[0030] (a3) The perovskite layer includes bromine; the Br content of bromine in the first region... - The binding energy of 3d orbital electrons is denoted as J5, and the Br in the second region is... - The binding energy of the 3d orbital electron is denoted as J6; wherein the Moran index of J6-J5 is less than or equal to 0.25, and optionally less than or equal to 0.15.

[0031] By controlling one or more of the aforementioned parameters within the range of the Moran index in the direction perpendicular to the thickness of the perovskite layer, it is beneficial to achieve more uniform in-plane control of the aforementioned binding energy shift vector, which is beneficial to better improve energy conversion efficiency and device stability.

[0032] In some embodiments of this application, the Moran index of the potential distribution of the first surface is less than or equal to 0.2, and optionally less than or equal to 0.12; wherein the potential of the first surface is obtained by measuring the potential of the first surface using a Kelvin atomic force microscope.

[0033] By controlling the potential distribution of the first surface within the aforementioned range, a more uniform potential distribution can be achieved, which in turn facilitates more uniform and efficient extraction of charge at the perovskite interface, thus improving energy conversion efficiency. Furthermore, it also helps improve charge transport stability at the perovskite interface, thereby enhancing device stability.

[0034] In some embodiments of this application, the band gap of the perovskite layer is 1.2 eV to 2.2 eV.

[0035] The aforementioned binding energy modulation method can be universally applied to a wide range of perovskite layer band gaps. When the band gap of the perovskite layer is within the above-mentioned range, it is beneficial to achieve higher perovskite crystal quality, thereby improving energy conversion efficiency. When the band gap of the perovskite layer is narrower or wider, the aforementioned binding energy modulation method can better compensate for the adverse effects of decreased crystal quality and increased surface defect concentration on energy efficiency.

[0036] In some embodiments of this application, the perovskite layer includes a first additive located in a region of the perovskite layer near the first surface; the first additive is an organic material.

[0037] Optionally, the first additive comprises at least one of a hydrocarbon halide amine or its corresponding salt, a heteroaryl Lewis base, a polar polymer, polystyrene, and polyethylene glycol, wherein the polar polymer contains a polar group located on its side chain, and the polar group includes a carboxylic acid C. 1-4 One or more of alkyl esters and cyano groups;

[0038] Further optionally, the first additive includes C 6-20 The alkyl halogenated amine, wherein the halogen in the alkyl halogenated amine or its corresponding salt includes at least one of chlorine, bromine, and iodine; the heteroaryl Lewis base contains at least one of a pyridine ring and a thiophene ring; and the polar polymer includes polymethacrylic acid C. 1-3 Alkyl esters, polyacrylic acid C 1-3 One or more of alkyl esters and polyacrylonitrile.

[0039] By introducing the aforementioned type of first additive into the region near the first surface (e.g., the first region can be controlled to contain the first additive), the electron-donating and / or electron-withdrawing groups in the first additive can occupy the charge curve in the perovskite crystal. For example, they can occupy positively charged defects such as iodine vacancies, and negatively charged defects such as lead vacancies. Through the interaction between the first additive and the perovskite defects in the region near the first surface, the Pb at the perovskite layer interface can be better controlled. 2+ The sum of 4f orbital electrons and I - The binding energy shift vector of 3d orbital electrons can passivate various defects and improve energy conversion efficiency. In addition, it can help avoid significant lattice distortion and the resulting lattice stress, thus enabling long-term and effective passivation of interface defects and improving device stability.

[0040] In some embodiments of this application, the first additive comprises a hydrocarbon-based haloamine or its corresponding salt, and the perovskite layer satisfies any one of the following characteristics:

[0041] (i) The halogen in the alkyl halogenated amine or its corresponding salt includes one or more of chlorine and bromine;

[0042] At this point, the aforementioned first type of additive is beneficial for better passivation of defects while controlling the lattice to avoid significant distortion, thereby improving energy conversion efficiency and device stability.

[0043] Optionally, the second surface is used for light incident, and the first surface is used for electron transport. In this case, hydrocarbon halide amines or their corresponding salts are beneficial for passivation doping with chlorine (Cl) and bromine (Br) elements to regulate the energy level structure at the interface of the first surface, so that the adjacent functions of the perovskite layer and the first surface side have better energy level matching, thereby improving the ability of the interface to transport electrons, which is beneficial to improving the ability of the interface at the first surface to collect photogenerated carriers (electrons) near the second surface, and thus improving the photoelectric conversion efficiency.

[0044] (ii) The halogen in the alkyl halogenated amine or its corresponding salt includes iodine;

[0045] Optionally, the second surface is used for light incident, and the first surface is used for hole transport. In this case, hydrocarbon-based haloamines or their corresponding salts are beneficial for passivation doping with iodine (I) to regulate the energy level structure at the interface of the first surface, so that the adjacent functions of the perovskite layer and the first surface side have better energy level matching, thereby improving the ability of the interface to transport holes. This is beneficial for improving the ability of the interface at the first surface to collect photogenerated carriers (holes) near the second surface, and for improving the photoelectric conversion efficiency.

[0046] In some embodiments of this application, the first region contains the first additive.

[0047] When the first additive has doping characteristics in the first region at the interface of the perovskite layer, it is beneficial to form an interfacial electric field, thereby further improving the ability to extract interfacial charges and better improving energy conversion efficiency.

[0048] In some embodiments of this application, the perovskite layer comprises a halogen, and the perovskite layer satisfies one or more of the following characteristics:

[0049] (b1) The molar percentage of iodine in the halogens of the perovskite layer is 10% to 100%, and can be selected as 80% to 100%;

[0050] (b2) The molar percentage of bromine in the halogens of the perovskite layer is 0% to 90%, and can be selected as 0% to 20%;

[0051] (b3) Let the molar ratio of lead to halogen in the perovskite layer be q:3, then q is 0.5~1, and can be selected as 0.9~1.

[0052] By controlling the molar ratio of iodine in the halogens of the perovskite layer within the aforementioned range, the first perovskite material can contain more iodine, which is beneficial for perovskite lattice stability, moderate band gap, and sufficient light absorption.

[0053] By controlling the molar proportion of bromine in the halogens of the perovskite layer within the aforementioned range, the first perovskite material can contain a certain amount of bromine, which is beneficial for regulating the band gap and crystallization kinetics of the perovskite.

[0054] By controlling the molar ratio of iodine and bromine in the perovskite layer within the aforementioned range, it is beneficial to obtain high-quality perovskite crystals while maintaining a suitable band gap.

[0055] In some embodiments of this application, the area of ​​the perovskite layer on a projection plane perpendicular to the Z direction is greater than or equal to 0.09 cm². 2 Optionally, greater than or equal to 1m 2 .

[0056] The aforementioned Pb 2+ The sum of 4f orbital electrons and I - The modulation of the binding energy of 3d orbital electrons is beneficial for effectively passivating the aforementioned defects even when the perovskite layer has a large area, and is conducive to effectively improving the energy conversion efficiency and device stability of large-area optoelectronic devices.

[0057] In some embodiments of this application, the optoelectronic device includes a photovoltaic device or a light-emitting device.

[0058] The aforementioned perovskite layer can be used in photovoltaic devices or light-emitting devices, which helps to improve the energy conversion efficiency of photovoltaic devices or light-emitting devices.

[0059] In some embodiments of this application, the optoelectronic device includes a photovoltaic device;

[0060] The optoelectronic device satisfies one or more of the following characteristics:

[0061] (c1) The perovskite layer is contained in the inverse or formal structure of the optoelectronic device;

[0062] (c2) The optoelectronic device includes a first charge transport layer and a second charge transport layer, wherein the perovskite layer is disposed between the first charge transport layer and the second charge transport layer, the first surface faces the first charge transport layer, and the second surface faces the second charge transport layer; wherein, one of the first charge transport layer and the second charge transport layer is a hole transport layer and the other is an electron transport layer;

[0063] (c3) The optoelectronic device includes a first electrode and a second electrode, the perovskite layer is disposed between the first electrode and the second electrode, the first surface faces the first electrode, and the second surface faces the second electrode.

[0064] The aforementioned implementation methods can be universally applied to photovoltaic devices with either conventional or inverted structures, thereby improving photoelectric conversion efficiency. Furthermore, they can also enhance device stability.

[0065] In some embodiments of this application, the optoelectronic device includes a photovoltaic device, with the second surface located on the light-incident side of the perovskite layer. This not only allows the perovskite layer to have better light absorption capabilities, potentially increasing short-circuit current density and open-circuit voltage, but also helps reduce the transport path of charge carriers in the perovskite layer, thus promoting effective carrier collection and ultimately contributing to higher photoelectric conversion efficiency.

[0066] In some embodiments of this application, the optoelectronic device includes a photovoltaic device. When the first surface is used for electron transport, the photovoltaic device includes an electron transport layer stacked with the perovskite layer, with the first surface facing the electron transport layer; or...

[0067] When the first surface is used for hole transport, the photovoltaic device includes a hole transport layer stacked with the perovskite layer, with the first surface facing the hole transport layer.

[0068] When the first surface is used for electron transport, the electron transport layer is located on the side close to the first surface of the perovskite layer, utilizing the Pb in the first region of the perovskite layer. 2+ The sum of 4f orbital electrons and I - The binding energy shift of 3d orbital electrons is beneficial to improving electron transport efficiency, which can enable optoelectronic devices to achieve higher photoelectric conversion efficiency.

[0069] When the first surface is used for hole transport, the hole transport layer is located on the side close to the first surface of the perovskite layer, utilizing the Pb region of the first perovskite layer. 2+ The sum of 4f orbital electrons and I - The binding energy shift of 3d orbital electrons is beneficial to improving the hole transport efficiency, which can enable optoelectronic devices to achieve higher photoelectric conversion efficiency.

[0070] In some embodiments of this application, the optoelectronic device includes a photovoltaic device; the photovoltaic device includes a solar cell, and the solar cell includes the perovskite layer.

[0071] The aforementioned perovskite layer can be incorporated into solar cells to improve their photoelectric conversion efficiency. Furthermore, it can also enhance device stability.

[0072] In some embodiments of this application, the optoelectronic device includes a solar cell, which is a multi-junction solar cell, and the multi-junction solar cell includes a first cell unit, which includes the perovskite layer.

[0073] The aforementioned perovskite layer can be incorporated into multi-junction solar cells to improve their photoelectric conversion efficiency. Furthermore, it can also enhance device stability.

[0074] In some embodiments of this application, the multi-junction solar cell further includes a second cell stacked with the first cell; the second cell and the first cell are connected by an interconnect layer, or the second cell and the first cell are isolated by an insulating layer; the second cell includes a second light-absorbing layer, and the band gap of the second light-absorbing layer is different from that of the perovskite layer.

[0075] By setting up multiple light-absorbing layers (perovskite layer and second light-absorbing layer) with different band gaps, multi-junction solar cells can effectively absorb light of different wavelengths, broaden the spectral range of light absorbed by multi-junction solar cells, and improve the photoelectric conversion efficiency of multi-junction solar cells.

[0076] In some embodiments of this application, the second light-absorbing layer in the second battery cell includes a semiconductor active material, which includes one or more of the following: a second perovskite material, a silicon-containing semiconductor material, copper zinc tin sulfide, copper zinc tin selenide, copper zinc tin selenide sulfide, copper indium gallium selenide, copper indium gallium diselenide, copper indium selenide, cadmium telluride, gallium arsenide, and organic active materials.

[0077] The aforementioned embodiments can be universally applied to the aforementioned different types of multi-junction solar cells.

[0078] In some embodiments of this application, the multi-junction solar cell includes a first electrode, a perovskite layer, an interconnect layer, a second light-absorbing layer, and a second electrode stacked together; wherein the interconnect layer is located between the perovskite layer and the second light-absorbing layer; the first electrode is located on the side of the perovskite layer opposite to the interconnect layer, and the second electrode is located on the side of the second light-absorbing layer opposite to the interconnect layer. Thus, two cell units in the multi-junction solar cell are connected through the interconnect layer to achieve current matching between the two cell units. This results in a relatively smaller size, the ability to absorb light of different wavelengths, a wider absorption spectrum range for the multi-junction solar cell, and an improved photoelectric conversion efficiency.

[0079] In some embodiments of this application, the multi-junction solar cell includes a first electrode, a perovskite layer, a third electrode, an insulating layer, a fourth electrode, a second light-absorbing layer, and a second electrode stacked together. The third electrode, the insulating layer, and the fourth electrode are stacked between the perovskite layer and the second light-absorbing layer. The third electrode is disposed on the side of the insulating layer facing the perovskite layer, and the fourth electrode is disposed on the side of the insulating layer facing the second light-absorbing layer. The first electrode is located on the side of the perovskite layer away from the third electrode, and the second electrode is located on the side of the second light-absorbing layer away from the fourth electrode. Thus, the multi-junction solar cell forms a mechanically stacked cell. The insulating layer isolates the two cell units, preventing direct conduction of charge carriers and eliminating the need for current matching. Furthermore, each cell has its own separate positive and negative electrodes for current extraction, allowing for flexible circuit adjustments.

[0080] In some embodiments of the second aspect of this application, a method for fabricating an optoelectronic device is provided, comprising the following steps:

[0081] A perovskite precursor liquid containing perovskite precursor material and a first solvent is coated and dried on a stage at 0℃~70℃ to remove part of the first solvent, thus preparing a perovskite intermediate phase film layer.

[0082] An additive solution is sprayed onto the surface of the perovskite mesophase film layer, and then annealed with a solvent, wherein the solvent for solvent annealing is chlorobenzene, to form a perovskite layer; wherein the additive solution includes a first additive and a second solvent, and the first additive is an organic material;

[0083] The formed perovskite layer comprises a first perovskite material containing lead and iodine. The thickness direction of the perovskite layer is denoted as the Z-direction. The perovskite layer has a first surface and a second surface opposite to each other in the Z-direction, the first surface corresponding to the surface coated with the additive solution. A first region with a thickness of 5 nm to 10 nm exists extending 20 nm from the first surface along the Z-direction into the perovskite layer. The thickness of the perovskite layer is denoted as H0. A second region with a thickness of 5 nm to 10 nm exists extending (1 / 40) H0 from 1 / 2·H0 of the perovskite layer towards both the first and second surfaces. The first region is located between the first surface and the second region. The first region contains lead (Pb). 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+ The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region - The binding energy of the 3d orbital electrons is denoted as J3, and the I of the iodine element in the second region is... - The binding energy of the 3d orbital electron is denoted as J4; wherein the perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

[0084] A perovskite mesophase film with non-significant crystallinity can be obtained by drying at a low temperature (e.g., 0℃~70℃) below the crystallization temperature of perovskite. Then, a uniform first additive film is introduced by spraying, which helps the first additive to achieve maximum physical contact with defects on the perovskite surface, thereby effectively passivating the defects to the greatest extent. Furthermore, by combining a solvent annealing process, using chlorobenzene as the solvent for annealing helps to extract the first solvent in the perovskite mesophase film, allowing the perovskite mesophase film to quickly reach a highly supersaturated state, inducing rapid and uniform nucleation of perovskite in large quantities. This can promote the first additive to have a large-area uniform coverage characteristic on the crystallized perovskite film while inducing effective crystallization of perovskite, thereby achieving large-area, long-term effective, and specific interface element binding energy regulation. The optoelectronic device described in the first aspect can be prepared. Furthermore, high energy conversion efficiency and long-term operational reliability can be achieved on large-area devices.

[0085] The above-mentioned preparation process has good versatility. It can utilize the binding energy peak position control of Pb, I and optional Br elements by the first additive. It is applicable to perovskite materials with different types and crystallographic properties, and can universally and effectively achieve the control of the binding energy shift vector by defect passivation. In addition, it has good process stability and can significantly improve the batch consistency of high-efficiency devices.

[0086] Furthermore, given the effect of the first additive on the large area (e.g., ≥1m) of the crystallized perovskite film... 2 Its uniform coverage characteristic enables effective and uniform control of the bonding energy of interface elements.

[0087] The preparation method described above can achieve large-area uniform interfacial element binding energy modulation on the surface of perovskite films with different types of perovskite materials and different crystallographic properties.

[0088] The preparation methods described above can use a variety of first additives, all of which can effectively and uniformly control the interfacial element binding energy by virtue of their large-area and uniform coverage of the crystallized perovskite film.

[0089] In some embodiments of this application, the method for fabricating the optoelectronic device satisfies one or more of the following features:

[0090] (d1) The stage temperature is 20℃~35℃, and the drying time is 1s~120s, which can be selected as 30s~90s;

[0091] Optionally, the drying process employs an air knife purging method;

[0092] (d2) The first additive is the first additive in the optoelectronic device described in the first aspect of this application.

[0093] (d3) The concentration of the first additive in the additive solution is 2 mg / mL to 8 mg / mL, and can be selected as 2 mg / mL to 6 mg / mL;

[0094] (d4) The second solvent includes at least one of chloroform, isopropanol and ethanol;

[0095] (d5) In the step of spraying the additive solution onto the surface of the perovskite mesophase film, a film with a thickness of 1 nm to 10 nm is formed by spraying.

[0096] Optionally, the spraying parameters include: a flow rate of 5 sccm to 30 sccm, a spraying air pressure range of 0.3 MPa to 0.5 MPa, a distance of 15 cm to 20 cm between the spray gun and the surface of the perovskite film, and a spray gun moving speed of 5 cm / s to 60 cm / s;

[0097] (d6) The solvent annealing adopts a gradient annealing method; optionally, the solvent annealing includes performing a first stage annealing at a first temperature and then performing a second stage annealing at a second temperature, wherein the first temperature is lower than the second temperature;

[0098] Optionally, the first temperature is 85℃~95℃, and the second temperature is 100℃~120℃;

[0099] Optionally, the annealing time at the first temperature is 1 min to 3 min, and the annealing time at the second temperature is 5 min to 10 min;

[0100] Optionally, the volume percentage of chlorobenzene in the annealing atmosphere is 5% to 20%.

[0101] By controlling the spraying parameters, it is beneficial to enable the first additive to make greater physical contact with the defects on the perovskite surface, thereby achieving more effective passivation of defects.

[0102] During the first-stage annealing process at a relatively low temperature, the perovskite can be induced to nucleate uniformly and achieve pre-crystallization even with a relatively high amount of solvent residue. Then, the second-stage annealing is carried out at a relatively high temperature to induce the formation of high-quality perovskite crystals, which helps to reduce defects and improve the energy conversion efficiency of the device.

[0103] In some embodiments of the third aspect of this application, an electrical device is provided, which includes at least one of the optoelectronic devices described in the first aspect of this application and optoelectronic devices prepared by the preparation method of the optoelectronic devices described in the second aspect of this application.

[0104] In some embodiments of the fourth aspect of this application, a power generation device is provided, which includes at least one of the optoelectronic devices described in the first aspect of this application and optoelectronic devices prepared by the preparation method of the optoelectronic devices described in the second aspect of this application.

[0105] Both the power-consuming devices and power-generating devices containing the aforementioned optoelectronic devices can leverage the advantages of optoelectronic devices.

[0106] Details of one or more embodiments or examples of this application are set forth in the following drawings and description. Other features, objects, and advantages of this application will become apparent from the specification, drawings, and claims. Attached Figure Description

[0107] To better describe and illustrate the embodiments, examples, or models provided in this application, reference may be made to one or more accompanying drawings. Additional details or examples used to describe the drawings should not be considered as limiting the scope of any of the disclosed applications, the currently described embodiments, examples, or models, or the best mode of these applications as currently understood. Furthermore, the same reference numerals denote the same parts throughout the drawings. It should also be noted that the drawings are drawn in a simplified form and are only intended to facilitate and clarify the illustration of this application. The various dimensions of each part shown in the drawings are arbitrarily shown and may be precise or not drawn to scale. For example, the dimensions of parts are appropriately exaggerated in some places in the drawings to make the illustration clearer. Unless otherwise specified, the parts in the drawings are not drawn to scale. This application does not limit every dimension of every part. In the drawings:

[0108] Figure 1 This is a schematic diagram of the structure of a perovskite layer in an optoelectronic device according to an embodiment of this application. The perovskite layer has a first region and a second region, with the first region located between the first surface and the second region.

[0109] Figure 2 This is a schematic diagram of the structure of the perovskite layer and the charge transport layer in an optoelectronic device according to an embodiment of this application. The perovskite layer and the charge transport layer are stacked together. The first region is located between the charge transport layer and the second region, that is, the first surface faces the charge transport layer.

[0110] Figure 3 yes Figure 2 The diagram shows a partial structure of one embodiment of the optoelectronic device, where the charge transport layer is an electron transport layer.

[0111] Figure 4 This is a schematic diagram of the structure of the perovskite layer in an optoelectronic device according to an embodiment of this application. A first additive is present in the region of the perovskite layer near the first surface.

[0112] Figure 5This is a schematic diagram of the structure of the perovskite layer in an optoelectronic device according to an embodiment of this application. A first additive is present in the region of the perovskite layer near the first surface.

[0113] Figure 6 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of the present application. The optoelectronic device includes a first charge transport layer, a perovskite layer and a second charge transport layer stacked together. In the thickness direction of the perovskite layer, the first charge transport layer and the second charge transport layer are respectively disposed on both sides of the perovskite layer. It can be understood that one of the first charge transport layer and the second charge transport layer is an electron transport layer and the other is a hole transport layer.

[0114] Figure 7 yes Figure 6 The diagram shows a partial structure of the optoelectronic device, which includes a first charge transport layer, a perovskite layer, and a second charge transport layer stacked together. The perovskite layer is located between the first charge transport layer and the second charge transport layer. The perovskite layer has a first surface and a second surface that are opposite to each other in the thickness direction. The perovskite layer includes a first region located near the first surface and a second region located near 1 / 2 of the thickness. The first surface faces the second charge transport layer, and the second surface faces the first charge transport layer.

[0115] Figure 8 yes Figure 7 The schematic diagram shows a partial structure of the optoelectronic device. The first charge transport layer is a hole transport layer, and the second charge transport layer is an electron transport layer. The optoelectronic device includes a stacked hole transport layer, a perovskite layer, and an electron transport layer. The perovskite layer is located between the hole transport layer and the electron transport layer. The perovskite layer has a first surface and a second surface that are opposite to each other in the thickness direction. The perovskite layer includes a first region located near the first surface and a second region located near 1 / 2 of the thickness. The first surface faces the electron transport layer, and the second surface faces the hole transport layer.

[0116] Figure 9 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of this application. The optoelectronic device includes a first electrode, a first charge transport layer, a perovskite layer, a second charge transport layer, and a second electrode stacked together. In the thickness direction of the perovskite layer, the first charge transport layer and the second charge transport layer are respectively disposed on both sides of the perovskite layer. It can be understood that one of the first charge transport layer and the second charge transport layer is an electron transport layer and the other is a hole transport layer. The first electrode is disposed on the side of the first charge transport layer away from the perovskite layer, and the second electrode is disposed on the side of the second charge transport layer away from the perovskite layer.

[0117] Figure 10 yes Figure 9The schematic diagram of the optoelectronic device shown shows that the first charge transport layer is a hole transport layer and the second charge transport layer is an electron transport layer. The optoelectronic device includes a first electrode, a hole transport layer, a perovskite layer, an electron transport layer, and a second electrode stacked together. In the thickness direction of the perovskite layer, the hole transport layer and the electron transport layer are respectively disposed on both sides of the perovskite layer. The first electrode is disposed on the side of the hole transport layer away from the perovskite layer, and the second electrode is disposed on the side of the electron transport layer away from the perovskite layer.

[0118] Figure 11 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of this application. The optoelectronic device includes a substrate layer, a first electrode, a first charge transport layer, a perovskite layer, a second charge transport layer, and a second electrode stacked together. In the thickness direction of the perovskite layer, the first charge transport layer and the second charge transport layer are respectively disposed on both sides of the perovskite layer. It can be understood that one of the first charge transport layer and the second charge transport layer is an electron transport layer and the other is a hole transport layer. The first electrode is disposed on the side of the first charge transport layer away from the perovskite layer, the second electrode is disposed on the side of the second charge transport layer away from the perovskite layer, and the substrate layer is disposed on the side of the first electrode away from the perovskite layer.

[0119] Figure 12 This is a schematic diagram of the structure of an inverted optoelectronic device according to an embodiment of this application. The optoelectronic device includes a substrate layer, an incident electrode, a hole transport layer, a perovskite layer, an electron transport layer, and a back electrode stacked together. In the thickness direction of the perovskite layer, the hole transport layer and the electron transport layer are respectively disposed on both sides of the perovskite layer. The incident electrode is disposed on the side of the hole transport layer away from the perovskite layer, the back electrode is disposed on the side of the electron transport layer away from the perovskite layer, and the substrate layer is disposed on the side of the incident electrode away from the perovskite layer.

[0120] Figure 13 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of this application. The optoelectronic device includes a substrate layer, an incident electrode, an electron transport layer, a perovskite layer, a hole transport layer, and a back electrode stacked together. In the thickness direction of the perovskite layer, the hole transport layer and the electron transport layer are respectively disposed on both sides of the perovskite layer. The incident electrode is disposed on the side of the electron transport layer away from the perovskite layer, the back electrode is disposed on the side of the hole transport layer away from the perovskite layer, and the substrate layer is disposed on the side of the incident electrode away from the perovskite layer.

[0121] Figure 14 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of the present application. The optoelectronic device is provided with a first channel region, a second channel region and a third channel region.

[0122] Figure 15 This is a schematic diagram of an electrical device according to an embodiment of this application, in which an optoelectronic device is used as a power generation device.

[0123] Figure 16 This is an X-ray photoelectron spectroscopy (XPS) test result of Pb element in the perovskite layer of the optoelectronic device according to an embodiment of this application. The horizontal axis is the binding energy (abbreviated as BE), and the vertical axis is the signal intensity.

[0124] Figure 17 This is an XPS test result graph of element I in the perovskite layer of an optoelectronic device according to an embodiment of this application. The horizontal axis represents the binding energy (abbreviated as BE), and the vertical axis represents the signal intensity.

[0125] Explanation of reference numerals in the attached figures:

[0126] 10, Optoelectronic device; 100, Perovskite layer; Z, Thickness direction of perovskite layer; 101, First surface; 102, Second surface; 110, First region; 120, Second region; 111, First additive; 300, Charge transport layer; 310, First charge transport layer; 320, Second charge transport layer; 410, First electrode; 420, Second electrode; 500, Substrate layer; 610, Hole transport layer; 620, Electron transport layer; 700, Light-incident side electrode; 800, Back electrode; P1, First channel region; P2, Second channel region; P3, Third channel region; 6, Electrical device.

[0127] It should be noted that, Figure 1-5 The dashed lines marked within the perovskite layer in sections 7-8 only indicate the positions of the first or second region on both sides in the thickness direction of the perovskite layer, but do not imply that the marked first or second region forms an interface of different phases with the adjacent portion within the perovskite layer; in some embodiments, the phases on both sides shown by the dashed lines are continuously distributed. Detailed Implementation

[0128] The following describes in detail, with appropriate reference to the accompanying drawings, some embodiments and examples of the optoelectronic device, fabrication method, power supply device, and power generation device of this application. However, some unnecessary detailed descriptions may be omitted. For example, detailed descriptions of well-known matters and repetitive descriptions of practically identical structures may be omitted. This is to avoid unnecessarily lengthy descriptions and to facilitate understanding by those skilled in the art. Furthermore, the accompanying drawings and the following description are provided for the purpose of enabling those skilled in the art to fully understand this application and are not intended to limit the subject matter of the claims.

[0129] The "range" disclosed in this application can be defined in the form of a lower limit and an upper limit. A given range is defined by selecting a lower limit and an upper limit, which define the boundaries of a particular range. Ranges defined in this way can include or exclude endpoints. Any endpoint can be included or excluded independently and can be combined arbitrarily; that is, any lower limit can be combined with any upper limit to form a range. For example, if ranges of 60-120 and 80-110 are listed for a specific parameter, it is expected that ranges of 60-110 and 80-120 are also included. Furthermore, if minimum range values ​​1 and 2 are listed, and maximum range values ​​3, 4, and 5 are also listed, then the following ranges are all expected: 1-3, 1-4, 1-5, 2-3, 2-4, and 2-5. In this application, unless otherwise stated, the numerical range "ab" represents a shortened representation of any combination of real numbers between a and b, where a and b are real numbers. For example, the numerical range "0-5" indicates that all real numbers between "0" and "5" have been listed in this article; "0-5" is simply a shortened representation of these numerical combinations. Furthermore, when describing a parameter as an integer ≥ 2, it is equivalent to listing integers such as 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, and 12 for that parameter. For instance, when describing a parameter as an integer selected from "2-10", it is equivalent to listing the integers 2, 3, 4, 5, 6, 7, 8, 9, and 10.

[0130] In this application, the term "numerical value" includes the number itself and its reasonable approximations. The definition of "numerical value" can apply to discrete numerical points or to the endpoints of a numerical range. Unless otherwise specified, the term "approximation" covers a numerical interval based on a reasonable range of fluctuations of the number itself. This reasonable range of fluctuations can vary depending on the type and magnitude of the number. This reasonable range of fluctuations can be reasonably determined based on the accuracy of the testing or measurement method. Therefore, when referring to a numerical value or a numerical range, unless otherwise specified, it should be understood that the numerical value includes its reasonable approximation, and the numerical range includes reasonable approximations at both endpoints. Those skilled in the art will understand that acceptable fluctuation ranges of the relevant approximations can be included within the definition of the numerical value or the numerical range. In this application, unless otherwise specified, "N1" can be reasonably understood as "about N1," and "N1~N2" can be reasonably understood as "about N1 to about N2," where N1 and N2 are two unequal numerical values.

[0131] In this application, unless otherwise specified, "about" means within a reasonable range above and below the number, and the range of fluctuation may vary depending on the type and value of the number. For example, a range of ±10%, ±5%, ±2%, ±1% may be allowed.

[0132] In this application, the terms "multiple," "various," or "multiple items" are used unless otherwise specified, referring to a quantity greater than or equal to 2. For example, "one or more" means one item or two or more (greater than or equal to) items. It can be understood that when "any number of" items are involved, it refers to any suitable combination of multiple items, that is, a combination of "any number of" items in a manner that does not conflict and enables the implementation of this application.

[0133] Unless otherwise specified, all embodiments and optional embodiments of this application can be combined to form new technical solutions.

[0134] In this document, the term "embodiment" means that a particular feature, structure, or characteristic described in connection with an embodiment may be included in at least one embodiment or implementation of this application. The appearance of this phrase in various places throughout the specification does not necessarily refer to the same embodiment, nor is it a separate or alternative embodiment mutually exclusive with other embodiments. It will be explicitly and implicitly understood by those skilled in the art that the embodiments described herein can be combined with other embodiments. The term "implementation" as used herein has a similar understanding.

[0135] Those skilled in the art will understand that, unless otherwise specified, the order in which the steps are written in the various embodiments or methods of this application does not imply a strict execution order and does not constitute any limitation on the implementation process. The detailed execution order of each step should be determined by its function and possible internal logic. Unless otherwise specified, all steps of this application may be performed sequentially or randomly, but are preferably performed sequentially. For example, if method M includes steps (a) and (b), it means that the method may include steps (a) and (b) performed sequentially, or it may include steps (b) and (a) performed sequentially. For example, method M may also include step (c), meaning that step (c) can be added to method M in any order. For example, method M may include steps (a), (b), and (c), or it may include steps (a), (c), and (b), or it may include steps (c), (a), and (b), etc.

[0136] In this application, open-ended technical features or solutions described using terms such as "containing," "comprising," or "including" do not exclude additional members beyond those listed unless otherwise specified. They can be considered as providing both closed-ended features or solutions comprised of the listed members and open-ended features or solutions that include additional members beyond the listed members. For example, if 'a' includes a1, a2, and a3, it may also include other members or exclude additional members unless otherwise specified. This can be considered as providing both features or solutions where "a consists of a1, a2, and a3" or "a is selected from a1, a2, and a3," and features or solutions where "a includes not only a1, a2, and a3, but also other members."

[0137] In this application, unless otherwise specified, M (e.g., m1) means that m1 is a non-limiting example of M, and it is understood that M is not limited to m1.

[0138] In this application, "optionally," "optionally," and "optional" mean that something is optional, that is, it is selected from either "with" or "without." If multiple "options" appear in a technical solution, unless otherwise specified and there are no contradictions or mutual constraints, each "option" is independent. Unless otherwise specified, the descriptions such as "optionally include" and "optionally contain" in this application, taking "optionally include" as an example, mean "may include or not include."

[0139] In this application, unless otherwise specified, the features or solutions corresponding to "and / or" include any one of two or more of the related listed items, as well as any and all combinations of the related listed items. Any and all combinations include any two related listed items, any more related listed items, or a combination of all related listed items. For example, "M and / or N" represents the group consisting of M, N, and "a combination of M and N". "Containing M and / or N" can mean "containing M, containing N, and containing both M and N", or "containing M, containing N, or containing both M and N", and can be appropriately understood according to the context.

[0140] In this document, the word "suitable" in "suitable combination" or "suitable method" refers to the technical solution that can implement this application.

[0141] In this document, terms such as "preferred," "better," and "good" are merely descriptions of implementation methods or embodiments that achieve better results and should be understood not to limit the scope of protection of this application. If multiple "preferred" terms appear in a technical solution, unless otherwise specified and there are no contradictions or mutual constraints, each "preferred" term shall be independent.

[0142] In this application, terms such as "further," "even more," "especially," "for example," "as," "example," and "exemplary" are used for descriptive purposes to indicate differences in content, but should not be construed as limiting the scope of protection of this application.

[0143] In this application, the terms "first aspect," "second aspect," "third aspect," "fourth aspect," etc., are used for descriptive purposes only and should not be construed as indicating or implying relative importance or quantity, nor should they be construed as implicitly indicating the importance or quantity of the indicated technical features. Moreover, "first," "second," "third," "fourth," etc., serve only as a non-exhaustive enumeration and should be understood not to constitute a closed limitation on quantity.

[0144] In this application, the term "room temperature" generally refers to 4℃~35℃, and may refer to 20℃±5℃. In some embodiments or examples of this application, room temperature refers to 20℃~30℃.

[0145] In this application, when a unit is specified for a data range, if the unit is only followed by the right endpoint, it indicates that the units for the left and right endpoints are the same. For example, 3~5μm or 3-5μm both mean that the unit for the left endpoint "3" and the right endpoint "5" is μm (micrometer), and both have the same meaning as 3μm~5μm. Furthermore, similar descriptions of other parameters such as temperature and concentration are interpreted in the same way.

[0146] In this application, unless otherwise specified, wt% means weight percentage, which is numerically equal to the corresponding mass percentage.

[0147] In the description of the embodiments or examples of this application, the terms "center", "longitudinal", "lateral", "length", "height", "width", "thickness", "upper", "lower", "front", "rear", "left", "right", "vertical", "horizontal", "top", "bottom", etc., indicating the orientation or positional relationship are only for the convenience of describing the embodiments of this application and simplifying the description, and are not intended to indicate or imply that the device or element referred to must have a specific orientation, or be constructed and operated in a specific orientation, and therefore should not be construed as a limitation on the embodiments of this application.

[0148] In this application, unless otherwise expressly specified and limited, in the device structure, the first feature "above" or "below" the second feature can be in direct contact with the first feature, or indirect contact between the first and second features through an intermediate medium. In this application, unless otherwise expressly specified and limited, the first feature "above" or "below" the second feature can indicate a horizontal relative position, or it can simply indicate the existence of an attachment relationship without specifying a horizontal relative position.

[0149] In this application, the exemplary descriptions such as "in some implementations (or embodiments)" and "in one implementation (or embodiment)" may cover, but are not limited to, the following meanings: these solutions can be combined with other solutions in a suitable manner to form new technical solutions.

[0150] In this application, the terms "first," "second," and "third" in the following contexts are used for descriptive purposes only and should not be construed as indicating or implying relative importance or quantity, nor should they be construed as implicitly indicating the importance or quantity of the indicated technical features.

[0151] In this application, unless otherwise specified, "layered arrangement" refers to the description of the stacking direction between layered structures and does not constitute a limitation on the structural composition of the stacked body. For example, "including stacked structural layer A and structural layer B" means that the stacking direction of structural layer A and structural layer B is along their respective thickness directions; that is, the thickness direction of structural layer A is consistent with or substantially consistent with the thickness direction of structural layer B. It is understood that other intermediate structural layers are allowed to be set between structural layer A and structural layer B.

[0152] Unless otherwise stated, the improvements described in this application are not intended to be limited to any theoretical constraints.

[0153] In this application, unless otherwise specified, an "optoelectronic device" is a device capable of photoelectric conversion using a photoelectric conversion mechanism, which includes the process of converting light energy into electrical energy and vice versa. An optoelectronic device can be a photovoltaic device or a light-emitting device. In this application, unless otherwise specified, the core functional layer that exchanges energy with photons can be called the "active layer," which includes a semiconductor active material. In a photovoltaic device, the semiconductor active material absorbs photons to generate carrier pairs (which are electron-hole pairs), and this active layer can be called the "light-absorbing layer" or "light-absorbing layer." In a light-emitting device, the semiconductor active material recombines injected electrons and holes and releases photons, and this active layer can be called the "light-emitting layer." Optoelectronic devices can achieve photoelectric conversion through any suitable mechanism. Photovoltaic devices can convert light energy into electrical energy based on a light-absorbing layer, and light-emitting devices can convert electrical energy into light energy based on a light-emitting layer.

[0154] In this application, unless otherwise specified, "active layer" refers to a structural layer comprising a semiconductor active material. The semiconductor active material can be any suitable type of semiconductor active material capable of photoelectric conversion. Non-limiting examples of semiconductor active materials may include one or more of perovskite materials, silicon-containing semiconductor materials, copper zinc tin sulfide, copper zinc tin selenide, copper zinc tin selenide sulfide, copper indium gallium selenide, copper indium gallium diselenide, copper indium selenide, cadmium telluride, and organic active materials. Exemplarily, the semiconductor active material may include one or more of perovskite materials, gallium arsenide (GaAs), cadmium telluride (CdTe), copper indium selenide (CIGS), and organic active materials.

[0155] In this application, unless otherwise stated, a "photovoltaic device" is a photoelectric device capable of converting solar energy into electrical energy using a photoelectric conversion mechanism. The active layer in a photovoltaic device can generate carrier pairs (which can be electron-hole pairs) upon excitation by incident photons. The flow of electrons and holes generates current, thereby realizing the conversion from light energy to electrical energy. The active layer in a photovoltaic device can be referred to as a "light-absorbing layer." Application examples of photovoltaic devices may include, but are not limited to, solar cells.

[0156] In this application, unless otherwise specified, "solar cell" refers to a battery capable of converting solar energy into electrical energy using a photoelectric conversion mechanism. It is understood that a solar cell includes a light-absorbing layer. When the light-absorbing layer comprises perovskite material, the solar cell is a "perovskite solar cell".

[0157] In this application, unless otherwise specified, a "light-emitting device" is a photoelectric device capable of converting electrical energy into solar energy using a photoelectric conversion mechanism. The active layer in a photoelectric device can recombine injected charge carriers (electrons and holes), releasing energy in the form of photons. Non-limiting examples of light-emitting devices may include light-emitting diodes (LEDs), laser diodes (LDs), etc. Applications of light-emitting devices may include, but are not limited to, lighting and display applications.

[0158] In this application, unless otherwise specified, "energy conversion efficiency" refers to the efficiency of converting light energy (or electrical energy) into electrical energy (or light energy) in an optoelectronic device. In photovoltaic devices, energy conversion efficiency refers to the efficiency of converting light energy into electrical energy, generally referred to as photoelectric conversion efficiency (PCE). In light-emitting devices, energy conversion efficiency refers to the efficiency of converting electrical energy into light energy, which can be expressed as external quantum efficiency (EQE).

[0159] In this application, unless otherwise specified, "charge carrier" can be an electron or a hole. "Carrier pair" refers to an electron-hole pair.

[0160] In some embodiments of this application, when the photovoltaic device is operating, after the light-absorbing layer is illuminated, the internal electrons gain energy and break free from the binding force of the light-absorbing layer to form negatively charged electron carriers, and simultaneously form positively charged hole carriers, thus generating electron-hole pairs. The free electrons and free holes propagate in opposite directions, causing electrons and holes to flow and forming an external current, thereby realizing the conversion of light energy into electrical energy. Furthermore, after the light-absorbing layer absorbs photons, it is stimulated to generate electron-hole pairs. These pairs further dissociate to form free carriers with opposite charges. The free electrons propagate towards the negative electrode, and the free holes propagate towards the positive electrode. Both types of free carriers are collected by their respective electrodes, further forming a photocurrent in the circuit of the photovoltaic device.

[0161] In some embodiments of this application, in a photovoltaic device, free electrons are transported to the negative electrode through an electron transport layer, and free holes are transported to the positive electrode through a hole transport layer. The two types of free carriers are collected by their respective electrodes, and further form a photocurrent in the circuit of the photovoltaic device.

[0162] In photovoltaic devices, the electron transport layer can extract and transport electron carriers and block free holes from passing through.

[0163] In photovoltaic devices, the hole transport layer can extract and transport hole carriers and block free electrons from passing through.

[0164] In some embodiments of this application, when the light-emitting device is operating, an external forward bias voltage is applied to inject electrons from the cathode and holes from the anode. The injected charge carriers (electrons and holes) are transported to the light-emitting layer, where they recombine, releasing energy and emitting light in the form of photons. The cathode is typically connected to the negative terminal of the power supply, and the anode is typically connected to the positive terminal of the voltage.

[0165] In light-emitting devices, the electron transport layer is responsible for injecting and transporting electron carriers and can block free holes from passing through.

[0166] In light-emitting devices, the hole transport layer is responsible for injecting and transporting hole carriers and can block free electrons from passing through.

[0167] In this application, unless otherwise specified, from the perspective of the type of semiconductor active material, optoelectronic devices whose active layer includes perovskite material can be referred to as "perovskite devices". The active layer in a perovskite device can be referred to as a "perovskite layer". From an application perspective, perovskite devices can be used in both photovoltaic and light-emitting fields; that is, perovskite devices can function as both photovoltaic devices and light-emitting devices.

[0168] In this application, unless otherwise specified, "perovskite layer" refers to the active layer comprising perovskite material. The perovskite layer has a certain thickness, for example, but not limited to 100nm~2000nm, and optionally 200nm~1500nm.

[0169] In this application, the "thickness direction of the perovskite layer" can be denoted as the Z direction, and the direction perpendicular to the Z direction can be denoted as the transverse direction.

[0170] In this application, unless otherwise specified, the perovskite layer 100 includes two surfaces that are opposite to each other in its thickness direction (Z direction), which may be referred to as the first surface 101 and the second surface 102, respectively. (See reference...) Figure 1 The spacing between the first and second surfaces roughly corresponds to the thickness of the perovskite layer. In some embodiments of this application, the first and second surfaces of the perovskite layer respectively contact different structural layers disposed adjacent to the perovskite layer. In some embodiments, the first and second surfaces of the perovskite layer respectively contact different charge transport layers.

[0171] Optoelectronic devices can be either photovoltaic (PV) devices or light-emitting devices. A representative PV device is the perovskite solar cell, in which the light-absorbing layer is a perovskite layer containing perovskite material. Due to its high conversion efficiency and the ability to be fabricated using low-cost solution methods, perovskite solar cells have attracted widespread attention from industry. Photovoltaic conversion efficiency is crucial for the practical application of perovskite solar cells. Therefore, researching ways to improve the energy conversion efficiency of optoelectronic devices is of great significance.

[0172] Taking perovskite solar cells as an example, crystal defects are one of the important factors affecting device efficiency. Passivating defects by introducing additives is one approach to improve device efficiency. Common methods of introducing additives are: (1) adding them directly to the perovskite precursor solution; (2) introducing additives by coating them onto the surface of the perovskite layer after obtaining the crystallized perovskite layer. However, both methods have shortcomings. Method (1) may passivate bulk defects, but it may reduce the crystal quality, resulting in limited improvement in device efficiency. Method (2) may affect interface charge transport while passivating interface defects, thus limiting the improvement in device efficiency. Therefore, it is necessary to develop new solutions to improve the energy conversion efficiency of optoelectronic devices.

[0173] According to various embodiments and examples of this application, this application provides an optoelectronic device, a fabrication method, an electrical device, and a power generation device. The optoelectronic device exhibits high photoelectric conversion efficiency.

[0174] In some embodiments of this application, the optoelectronic device 10 includes a perovskite layer 100. Figure 1 This is a schematic diagram of the structure of a perovskite layer 100 in an optoelectronic device according to an embodiment of this application. The perovskite layer 100 has a first surface 101 and a second surface 102 that are opposite to each other in the thickness direction (Z direction) of the perovskite layer, and has a first region 110 located near the first surface 101 and a second region 120 located in the bulk phase portion of the perovskite layer 100. The first region 110 is located between the first surface 101 and the second region 102.

[0175] It can be understood that the perovskite layer includes perovskite material (denoted as the first perovskite material).

[0176] In some embodiments of this application, the optoelectronic device includes a charge transport layer 300. Figure 2 This is a schematic diagram of the structure of a perovskite layer 100 and at least one charge transport layer 300 in an optoelectronic device according to an embodiment of this application. The perovskite layer 100 and the charge transport layer 300 are stacked together. A first region 110 is located between the charge transport layer 300 and a second region 120, that is, the first surface 101 faces the charge transport layer 300. The charge transport layer 300 can be a hole transport layer 610 or an electron transport layer 620.

[0177] Figure 3 yes Figure 2 A schematic diagram of a partial structure of one embodiment of the optoelectronic device shown. Figure 2 The charge transport layer 300 is an electron transport layer 620.

[0178] In some embodiments of this application, a region with a thickness of 5nm to 10nm that extends 20nm from the first surface toward the interior of the perovskite layer along the Z direction is referred to as the first region.

[0179] In some embodiments of this application, the thickness of the perovskite layer is denoted as H0; a region with a thickness of 5nm to 10nm that extends from (1 / 2) H0 of the perovskite layer toward the first surface and the second surface respectively is denoted as the second region; the first region is located between the first surface and the second region.

[0180] In this application, unless otherwise specified, "first region" refers to the region within the perovskite layer located near the first surface, and "second region" refers to the region located in the bulk phase portion of the perovskite layer. It is understood that the first region is located between the first surface and the second region, and the second region is located between the first region and the second surface. The properties of the perovskite material within the first region reflect the properties at the perovskite layer interface, and the properties of the perovskite material within the second region reflect the properties of the bulk phase of the perovskite layer. Both the first and second regions independently possess a relatively thin thickness (e.g., 5 nm to 10 nm), which can be matched to the detection depth during XPS testing and the detection depth during energy level testing, such as the detection depth when using X-ray photoelectron spectroscopy (XPS) to test the binding energy, or the detection depth when using ultraviolet photoelectron spectroscopy (UPS) to test the energy level. In some embodiments, the first and second regions have the same thickness, which can be achieved by controlling parameters such as the incident angle during UPS testing.

[0181] In some embodiments of this application, the perovskite layer includes a first perovskite material containing lead and iodine. In this case, the perovskite layer includes lead (Pb) and iodine (I).

[0182] In this application, the Pb content of lead in the first region is... 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+ The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region... - The binding energy of 3d orbital electrons is denoted as J3, and the I of iodine in the second region is... - The binding energy of 3d orbital electrons is denoted as J4.

[0183] In this application, unless otherwise stated, the term "binding energy" for orbital electrons has the well-known meaning in the art, referring to the minimum energy required to completely remove an electron in a specific atomic orbital (such as 4f, 3d, etc.) from its bound state. The magnitude of the binding energy reflects the strength of the bond between the orbital atom and the atomic nucleus; the higher the binding energy, the more difficult it is to remove the orbital electron from the atomic nucleus.

[0184] Pb 2+ The 4f orbital electrons have two peaks in the XPS spectrum; in this application, unless otherwise specified, the higher intensity Pb ​​will be used. 2+ 4f 7 / 2 The binding energy of orbital electrons as "Pb 2+ "The binding energy of the 4f orbital electrons" means that when a displacement occurs, the displacement amplitudes of the two orbitals are equal.

[0185] I -The 3d orbital electron has two peaks in the XPS spectrum. In this application, unless otherwise specified, the higher intensity I will be used. - 3D 3 / 2 The binding energy of orbital electrons is used as "I - "The binding energy of 3d orbital electrons".

[0186] Furthermore, in the case where the first perovskite material also includes bromine (Br), Br - The 3d orbital electron has two peaks in the XPS spectrum. In this application, unless otherwise specified, the higher-intensity Br will be used. - 3D 3 / 2 The binding energy of orbital electrons is used as the "Br - "The binding energy of 3d orbital electrons".

[0187] When an atom bonds with other atoms, its electron cloud density changes, causing a shift in the binding energy of its inner-shell electrons (i.e., a chemical shift). This change indirectly reflects the nature of the bond. A larger chemical shift indicates more electrons transferred; for the same type of orbital electrons, a larger chemical shift indicates a stronger bond.

[0188] When the binding energy of orbital electrons shifts towards higher binding energies, it indicates a decrease in electron cloud density, meaning the atom is in a more electron-deficient state; conversely, when the binding energy of orbital electrons shifts towards lower binding energies, it indicates an increase in electron cloud density, meaning the atom is in a more electron-rich state.

[0189] Those skilled in the art can use methods already existing in the art to obtain the orbital electron binding energy of selected atoms, including but not limited to X-ray photoelectron spectroscopy (XPS). Instrument models may include, but are not limited to, Thermo Fisher Scientific ESCALAB QXi.

[0190] Taking a perovskite layer sample from one embodiment as an example, the perovskite layer thickness is 450 nm. The 20 nm thickness region of the perovskite layer closest to the FTO side is defined as the lower interface region. The perovskite layer portion within a 20 nm range of the thickness center region is used to represent the bulk phase of the perovskite layer (the second region is included in the bulk phase portion). The 20 nm thickness region of the perovskite layer on the other side is defined as the upper interface region of the perovskite layer. At least one of the lower interface region and the upper interface region contains a first region.

[0191] X-ray photoelectron spectroscopy (XPS) can be used to obtain elemental distribution information at different depths (including the first and second regions) of the perovskite layer by sputtering the sample surface layer by layer and combining it with full elemental scanning. The depth sampling depth of XPS testing is 0.5 nm to 10 nm, and it can be performed by ion sputtering (such as Ar). + C +0The sample is peeled layer by layer using either a cluster ion beam or a phantom ion beam. XPS full spectrum or specific elemental spectrum is acquired after each layer is peeled off. The thickness of each layer can be adjusted according to the thickness of the perovskite layer. For example, when the perovskite layer thickness is 400 nm, information can be acquired at different thicknesses with intervals of 20 nm to 100 nm. This allows the acquisition of the binding energies of Pb orbitals and I orbitals in the first and second regions of the perovskite layer, including but not limited to Pb. 2+ The binding energy of 4f orbital electrons and I - Binding energy of 3d orbital electrons.

[0192] See also the Examples and Tests section below.

[0193] In some embodiments of this application, the perovskite layer includes a first perovskite material containing Pb and I elements. Further, the perovskite layer satisfies J1-J2 > 0 eV (i.e., the first region shifts towards a higher binding energy direction relative to the second region) and J4-J3 > 0 eV (i.e., the first region shifts towards a lower binding energy direction relative to the second region). In some embodiments, the perovskite layer satisfies J1-J2 ≥ 0.15 eV and J4-J3 ≥ 0.15 eV.

[0194] In some embodiments of this application, an optoelectronic device is provided, comprising a perovskite layer, the perovskite layer comprising a first perovskite material containing Pb and I elements; the perovskite layer having a first surface and a second surface opposite to each other in its thickness direction; the perovskite layer comprising a first region located near the first surface and a second region located in the bulk phase portion of the perovskite layer, wherein the perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

[0195] In some embodiments of the first aspect of this application, an optoelectronic device is provided, comprising a perovskite layer including Pb and I elements; the thickness direction of the perovskite layer is denoted as the Z direction; the perovskite layer has a first surface and a second surface that are opposite to each other in the Z direction; a first region with a thickness of 5 nm to 10 nm exists within a range extending 20 nm from the first surface along the Z direction toward the interior of the perovskite layer; the thickness of the perovskite layer is denoted as H0; a second region with a thickness of 5 nm to 10 nm exists within a range extending (1 / 40)·H0 from half the thickness of the perovskite layer toward the first surface and the second surface, respectively.

[0196] The first region is located between the first surface and the second region; the lead element Pb in the first region... 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region... - The binding energy of 3d orbital electrons is denoted as J3, and the I of iodine in the second region is... - The binding energy of 3d orbital electrons is denoted as J4;

[0197] Among them, the perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

[0198] The perovskite material (denoted as the first perovskite material) in the perovskite layer of this optoelectronic device contains lead (Pb) and iodine (I) elements. Furthermore, the perovskite layer includes a first region located near one side of the surface and a second region located in the bulk phase of the perovskite layer, further controlling the Pb content of the lead element within the first region. 2+ The binding energy of the 4f orbital electrons shifts towards higher binding energies relative to the second region, while the I energy of iodine in the first region... - The binding energy of 3d orbital electrons shifts towards lower binding energies relative to the second region. At this point, the valence state of lead in the first region is closer to +2, and the valence state of iodine is closer to -1. This is more conducive to the formation of a more stable crystal structure in the first region of the perovskite layer, reducing the distortion of the crystal structure caused by the binding energy shift of Pb or I elements in the perovskite material, and reducing lead or iodine vacancy defects. This alleviates the defects in the first region caused by excessive dangling bonds and uneven crystallization near the surface of the perovskite layer, thereby reducing the probability of nonradiative recombination of charge carriers in the first region and thus improving the overall energy conversion efficiency of optoelectronic devices.

[0199] It's understandable that I don't want to be limited to the above theories.

[0200] In some embodiments of this application, J1-J2 is greater than 0 eV, and further, greater than or equal to 0.15 eV, and may also be any of the following values ​​or a range selected from any two of the following values: 0.15 eV, 0.16 eV, 0.17 eV, 0.18 eV, 0.19 eV, 0.20 eV, 0.21 eV, 0.22 eV, 0.23 eV, 0.24 eV, 0.25 eV, 0.26 eV, 0.27 eV, 0.28 eV, 0.30 eV, etc.

[0201] In some embodiments of this application, 0.15 eV ≤ J1-J2 ≤ 0.3 eV, optionally, 0.16 eV ≤ J1-J2 ≤ 0.28 eV, and further optionally, 0.20 eV ≤ J1-J2 ≤ 0.25 eV. By controlling J1-J2 within the aforementioned range, it is possible to regulate the formation of a more stable lattice structure in the first region, thereby reducing lead vacancy defects in the perovskite layer. It is also possible to regulate the degree of electron cloud shift of the corresponding valence states of Pb or I elements, better avoiding excessive electron cloud shift of Pb elements, thereby reducing significant distortion of the perovskite lattice and the resulting introduction of suppressive lattice stress. Furthermore, the formation of a more stable lattice structure in the perovskite material in the first region can further reduce ion migration in the perovskite material, improving the long-term stability of the device.

[0202] In some embodiments of this application, J4-J3 is greater than 0 eV, and further, greater than or equal to 0.15 eV, and may also be any of the following values ​​or a range selected from any two of the following values: 0.15 eV, 0.16 eV, 0.17 eV, 0.18 eV, 0.19 eV, 0.20 eV, 0.21 eV, 0.22 eV, 0.23 eV, 0.24 eV, 0.25 eV, 0.26 eV, 0.27 eV, 0.28 eV, 0.30 eV, 0.32 eV, 0.34 eV, 0.35 eV, 0.36 eV, 0.38 eV, 0.40 eV, 0.42 eV, 0.44 eV, 0.45 eV, etc.

[0203] In some embodiments of this application, 0.15 eV ≤ J4-J3 ≤ 0.45 eV, optionally, 0.20 eV ≤ J4-J3 ≤ 0.45 eV, and further optionally, 0.35 eV ≤ J4-J3 ≤ 0.42 eV. By controlling J4-J3 within the aforementioned range, it is possible to regulate the formation of a more stable lattice structure in the first region, thereby reducing the defects of iodine vacancies in the perovskite layer. It is also beneficial to better avoid excessive electron cloud shift of element I, thereby reducing significant distortion of the perovskite lattice and the introduction of lattice stress thereafter.

[0204] Furthermore, the binding energy modulation of Pb and / or I is low or non-dependent on weak van der Waals forces, ionic bonds, and other interactions, which is beneficial for making the interfacial connections of the perovskite layer more stable and improving device stability.

[0205] In some embodiments of this application, the perovskite layer satisfies one or more of the following characteristics:

[0206] (z1) J2 is 138 eV~139 eV;

[0207] (z2)J4 is 619 eV~620 eV.

[0208] At this point, by controlling the Pb content of lead in the second region... 2+ The binding energy of the 4f orbital electrons and / or the I of iodine - The binding energy of 3d orbital electrons can regulate the valence distribution of lead and iodine in the perovskite bulk phase, placing them near +2 and -1 valences. This allows for overall regulation of the perovskite crystal structure within the perovskite layer, resulting in a more stable lattice structure and improving the long-term stability of optoelectronic devices.

[0209] In this application, the first perovskite material also includes bromine, and the Br content of bromine in the first region is... - The binding energy of 3d orbital electrons is denoted as J5, and the Br₂ of bromine in the second region is... - The binding energy of 3d orbital electrons is denoted as J6.

[0210] In some embodiments of this application, the first perovskite material includes bromine, in which case the perovskite layer includes bromine. In some embodiments, 0 eV <J6-J5。

[0211] In some embodiments of this application, 0eV <J6-J5≤0.5 eV。

[0212] In some embodiments of this application, the first perovskite material includes lead, iodine, and bromine. When the perovskite layer simultaneously includes lead, iodine, and bromine, the advantages of high crystallinity and high device efficiency of lead-containing perovskite can be utilized, as well as the advantages of bromine in regulating crystallization and improving the band gap can be leveraged.

[0213] In some embodiments of this application, J6-J5 is greater than 0 eV, and further, greater than or equal to 0.20 eV, and may also be any of the following values ​​or a range selected from any two of the following values: 0.20 eV, 0.21 eV, 0.22 eV, 0.23 eV, 0.24 eV, 0.25 eV, 0.26 eV, 0.27 eV, 0.28 eV, 0.30 eV, 0.32 eV, 0.34 eV, 0.35 eV, 0.36 eV, 0.38 eV, 0.40 eV, 0.42 eV, 0.44 eV, 0.45 eV, 0.46 eV, 0.48 eV, 0.5 eV, etc.

[0214] In some embodiments of this application, the perovskite layer further includes bromine; wherein J6-J5 ≥ 0.20 eV. In this case, by applying Br to the bromine in the first region... -The shift of the binding energy of 3d orbital electrons relative to the second region towards lower binding energy is beneficial for bringing the valence state of bromine in the first region closer to -1, making the lattice structure of bromine-containing perovskite crystals more stable and reducing defects such as halogen vacancies. Further controlling the shift amplitude within the aforementioned range (e.g., J6-J5≥0.20 eV) is even more beneficial for reducing defects such as halogen vacancies.

[0215] In some embodiments of this application, 0.2 eV ≤ J6-J5 ≤ 0.5 eV. In this case, by using the Br₂ of bromine in the first region... - The shift of the binding energy of 3d orbital electrons relative to the second region towards lower binding energy is beneficial for bringing the valence state of bromine in the first region closer to -1, making the lattice structure of bromine-containing perovskite crystals more stable, reducing defects such as halogen vacancies, further controlling the shift range within the aforementioned range, and also helping to better avoid significant lattice distortion and the introduction of lattice stress.

[0216] In some embodiments of this application, 0.28 eV ≤ J6-J5 ≤ 0.5 eV, and optionally, 0.35 eV ≤ J6-J5 ≤ 0.46 eV. In this case, by using the Br₂ of bromine in the first region... - The movement of the binding energy of 3d orbital electrons relative to the second region is within the aforementioned range, which is beneficial not only for effectively reducing defects such as halogen vacancies, but also for avoiding significant lattice distortion and the resulting introduction of lattice stress.

[0217] In addition to using the aforementioned XPS test results to obtain elemental composition information at different thicknesses of the perovskite layer, other suitable elemental analysis methods can be used to confirm the elemental composition at different thicknesses of the perovskite layer. These methods may include, but are not limited to, time-of-flight secondary ion mass spectrometry (TOF-SIMS), using instruments such as PHI nanoTOF Ⅲ Time-of-Flight SIMS, and selecting appropriate ion sources (such as Cs). + Bi 3+ (etc.), primary ion energy (e.g., 0.5keV~30keV), imaging region size (e.g., 500×500μm) 2 100×100μm 2 Test parameters such as mass range and mass resolution, sputtering parameters (such as sputtering time, sputtering area, sputtering rate, analysis mode (such as depth profile mode, neutralization mode, etc.)) are used to obtain the three-dimensional distribution information of the corresponding elements or components in the sample to be tested.

[0218] Based on the three-dimensional distribution information of an element or component, it can be determined whether that element or component is distributed in the perovskite crystal phase. If the element or component is distributed in the perovskite crystal phase, the perovskite material can be considered to contain that element or component.

[0219] In some embodiments of this application, the thickness of the perovskite layer is greater than or equal to 200 nm. In this case, it is beneficial to make the relative positional relationship between the first region and the second region more consistent with the aforementioned definition.

[0220] In some embodiments of this application, the thickness of the perovskite layer is 200 nm to 1500 nm, optionally 400 nm to 1000 nm, and may also be any of the following values ​​or a range selected from any two of the following values: 200 nm, 250 nm, 300 nm, 350 nm, 400 nm, 450 nm, 500 nm, 600 nm, 700 nm, 800 nm, 900 nm, 1000 nm, 1100 nm, 1200 nm, 1300 nm, 1400 nm, 1500 nm, etc. Exemplarily, the thickness of the perovskite layer may also be any of the following ranges: 400 nm to 800 nm, 400 nm to 600 nm, 200 nm to 600 nm, 200 nm to 800 nm, etc.

[0221] The aforementioned modulation of the binding energy of Pb and I can effectively avoid interface defects and the resulting energy level pinning even when the perovskite layer has a large thickness, and achieve effective interface charge transport, which is beneficial to effectively improve the energy conversion efficiency of optoelectronic devices with thick perovskite layers.

[0222] In some embodiments of this application, the perovskite layer satisfies one or more of the following characteristics in the direction perpendicular to the thickness of the perovskite layer:

[0223] (a1) The Moran index of J1-J2 is less than or equal to 0.2, optionally less than or equal to 0.15, and may also be less than or equal to any of the following values, or be any of the following values, or be selected from a range consisting of any two of the following values: 0.02, 0.04, 0.06, 0.08, 0.10, 0.12, 0.14, 0.15, 0.16, 0.18, 0.2, etc.;

[0224] (a2) The Moran index of J4-J3 is less than or equal to 0.2, optionally less than or equal to 0.15, and may also be less than or equal to any of the following values, or be any of the following values, or be selected from a range consisting of any two of the following values: 0.02, 0.04, 0.06, 0.08, 0.10, 0.12, 0.14, 0.15, 0.16, 0.18, 0.2, etc.;

[0225] (a3) The perovskite layer includes bromine; the Br content of bromine in the first region... - The binding energy of 3d orbital electrons is denoted as J5, and the Br₂ of bromine in the second region is... - The binding energy of the 3d orbital electron is denoted as J6; wherein the Moran index of J6-J5 is less than or equal to 0.2, optionally less than or equal to 0.15, and may also be less than or equal to any of the following values, or be any of the following values, or be selected from a range consisting of any two of the following values: 0.02, 0.04, 0.06, 0.08, 0.10, 0.12, 0.14, 0.15, 0.16, 0.18, 0.2, etc.

[0226] In some embodiments of this application, the Moran index of J1-J2 in the direction perpendicular to the thickness of the perovskite layer is greater than or equal to 0.

[0227] In some embodiments of this application, the Moran index of J4-J3 in the direction perpendicular to the thickness of the perovskite layer is greater than or equal to 0.

[0228] In some embodiments of this application, the Moran index of J6-J5 in the direction perpendicular to the thickness of the perovskite layer is greater than or equal to 0.

[0229] By controlling one or more of the aforementioned parameters within the range of the Moran index in the direction perpendicular to the thickness of the perovskite layer, it is beneficial to achieve more uniform in-plane control of the aforementioned binding energy shift vector, which is beneficial to better improve energy conversion efficiency and device stability.

[0230] In this application, unless otherwise stated, "Moran's I" has a well-known statistical meaning and is a classic statistic used to measure spatial autocorrelation. In this application, it is used to measure the uniformity of spatial data point distribution. When the Moran's I is approximately 0, there is no significant spatial correlation, corresponding to random uniformity of data points. When the Moran's I is greater than 0, the larger the value, the stronger the positive correlation of data points, the more obvious the "clustering" or "patching" characteristics of the data point distribution, and the worse the uniformity of data point distribution. When the Moran's I is less than 0, the data points show a significant negative correlation, with high and low values ​​regularly repelling and interleaving each other. In the extreme case, when it approaches -1, high and low values ​​maximize mutual repulsion and interleaving.

[0231] In some embodiments of this application, the Moran index involved is greater than or equal to 0.

[0232] When calculating the Moran's exponents of parameters J1-J2, J4-J3, J6-J5, etc., in the context, the following parameters are handled in the following manner:

[0233] 1. Parameters to be analyzed at different locations: Obtain the values ​​of the parameters to be analyzed at different locations within the region to be analyzed.

[0234] 2. Calculate the Moran index (I) using the selected statistical formula:

[0235]

[0236] Where n is the number of data points; W is the sum of all weights; ij x is an element in the spatial weight matrix; i and x j These are the parameter values ​​for the i-th and j-th positions; This is the average value of all position parameter values.

[0237] 3. Setting the spatial weight matrix:

[0238] The spatial weight matrix uses inverse distance weights, i.e. ,in The distance between the i-th and j-th positions is... p is the distance attenuation parameter; unless otherwise specified, p is 2.

[0239] 4. Statistical area and sampling interval of data points: The statistical area is 10 μm × 10 μm, and the sampling interval of data points is 50 nm.

[0240] In some embodiments of this application, the Moran index of the potential distribution of the first surface is less than or equal to 0.2, optionally less than or equal to 0.12, and may also be less than or equal to any of the following values, or be any of the following values, or be selected from a range consisting of any two of the following values: 0.02, 0.04, 0.06, 0.08, 0.10, 0.12, 0.14, 0.15, 0.16, 0.18, 0.2, etc.; wherein, the potential of the first surface is obtained by measuring the potential of the first surface using a Kelvin atomic force microscope.

[0241] In some embodiments of this application, the Moran index of the potential distribution on the first surface is greater than or equal to 0.

[0242] In this application, unless otherwise stated, the "Moran index of the potential distribution of the first surface" is obtained by Kelvin atomic force microscopy (KPFM) combined with Moran index analysis.

[0243] The instrument used for KPFM testing can be Bruker FastScan Bio.

[0244] KPFM testing can be performed as follows: By observing the change in electrostatic force between the probe and the sample, when the probe approaches the surface to be tested, due to the difference in their work functions, electrons will flow from the high Fermi level to the low Fermi level until the Fermi level is flattened. The contact potential difference can be deduced from the work function difference during this process, thereby obtaining potential data. By further combining in-plane scanning, the potential distribution data of the surface to be tested can be obtained.

[0245] By controlling the potential distribution of the first surface within the aforementioned range, a more uniform potential distribution can be achieved, which in turn facilitates more uniform and efficient extraction of charge at the perovskite interface, thus improving energy conversion efficiency. Furthermore, it also helps improve charge transport stability at the perovskite interface, thereby enhancing device stability.

[0246] In some embodiments of this application, the band gap of the perovskite layer is 1.2 eV to 2.2 eV, and may also be any of the following values ​​or a range selected from any two of the following values: 1.2 eV, 1.3 eV, 1.4 eV, 1.5 eV, 1.6 eV, 1.8 eV, 2.0 eV, 2.2 eV, etc.

[0247] In some embodiments of this application, the band gap of the second region in the perovskite layer is 1.2 eV to 2.2 eV, and may also be any of the following values ​​or a range selected from any two of the following values: 1.2 eV, 1.3 eV, 1.4 eV, 1.5 eV, 1.6 eV, 1.8 eV, 2.0 eV, 2.2 eV, etc.

[0248] In this application, unless otherwise specified, "band gap" has a commonly known meaning in the art and can be analyzed, compared, and confirmed using conventional methods within the art. Without limitation, the band gap of a material can be determined by its absorption or emission spectra; commonly used optical methods include ultraviolet-visible absorption spectroscopy, photoluminescence spectroscopy, and Raman spectroscopy.

[0249] In this application, unless otherwise specified, the terms "conduction band bottom (CBM)," "Fermi level (EF)," "valence band top (VBM)," and "band gap (Eg)" for semiconductor materials have their commonly known meanings in the art. Unless otherwise specified, the energy levels of CBM, EF, and VBM are all based on the vacuum level, and all energy levels of CBM, EF, and VBM are negative. EF is located between CBM and VBM, and CBM is closer to the vacuum level; that is, the energy level structure from top to bottom is vacuum level, CBM, EF, and VBM. The band gap is the distance between the conduction band bottom and the valence band top, Eg = CBM - VBM.

[0250] In this application, unless otherwise specified, "vacuum level" has a well-known meaning in the art, referring to the absolute zero point of electron potential energy, corresponding to the energy benchmark of an electron freely at rest outside a material, and numerically equal to the minimum energy required for an electron to completely escape the constraints of the material itself. The vacuum level provides a common benchmark for comparing the energy levels of different semiconductor materials. The "Fermi level" refers to the highest energy level occupied by an electron at T=0K; the "work function" refers to the minimum energy required to move an electron from the interior of a solid to its surface. Numerically, the work function is equal to the difference between the vacuum level and the Fermi level.

[0251] The aforementioned binding energy modulation method can be universally applied to a wide range of perovskite layer band gaps. When the band gap of the perovskite layer is in the range of 1.5 eV to 1.65 eV, it is beneficial to achieve higher perovskite crystal quality, thereby improving energy conversion efficiency. When the band gap of the perovskite layer is narrower or wider, the aforementioned binding energy modulation method can better compensate for the adverse effects of decreased crystal quality and increased surface defect concentration on energy efficiency.

[0252] Those skilled in the art can use methods known or existing in the art to obtain the “conduction band bottom (CBM),” “Fermi level (EF),” “valence band top (VBM),” and “band gap (Eg)” of the perovskite material in the perovskite layer.

[0253] By sputtering the sample surface layer by layer and combining it with UPS surface scanning tests, the in-plane energy level structure distribution information at different depths is obtained. For example, the energy level data of the perovskite material in the first and second regions can be obtained by testing the following method: obtain the perovskite layer of the sample to be tested exposed on the first surface, first perform an absorption spectral scan, and then perform a UPS full-spectrum scan and E... cutoff The sample is then scanned using both bubbly and ephemeral (Ev) scans to obtain the energy level positions of the CBM, EF, and VBM in the first region, and the band gap can be calculated. Subsequently, the sample is peeled layer by layer until the region corresponding to the thickness to be measured is exposed. An absorption spectral scan is then performed, followed by a UPS full-spectrum and Ev scan. cutoff Ev scanning yields the energy level structures CBM, EF, and VBM corresponding to the thickness, and the band gap (Eg) can be calculated. This process is repeated with etching, UPS full-spectrum scanning, and Ev scanning. cutoff The scanning and Ev scanning processes can obtain the energy level structures CBM, EF, and VBM of each target region, including but not limited to the energy level structure information of the second region (corresponding to the perovskite bulk phase). The CBM, EF, VBM, and band gap (Eg) data of the first and second regions can be compared to obtain the changes in the perovskite energy level structure regulated at the interface where the first surface is located relative to the energy level structure of the perovskite bulk phase.

[0254] The thickness of each layer during the peeling process can be adjusted according to the thickness of the perovskite layer. For example, when the perovskite layer thickness is 400 nm, information can be collected at different thicknesses with intervals of 20 nm to 100 nm. For instance, an absorption spectrum scan of the sample surface can be performed first, followed by UPS full-spectrum and E... cutoff Ev scan, followed by absorption spectral scans at 25 nm intervals near the interface (approximately 100 nm), and then UPS full spectrum and E... cutoff E v The scanning process involves performing a UPS surface scan of the remaining bulk phase region every 50 nm until the lower interface region is detected. This allows us to obtain the energy level structure information of the perovskite bulk phase and the lower interface.

[0255] Absorption spectroscopy scanning refers to ultraviolet-visible-near-infrared absorption spectroscopy, which can obtain a spectrum showing the change in the absorptivity of incident light with the wavelength of photons, and can obtain information including but not limited to band gap.

[0256] UPS full-spectrum scanning uses ultraviolet light as the excitation source to excite electrons in the sample and measure the kinetic energy distribution of these photoelectrons.

[0257] E cutoff The Secondary Electron Cutoff (SEC) scan is used to measure the high-energy region of the "secondary electron cutoff" and obtain work function data.

[0258] Ev (Valence band spectrum) scans measure a fine spectrum from the vicinity of the Fermi level to the top of the valence band.

[0259] Taking a perovskite layer sample from one embodiment as an example, the perovskite layer thickness is 450 nm. The 20 nm thickness region of the perovskite layer closest to the FTO side is defined as the lower interface region. The perovskite layer portion within a 20 nm range of the thickness center region is used to represent the bulk phase of the perovskite layer (the second region is included in the bulk phase portion). The 20 nm thickness region of the perovskite layer on the other side is defined as the upper interface region of the perovskite layer. A first region exists within either the lower interface region or the upper interface region.

[0260] Examples of instruments used to acquire perovskite material in perovskite layers include models such as the Thermo Fisher Scientific ESCALAB QXi, which can perform both UPS and XPS scans.

[0261] The X-ray photoelectron spectroscopy (XPS) test procedure can be as follows:

[0262] Elemental distribution information at different depths can be obtained by sputtering the sample surface layer by layer and combining it with full elemental scanning. The depth sampling depth of XPS testing is 0.5 nm to 10 nm, achieved through ion sputtering (such as Ar⁺, C⁺). 0 The sample is peeled off layer by layer using either a cluster ion beam or an ion beam, and XPS full spectrum or specific elemental spectrum is acquired after each layer is peeled off. The thickness of each layer can be adjusted according to the thickness of the perovskite layer. For example, when the thickness of the perovskite layer is 400 nm, information can be acquired at different thicknesses by peeling off layers at intervals of 20 nm to 100 nm.

[0263] XPS testing can be used to determine the location of different thicknesses of the perovskite layer, thereby allowing the selection of an appropriate etching ion beam rate. Then, UPS is used to perform band structure testing on the target area.

[0264] The UPS testing process can be as follows:

[0265] (i) First, the 450 nm perovskite layer film is etched using an Ar+ ion beam. Then, the signal of a selected element (such as Pb) in the perovskite crystal phase of the perovskite layer is detected. 4f (Related signals) to determine the etching location, pending Pb 4f When the signal intensity drops to 1 / e of the plateau intensity, it is defined as the perovskite etching is complete, and the etching rate of the perovskite layer by the ion beam is calculated. Among them, the signal of the selected element in the perovskite crystal phase has a high concentration in the perovskite layer, and it is easy to form a region with the elements of the possible adjacent structural layers, thereby determining the boundary between the perovskite layer and the possible adjacent structural layers.

[0266] (ii) Identify the sample to be tested, first perform an absorption spectrum scan, then perform UPS full spectrum and E... cutoff Ev scanning was performed to obtain the corresponding CBM, EF, and VBM positions; then etching was performed to expose the center region of the thickness, followed by an absorption spectroscopy scan, and then UPS full spectrum and Ev scanning were performed. cutoff Energy level structures of the perovskite bulk phase were obtained by Ev scanning.

[0267] In some embodiments of this application, the perovskite layer includes a first additive located in a region of the perovskite layer near the first surface; the first additive is an organic material. In some embodiments, the first additive includes at least one selected from the following: a hydrocarbon halide amine or its corresponding salt, a heteroaryl Lewis base, a polar polymer, polystyrene, and polyethylene glycol; wherein the polar polymer contains a polar group located on its side chain, and the polar group includes a carboxylic acid C. 1-4 One or more of alkyl esters and cyano groups.

[0268] In some embodiments, the halogen in the alkyl halogenated amine or its corresponding salt includes at least one of chlorine and bromine.

[0269] In some of these embodiments, the halogen in the hydrocarbon halide amine or its corresponding salt includes iodine.

[0270] In some embodiments, the heteroaryl Lewis base contains at least one of a pyridine ring and a thiophene ring. Non-limiting examples of heteroaryl Lewis bases may include at least one of pyridine and thiophene.

[0271] In some embodiments, the polar polymer includes polymethacrylic acid C 1-3 Alkyl esters, polyacrylic acid C 1-3 One or more of alkyl esters and polyacrylonitrile, and may further include one or more of polymethyl methacrylate, polymethyl acrylate and polyacrylonitrile.

[0272] By introducing the aforementioned type of first additive into the region near the first surface (e.g., the first region can be controlled to contain the first additive), the electron-donating and / or electron-withdrawing groups in the first additive can occupy the charge curve in the perovskite crystal. For example, they can occupy positively charged defects such as iodine vacancies, and negatively charged defects such as lead vacancies. Through the interaction between the first additive and the perovskite defects in the region near the first surface, the Pb at the perovskite layer interface can be better controlled. 2+ The sum of 4f orbital electrons and I - The binding energy shift vector of 3d orbital electrons can passivate various defects and improve energy conversion efficiency. In addition, it can help avoid significant lattice distortion and the resulting lattice stress, thus enabling long-term and effective passivation of interface defects and improving device stability.

[0273] In some embodiments of this application, the molar percentage of the first additive relative to the first perovskite material is 1% to 20%, optionally 1% to 10%, and may also be any of the following percentages or a range selected from any two of the following percentages: 1%, 2%, 3%, 4%, 5%, 6%, 7%, 8%, 9%, 10%, 12%, 14%, 15%, 16%, 18%, 20%, etc. The molar amount of the first perovskite material is calculated based on the molar amount of divalent cations in the first perovskite material. Unless otherwise specified, the atomic ratio of monovalent anions in the first perovskite material is equal to 3. In this case, the first perovskite material mainly has an ABX3 type structure. This is beneficial for better exerting the aforementioned effects of the first additive.

[0274] In some embodiments of this application, the first additive comprises a hydrocarbon haloamine or its corresponding salt. The carbon atoms in the hydrocarbon haloamine can be 6 to 20, or any of the following values ​​or a range selected from any two of the following values: 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20.

[0275] In some embodiments of this application, the first additive includes C 6-20 Hydroxyl halogenated amines or their corresponding salts. C 6-20 The number of carbon atoms in a hydrocarbon haloamine can be 6 to 20, or any of the following values ​​or a range selected from any two of the following values: 6, 8, 10, 12, 14, 16, 18, 20, etc.

[0276] In some embodiments of this application, the alkyl halide amine satisfies one or more of the following characteristics:

[0277] (1) The number of carbon atoms in the hydrocarbon haloamine is 6~20, and can be 6~10;

[0278] (2) The hydrocarbon group in the hydrocarbon halogenated amine is an aliphatic hydrocarbon group, which can be alkyl or alkenyl;

[0279] (3) The hydrocarbon group in the hydrocarbon halide amine is a chain hydrocarbon group, which can be selected as a straight chain hydrocarbon group.

[0280] In this application, unless otherwise specified, "hydrocarbon group" refers to an organic group consisting of carbon and hydrogen atoms. Hydrocarbon groups can be alkyl, aryl, or aralkyl. The definitions of alkyl and aryl are provided in the relevant descriptions within the context of this application.

[0281] In this application, "aliphatic hydrocarbon group" refers to the residue formed after an aliphatic hydrocarbon loses at least one hydrogen atom. Unless otherwise specified, "aliphatic hydrocarbon group" in this application specifically refers to a monovalent aliphatic hydrocarbon group. Aliphatic hydrocarbon groups include saturated aliphatic hydrocarbon groups and unsaturated aliphatic hydrocarbon groups.

[0282] In this application, the term "alkyl" refers to a monovalent residue formed by the loss of a hydrogen atom from a saturated hydrocarbon containing a primary (normal) carbon atom, or a secondary carbon atom, or a tertiary carbon atom, or a quaternary carbon atom, or a combination thereof. Suitable examples include, but are not limited to: methyl (Me, -CH3), ethyl (Et, -CH2CH3), 1-propyl (n-Pr, n-propyl, -CH2CH2CH3), 2-propyl (i-Pr, i-propyl, -CH(CH3)2), 1-butyl (n-Bu, n-butyl, -CH2CH2CH2CH3), 2-methyl-1-propyl (i-Bu, i-butyl, -CH2CH(CH3)2), 3,3-dimethyl-2-butyl (-CH(CH3)C(CH3)3) and octyl (-(CH2)7CH3), etc.

[0283] In this application, the term "alkenyl" refers to a monovalent residue formed by the loss of a hydrogen atom from an unsaturated hydrocarbon containing a primary (or secondary) carbon atom or a combination thereof. Suitable examples include, but are not limited to: methyl (Me, -CH3), ethyl (Et, -CH2CH3), 1-propyl (n-Pr, n-propyl, -CH2CH2CH3), 2-propyl (i-Pr, i-propyl, -CH(CH3)2), 1-butyl (n-Bu, n-butyl, -CH2CH2CH2CH3), 2-methyl-1-propyl (i-Bu, i-butyl, -CH2CH(CH3)2), 3,3-dimethyl-2-butyl (-CH(CH3)C(CH3)3) and octyl (-(CH2)7CH3), etc.

[0284] In this application, the term "alkane group" refers to a group formed when an alkane loses one hydrogen atom, in which all carbon atoms are connected by carbon-carbon single bonds and do not form a ring, and the remaining valence bonds are combined with hydrogen atoms. This includes straight-chain alkane groups and branched-chain alkane groups.

[0285] In some embodiments of this application, the alkyl halogenated amines include one or more of phenylethyl iodide, propyl ammonium chloride, 1,3-propanediamine dihydroiodate, octyl ammonium chloride, octyl ammonium bromide, 9-octadecenyl ammonium chloride, and the context example types.

[0286] In some embodiments of this application, the first additive includes C 6-20 Hydrocarbon-based halogenated amines.

[0287] Figure 5 This is a schematic diagram of the structure of the perovskite layer 100 in an optoelectronic device according to an embodiment of this application. The perovskite layer 100 contains a first additive 111 in the region near the first surface 101 (corresponding to the fourth region).

[0288] In this application, unless otherwise specified, the region in the perovskite layer where the first additive is distributed may be referred to as the fourth region.

[0289] In some embodiments of this application, the fourth region is located between the first surface 101 and the second region 120, as can be seen in [reference]. Figure 5 .

[0290] In some embodiments of this application, the fourth region may or may not overlap with the first region. Furthermore, when the fourth region overlaps with the first region, they may overlap completely or partially.

[0291] In some of these embodiments, the perovskite layer satisfies any one of the following characteristics:

[0292] (i) The halogens in the hydrocarbon halogenated amines or their corresponding salts include one or more of chlorine and bromine;

[0293] At this point, the aforementioned first type of additive is beneficial for better passivation of defects while controlling the lattice to avoid significant distortion, thereby improving energy conversion efficiency and device stability.

[0294] Optionally, the second surface is used for light incident, and the first surface is used for electron transport. In this case, hydrocarbon-based haloamines or their corresponding salts are beneficial for passivation doping with chlorine (Cl) and bromine (Br) elements to regulate the energy level structure at the interface of the first surface, so that the adjacent functions of the perovskite layer and the first surface side have better energy level matching, thereby improving the ability of the interface to transport electrons. This is beneficial for improving the ability of the interface at the first surface to collect photogenerated carriers (electrons) near the second surface, and for improving the photoelectric conversion efficiency.

[0295] (ii) The halogens in alkyl halogenated amines or their corresponding salts include iodine;

[0296] Optionally, the second surface is used for light incident, and the first surface is used for hole transport. In this case, hydrocarbon-based haloamines or their corresponding salts are beneficial for passivation doping with iodine (I) to modulate the energy level structure at the interface of the first surface, so that the adjacent functions of the perovskite layer and the first surface side have better energy level matching, thereby improving the ability of the interface to transport holes. This is beneficial for improving the ability of the interface at the first surface to collect photogenerated carriers (holes) near the second surface, and for improving the photoelectric conversion efficiency.

[0297] In some embodiments of this application, the first region contains a first additive.

[0298] When the first additive has doping characteristics in the first region at the interface of the perovskite layer, it is beneficial to form an interfacial electric field, thereby further improving the ability to extract interfacial charges and better improving energy conversion efficiency.

[0299] In some embodiments of this application, the perovskite layer includes a halogen, and the perovskite layer satisfies one or more of the following characteristics (any numerical parameter of the following characteristics may also be selected from any suitable value or range in the context):

[0300] (b1) The molar percentage of iodine in the halogen of the perovskite layer is 10% to 100%, which can be 80% to 100%, or any of the following percentages or a range of any two of the following percentages: 10%, 15%, 20%, 25%, 30%, 40%, 50%, 60%, 70%, 80%, 90%, 100%, etc.

[0301] (b2) The molar percentage of bromine in the halogens of the perovskite layer is 0% to 90%, which can be 0% to 20%, or any of the following percentages or a range of any two of the following percentages: 0%, 10%, 15%, 20%, 25%, 30%, 40%, 50%, 60%, 70%, 80%, 90%, etc.

[0302] (b3) If the molar ratio of lead to halogen in the perovskite layer is q:3, then q is 0.5~1, which can be 0.9~1, or any of the following values ​​or a range of any two of the following values: 0.5, 0.55, 0.6, 0.65, 0.7, 0.75, 0.8, 0.85, 0.9, 0.95, 1, etc.

[0303] By controlling the molar ratio of iodine in the halogens of the perovskite layer within the aforementioned range, the first perovskite material can contain more iodine, which is beneficial for perovskite lattice stability, moderate band gap, and sufficient light absorption.

[0304] By controlling the molar proportion of bromine in the halogens of the perovskite layer within the aforementioned range, the first perovskite material can contain a certain amount of bromine, which is beneficial for regulating the band gap and crystallization kinetics of the perovskite.

[0305] By controlling the molar ratio of iodine and bromine in the perovskite layer within the aforementioned range, it is beneficial to obtain high-quality perovskite crystals while maintaining a suitable band gap.

[0306] In some embodiments of this application, the perovskite layer comprises iodine and bromine, and further, the molar ratio of bromine to iodine is (0.01~0.9):(0.1~1).

[0307] In some embodiments of this application, the first perovskite material includes iodine and bromine, and further, the molar ratio of bromine to iodine is (0.01~0.9):(0.1~1).

[0308] In some embodiments of this application, the first perovskite material includes lead, iodine and bromine.

[0309] In some embodiments of this application, the area of ​​the perovskite layer is greater than or equal to 0.09 cm² in the direction perpendicular to the thickness of the perovskite layer. 2 .

[0310] The aforementioned modulation of the binding energy of Pb and I is beneficial for effectively passivating the aforementioned defects even when the perovskite layer has a large area, and is conducive to effectively improving the energy conversion efficiency and device stability of large-area optoelectronic devices.

[0311] When the size of the optoelectronic device is large, and the detection method involved in this application cannot cover the entire device area, an appropriate number of test samples can be selected based on the relative relationship between the area that the detection method can cover and the device area. For example, a reasonably distributed and appropriately sized sampling area can be selected on a projection plane perpendicular to the Z direction. The qualitative analysis results of each area are used to determine whether it meets the corresponding characteristics, and the average value is calculated based on the quantitative analysis results of each area as the test value. For example, for an area of ​​1 square meter (m²)... 2 For devices with this capability, ≥4 (e.g., ~9) regions can be selected for detection.

[0312] In some embodiments of this application, the area of ​​the perovskite layer on the projection plane perpendicular to the Z direction can be any of the following values, or greater than or equal to any of the following values, or selected from a range consisting of any two of the following values: 0.09 cm 2 0.1 cm 2 0.12 cm 2 0.125 cm 2 0.15 cm 2 0.16 cm 2 0.175 cm 2 0.18 cm 2 0.2cm 2 0.22 cm 2 0.225 cm 2 0.25 cm 2 1 cm 2 4 cm 2 9 cm 2 10 cm 2 16 cm 2 20 cm 2 25 cm 2 36cm 2 49 cm 2 50 cm 2 60 cm 2 64 cm 2 65 cm 2 70 cm 2 80 cm 2 81 cm 2 90 cm 2 100 cm 2 120cm 2 121 cm 2 125 cm 2 130 cm 2 140 cm 2、144 cm 2 、150 cm 2 、160 cm 2 、169 cm 2 、170 cm 2 、180cm 2 、190 cm 2 、196 cm 2 、200 cm 2 、225 cm 2 、250 cm 2 、256 cm 2 、260 cm 2 、280 cm 2 、289 cm 2 、290cm 2 、300 cm 2 、320 cm 2 、324 cm 2 、325 cm 2 、330 cm 2 、350 cm 2 、360 cm 2 、361 cm 2 、370 cm 2 、380cm 2 、400 cm 2 、440 cm 2 、441 cm 2 、450 cm 2 、480 cm 2 、484 cm 2 、500 cm 2 、600 cm 2 、625 cm 2 、660cm 2 、676 cm 2 、680 cm 2 、700 cm 2 、720 cm 2 、729 cm 2 、730 cm 2 、780 cm 2 、784 cm 2 、800 cm 2 、820cm 2 、840 cm 2 、841 cm 2 、850 cm 2 、860 cm 2, 900 cm 2 , 950 cm 2 , 961 cm 2 , 980 cm 2 , 0.1 m 2 , 0.12 m 2 , 0.14 m 2 , 0.15 m 2 , 0.16 m 2 , 0.18 m 2 , 0.2 m 2 , 0.3 m 2 , 0.4 m 2 , 0.5 m 2 , 0.6 m 2 , 0.7 m 2 , 0.8 m 2 , 0.9 m 2 , 10000 cm 2 (1 m 2 ), 1.1 m 2 , 1.2 m 2 , 1.3 m 2 , 1.4 m 2 , 1.5 m 2 , 1.6 m 2 , 1.7 m 2 , 1.8 m 2 , 1.9 m 2 , 2 m 2 , 2.1 m 2 , 2.2 m 2 , 2.3 m 2 , 2.4 m 2 , 2.5 m 2 , 2.6 m 2 , 2.7 m 2 , 2.8 m 2 , 2.9 m 2 , 3 m 2 , 3.2 m 2 , 3.4 m 2 , 3.5 m 2 , 3.6 m 2 , 3.7 m 2 , 3.8 m 2 , 4 m 2 , 4.2 m 2 , 4.4 m 2 , 4.5 m 2 etc.

[0313] In some embodiments of this application, the optoelectronic device includes a photovoltaic device or a light-emitting device.

[0314] The aforementioned perovskite layer can be used in photovoltaic devices or light-emitting devices, which helps to improve the energy conversion efficiency of photovoltaic devices or light-emitting devices.

[0315] In some embodiments of this application, the optoelectronic device includes a photovoltaic device.

[0316] In some of these embodiments, the optoelectronic device satisfies one or more of the following characteristics:

[0317] (c1) The perovskite layer is contained in the inverse or formal structure of the optoelectronic device;

[0318] (c2) The optoelectronic device includes a first charge transport layer and a second charge transport layer, with a perovskite layer disposed between the first charge transport layer and the second charge transport layer, a first surface facing the first charge transport layer, and a second surface facing the second charge transport layer; wherein, one of the first charge transport layer and the second charge transport layer is a hole transport layer, and the other is an electron transport layer.

[0319] (c3) The optoelectronic device includes a first electrode and a second electrode, a perovskite layer is disposed between the first electrode and the second electrode, the first surface faces the first electrode and the second surface faces the second electrode.

[0320] The aforementioned implementation methods can be universally applied to photovoltaic devices with either conventional or inverted structures, thereby improving photoelectric conversion efficiency. Furthermore, they can also enhance device stability.

[0321] In some embodiments of this application, the optoelectronic device includes a photovoltaic device, with the second surface located on the light-incident side of the perovskite layer. This not only allows the perovskite layer to have better light absorption capabilities, potentially increasing short-circuit current density and open-circuit voltage, but also helps reduce the transport path of charge carriers in the perovskite layer, thus promoting effective carrier collection and ultimately contributing to higher photoelectric conversion efficiency.

[0322] In the thickness direction of the perovskite layer, for a photovoltaic device, when light can be incident on only one side, that side is called the "light-incident side"; when light can be incident on both sides of the photovoltaic device, the side with higher device efficiency (PCE) when light is incident is defined as the "light-incident side".

[0323] In some embodiments of this application, the optoelectronic device includes a photovoltaic device. Where the first surface is used for electron transport, the photovoltaic device includes an electron transport layer stacked with the perovskite layer, with the first surface facing the electron transport layer; or...

[0324] When the first surface is used for hole transport, the photovoltaic device includes a hole transport layer stacked with the perovskite layer, with the first surface facing the hole transport layer.

[0325] When the first surface is used for electron transport, the electron transport layer is located on the side close to the first surface of the perovskite layer, utilizing the Pb in the first region of the perovskite layer. 2+ The sum of 4f orbital electrons and I - The binding energy shift of 3d orbital electrons is beneficial to improving electron transport efficiency, which can enable optoelectronic devices to achieve higher photoelectric conversion efficiency.

[0326] When the first surface is used for hole transport, the hole transport layer is located on the side close to the first surface of the perovskite layer, utilizing the Pb region of the first perovskite layer. 2+ The sum of 4f orbital electrons and I - The binding energy shift of 3d orbital electrons is beneficial to improving the hole transport efficiency, which can enable optoelectronic devices to achieve higher photoelectric conversion efficiency.

[0327] In some embodiments of this application, the optoelectronic device includes a first charge transport layer 310, a perovskite layer 100, and a second charge transport layer 320 stacked together. The first charge transport layer 310 and the second charge transport layer 320 are respectively disposed on opposite sides of the perovskite layer 100 in the thickness direction (Z direction) of the perovskite layer. (See reference...) Figure 6 . Figure 6 In the illustrated embodiment, the perovskite layer and the first and second charge transport layers located on either side are respectively disposed adjacent to each other. It is understood that the first and second charge transport layers can be disposed independently without being adjacent to the perovskite layer. For example, other functional layers, such as one or more of a barrier layer, buffer layer, and interface layer, can be disposed between at least one of the first and second charge transport layers and the perovskite layer. One of the first charge transport layer 310 and the second charge transport layer 320 can be a hole transport layer, and the other can be an electron transport layer. In some embodiments, the first surface faces the electron transport layer, and the second surface faces the hole transport layer.

[0328] Figure 7 yes Figure 6The schematic diagram shows a partial structure of the optoelectronic device. The optoelectronic device includes a first charge transport layer 310, a perovskite layer 100, and a second charge transport layer 320 stacked together. The perovskite layer 100 is located between the first charge transport layer 310 and the second charge transport layer 320. The perovskite layer 100 has a first surface 101 and a second surface 102 that are opposite to each other in the thickness direction (Z direction). The perovskite layer 100 includes a first region 110 near the first surface 101 and a second region 120 located in the bulk phase of the perovskite layer. The first region 110 is located between the first surface 101 and the second region 120. The first surface 101 faces the second charge transport layer 320, and the second surface 102 faces the first charge transport layer 310.

[0329] Figure 8 yes Figure 7 The schematic diagram of a partial structure of the optoelectronic device shown shows that the first charge transport layer 310 is a hole transport layer 610, and the second charge transport layer 320 is an electron transport layer 620.

[0330] In some embodiments of this application, the optoelectronic device includes a hole transport layer 610, a perovskite layer 100, and an electron transport layer 620 stacked together, with the perovskite layer 100 located between the hole transport layer 610 and the electron transport layer 620. The perovskite layer 100 has a first surface 101 and a second surface 102 that are opposite to each other in the thickness direction (Z direction). The perovskite layer 100 includes a first region 110 adjacent to the first surface 101 and a second region 120 located in the bulk phase portion of the perovskite layer. The first region 110 is located between the first surface 101 and the second region 120, with the first surface 101 facing the electron transport layer 620 and the second surface 102 facing the hole transport layer 610. See also... Figure 8 .

[0331] In some embodiments of this application, the photovoltaic device includes a first electrode and a second electrode, with a perovskite layer located between the first electrode and the second electrode.

[0332] In a photovoltaic device, one of the first electrode and the second electrode is a positive electrode, and the other is a negative electrode.

[0333] In photovoltaic devices, at least one of the first electrode and the second electrode is a transparent electrode. Either transparent electrode can be used for light incident.

[0334] In photovoltaic devices, both the first electrode and the second electrode are transparent electrodes.

[0335] Unless otherwise specified, if the first and second electrodes consist of only one transparent electrode, that transparent electrode is defined as the "incident electrode". If the photovoltaic device includes two transparent electrodes, the transparent electrode that provides higher device efficiency when light is incident on the corresponding transparent electrode is defined as the "incident electrode". In this case, the other electrode can be defined as the "back electrode".

[0336] It is understood that the incident light-side electrode is a transparent electrode. The back electrode may or may not be a transparent electrode; for example, the back electrode may be a metal electrode. The meanings of transparent electrode and metal electrode are well known to those skilled in the art, and their implications are understandable.

[0337] In some embodiments of this application, one of the "first electrode" and the "second electrode" is a transparent electrode for light incident. In some embodiments, the first electrode is a transparent electrode.

[0338] In some embodiments of this application, the second electrode is a metal electrode.

[0339] In some embodiments of this application, the first electrode is a transparent electrode and the second electrode is a metal electrode.

[0340] In some embodiments of this application, the optoelectronic device includes a first charge transport layer and a second charge transport layer, wherein the first charge transport layer and the second charge transport layer are located on opposite sides of the perovskite layer in the thickness direction of the perovskite layer. Further, one of the first charge transport layer and the second charge transport layer is an electron transport layer, and the other is a hole transport layer. In some embodiments, the first charge transport layer is a hole transport layer. In other embodiments, the first charge transport layer is an electron transport layer.

[0341] Figure 9 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of this application. The optoelectronic device 10 includes a first electrode 410, a first charge transport layer 310, a perovskite layer 100, a second charge transport layer 320, and a second electrode 420 stacked together. In the thickness direction (Z direction) of the perovskite layer, the first charge transport layer 310 and the second charge transport layer 320 are respectively disposed on opposite sides of the perovskite layer 100. The first electrode 410 is disposed on the side of the first charge transport layer 310 away from the perovskite layer 100, and the second electrode 420 is disposed on the side of the second charge transport layer 320 away from the perovskite layer 100. In some embodiments, the first electrode is a transparent electrode, and the second electrode is a metal electrode. It can be understood that one of the first charge transport layer 310 and the second charge transport layer 320 can be a hole transport layer, and the other can be an electron transport layer. In some embodiments, the first surface faces the electron transport layer, and the second surface faces the hole transport layer.

[0342] Figure 10 yes Figure 9 The schematic diagram of the optoelectronic device shown shows that the first charge transport layer 310 is a hole transport layer 610, and the second charge transport layer 320 is an electron transport layer 620. At this time, the optoelectronic device 10 includes a first electrode 410, a hole transport layer 610, a perovskite layer 100, an electron transport layer 620, and a second electrode 420 stacked together. In the thickness direction (Z direction) of the perovskite layer 100, the hole transport layer 610 and the electron transport layer 620 are respectively disposed on both sides of the perovskite layer 100. The first electrode 410 is disposed on the side of the hole transport layer 610 away from the perovskite layer 100, and the second electrode 420 is disposed on the side of the electron transport layer 620 away from the perovskite layer 100.

[0343] Figure 11 This is a schematic diagram of the structure of an optoelectronic device according to an embodiment of this application. The optoelectronic device 10 includes a substrate layer 500, a first electrode 410, a first charge transport layer 310, a perovskite layer 100, a second charge transport layer 320, and a second electrode 420 stacked together. In the thickness direction (Z direction) of the perovskite layer, the first charge transport layer 310 and the second charge transport layer 320 are respectively disposed on opposite sides of the perovskite layer 100. The first electrode 410 is disposed on the side of the first charge transport layer 310 away from the perovskite layer 100, and the second electrode 420 is disposed on the side of the second charge transport layer 320 away from the perovskite layer 100. The substrate layer 500 is disposed on the side of the first electrode 410 away from the perovskite layer 100. It can be understood that one of the first charge transport layer 310 and the second charge transport layer 320 can be a hole transport layer, and the other can be an electron transport layer. In some embodiments, the first surface faces the electron transport layer, and the second surface faces the hole transport layer.

[0344] In some embodiments of this application, the optoelectronic device can be a formal structure or an inverse structure.

[0345] In some embodiments of this application, the optoelectronic device is an inverted pin structure or a formal nip structure.

[0346] Figure 12This is a schematic diagram of the structure of an inverted optoelectronic device according to one embodiment of this application. The optoelectronic device 10 includes a substrate layer 500, an incident light-side electrode 700, a hole transport layer 610, a perovskite layer 100, an electron transport layer 620, and a back electrode 800, all stacked together. In the thickness direction (Z direction) of the perovskite layer, the hole transport layer 610 and the electron transport layer 620 are respectively disposed on opposite sides of the perovskite layer 100. The incident light-side electrode 700 is disposed on the side of the hole transport layer 610 away from the perovskite layer 100, and the back electrode 800 is disposed on the side of the electron transport layer 620 away from the perovskite layer 100. The substrate layer 500 is disposed on the side of the incident light-side electrode 700 away from the perovskite layer 100. In some embodiments, the first surface faces the electron transport layer, and the second surface faces the hole transport layer.

[0347] Figure 13 This is a schematic diagram of the formal structure of an optoelectronic device according to one embodiment of this application. The optoelectronic device 10 includes a substrate layer 500, an incident light-side electrode 700, an electron transport layer 620, a perovskite layer 100, a hole transport layer 610, and a back electrode 800, all stacked together. In the thickness direction (Z direction) of the perovskite layer, the hole transport layer 610 and the electron transport layer 620 are respectively disposed on opposite sides of the perovskite layer 100. The incident light-side electrode 700 is disposed on the side of the electron transport layer 620 away from the perovskite layer 100, and the back electrode 800 is disposed on the side of the hole transport layer 610 away from the perovskite layer 100. The substrate layer 500 is disposed on the side of the incident light-side electrode 700 away from the perovskite layer 100. In some embodiments, the first surface faces the electron transport layer, and the second surface faces the hole transport layer.

[0348] In some embodiments of this application, the optoelectronic device includes a photovoltaic device; the photovoltaic device includes a solar cell, and the solar cell includes a perovskite layer.

[0349] The aforementioned perovskite layer can be incorporated into solar cells to improve their photoelectric conversion efficiency. Furthermore, it can also enhance device stability.

[0350] In some embodiments of this application, the photovoltaic device includes a multijunction solar cell.

[0351] In this application, unless otherwise specified, a "multi-junction solar cell" refers to a solar cell in which two or more cell cells made of semiconductor active materials with different band gaps are stacked together in series optically and / or electrically. Multi-junction solar cells can broaden the absorption spectrum of solar cells, maximizing the conversion of light energy into electrical energy, and also help reduce thermal relaxation losses. Multi-junction solar cell design is an important way to overcome the Shockley-Queisser limit efficiency of single-junction solar cells. A multi-junction solar cell includes at least two cell cells, each cell cell including at least one light-absorbing layer, and each light-absorbing layer has a different band gap.

[0352] It is understandable that a "cell" in a multi-junction solar cell includes at least a light-absorbing layer. The light-absorbing layers in different cells can provide different band gaps.

[0353] In this application, unless otherwise specified, "battery cell" and "battery section" have the same meaning and can be used interchangeably.

[0354] In this application, unless otherwise specified, "light-absorbing layer" and "light-absorbing layer" have the same meaning and can be used interchangeably.

[0355] In this application, unless otherwise specified, "band gap" has a commonly known meaning in the art and can be analyzed, compared, and confirmed using conventional methods within the art. Without limitation, the band gap of a material can be determined by its absorption or emission spectra; commonly used optical methods include ultraviolet-visible absorption spectroscopy, photoluminescence spectroscopy, and Raman spectroscopy.

[0356] When solar cells are multi-junction solar cells, they are advantageous in improving the utilization rate of incident light, while also retaining the aforementioned advantages of high photoelectric conversion efficiency. Multi-junction solar cells can be monolithic integrated tandem solar cells or mechanically tandem solar cells, offering flexibility in form and a wide range of applications.

[0357] In some embodiments of this application, the photovoltaic device includes a solar cell, which is a multi-junction solar cell. The multi-junction solar cell includes a first cell unit, which includes a light-absorbing layer (which may be referred to as a first light-absorbing layer or first light-absorbing layer). The first light-absorbing layer may include the aforementioned perovskite layer.

[0358] The first light-absorbing layer includes a first semiconductor active material.

[0359] In some embodiments of this application, the first light-absorbing layer is the aforementioned perovskite layer. In this case, the first semiconductor active material includes the first perovskite material.

[0360] In some embodiments of this application, the optoelectronic device includes a solar cell, which is a multi-junction solar cell. The multi-junction solar cell includes a first cell unit, which includes a perovskite layer.

[0361] The aforementioned perovskite layer can be incorporated into multi-junction solar cells to improve their photoelectric conversion efficiency. Furthermore, it can also enhance device stability.

[0362] In some embodiments of this application, the multijunction solar cell further includes a second cell stacked with the first cell cell; the second cell cell and the first cell cell are connected by an interconnect layer, or the second cell cell and the first cell cell are isolated by an insulating layer; the second cell cell includes a light absorption layer (which may be referred to as the second light absorption layer or the second light-absorbing layer), and the second light absorption layer and the first light absorption layer have different band gaps.

[0363] In some embodiments of this application, the interconnect layer includes a carrier recombination layer or a tunneling layer. In some embodiments, the interconnect layer can be a carrier recombination layer or a tunneling layer.

[0364] In some embodiments of this application, the interconnect layer includes a carrier recombination layer.

[0365] In some embodiments of this application, the interconnect layer includes a tunneling layer.

[0366] In some embodiments of this application, the second light-absorbing layer and the perovskite layer have different band gaps. Thus, by providing multiple light-absorbing layers with different band gaps, the multi-junction solar cell can effectively absorb light of different wavelengths, broadening the spectral range of absorbed light and improving the photoelectric conversion efficiency of the multi-junction solar cell.

[0367] In some embodiments, the multijunction solar cell is a tandem solar cell.

[0368] In some embodiments of this application, the multijunction solar cell further includes a second cell stacked with the first cell cell; the second cell cell and the first cell cell are connected by an interconnect layer, or the second cell cell and the first cell cell are isolated by an insulating layer; the second cell cell includes a light-absorbing layer (i.e., a second light-absorbing layer), and the second light-absorbing layer and the perovskite layer have different band gaps.

[0369] By setting up multiple light-absorbing layers (perovskite layer and second light-absorbing layer) with different band gaps, multi-junction solar cells can effectively absorb light of different wavelengths, broaden the spectral range of light absorbed by multi-junction solar cells, and improve the photoelectric conversion efficiency of multi-junction solar cells.

[0370] In some embodiments of this application, the light-absorbing layer (i.e., the second light-absorbing layer) in the second battery cell includes a semiconductor active material (which may be referred to as the second semiconductor active material). The second semiconductor active material includes one or more of the following: a second perovskite material, a silicon-containing semiconductor material, copper zinc tin sulfide, copper zinc tin selenide, copper zinc tin selenide sulfide, copper indium gallium selenide, copper indium gallium diselenide, copper indium selenide, cadmium telluride, gallium arsenide, and organic active materials.

[0371] The aforementioned embodiments can be universally applied to the aforementioned different types of multi-junction solar cells.

[0372] In some embodiments of this application, a carrier recombination layer or a tunneling layer is provided between the monolithically integrated battery cells.

[0373] In this application, unless otherwise specified, the "carrier recombination layer" is a structural layer in which electrons and holes transported from two different battery cells recombine, enabling the two battery cells to achieve ohmic connection and share the positive and negative electrodes.

[0374] In some embodiments of this application, a carrier recombination layer is provided between the first battery cell and the second battery cell.

[0375] In some embodiments of this application, interconnection structures are provided between the battery cells connected in series, which can provide tunneling junctions (also known as tunneling layers) to realize tunneling conduction and electrical series connection between different battery cells, while maintaining optical transparency so that photons can pass smoothly through the previous battery cell to the next battery cell.

[0376] In some embodiments of this application, an interconnection structure is provided between the first battery cell and the second battery cell.

[0377] In some embodiments of this application, a tunnel junction may be formed between the first battery cell and the second battery cell.

[0378] In some embodiments of this application, the charge carrier recombination layer is a structural layer in which electrons transported from the first battery cell and holes transported from the second battery cell recombine, or in which holes transported from the first battery cell and electrons transported from the second battery cell recombine, thereby connecting the first battery cell and the second battery cell in series.

[0379] In some embodiments of this application, a multi-junction solar cell includes a first electrode, a perovskite layer, an interconnect layer, a second light-absorbing layer, and a second electrode stacked together. The interconnect layer is located between the perovskite layer and the second light-absorbing layer. The first electrode is located on the side of the perovskite layer facing away from the interconnect layer, and the second electrode is located on the side of the second light-absorbing layer facing away from the interconnect layer. Thus, two cell units in a multi-junction solar cell are connected through the interconnect layer to achieve current matching between the two cell units. This results in a relatively smaller size, the ability to absorb light of different wavelengths, a wider absorption spectrum range for the multi-junction solar cell, and an improved photoelectric conversion efficiency.

[0380] In some embodiments of this application, a multi-junction solar cell includes a first electrode, a perovskite layer, a third electrode, an insulating layer, a fourth electrode, a second light-absorbing layer, and a second electrode stacked together. The third electrode, insulating layer, and fourth electrode are stacked between the perovskite layer and the second light-absorbing layer. The third electrode is located on the side of the insulating layer facing the perovskite layer, and the fourth electrode is located on the side of the insulating layer facing the second light-absorbing layer. The first electrode is located on the side of the perovskite layer away from the third electrode, and the second electrode is located on the side of the second light-absorbing layer away from the fourth electrode. Thus, the multi-junction solar cell forms a mechanically stacked cell. The insulating layer isolates the two cell units, preventing direct conduction of charge carriers and eliminating the need for current matching. Furthermore, each cell has its own independent positive and negative electrodes for current extraction, allowing for flexible circuit adjustments.

[0381] In this application, unless otherwise specified, a multi-junction solar cell with two battery cells may also be referred to as a "tandem solar cell". A tandem solar cell may be a two-terminal structure or a four-terminal structure.

[0382] In some embodiments of this application, the tandem solar cell has a two-end structure. In this case, two cell units are directly connected in series through a tunneling layer or a carrier recombination layer. The tandem solar cell only has two output electrodes, one positive and the other negative, and the current between the two cell units remains consistent. This type of tandem solar cell can also be called a monolithic integrated tandem cell, which refers to cell units stacked along the thickness direction that are electrically connected in series between a pair of electrode layers. Different cell units are connected through a carrier recombination layer or a tunneling layer to achieve current matching between adjacent cell units, so that adjacent cell units form an integrated structure of electrical and optical series connection.

[0383] In some embodiments of this application, the tandem solar cell includes a first electrode, a first light-absorbing layer, a carrier recombination layer, a second light-absorbing layer, and a second electrode. The first light-absorbing layer and the second light-absorbing layer are respectively disposed on both sides of the carrier recombination layer. The first electrode is located on the side of the first light-absorbing layer away from the carrier recombination layer, and the second electrode is located on the side of the second light-absorbing layer away from the carrier recombination layer.

[0384] In some embodiments of this application, the tandem solar cell includes a first electrode, a first light-absorbing layer, a tunneling layer, a second light-absorbing layer, and a second electrode. The first light-absorbing layer and the second light-absorbing layer are respectively disposed on both sides of the tunneling layer. The first electrode is located on the side of the first light-absorbing layer away from the tunneling layer, and the second electrode is located on the side of the second light-absorbing layer away from the tunneling layer.

[0385] In some embodiments of this application, the tandem solar cell has a four-terminal structure. In this case, the cell cells are electrically independent and operate independently, with coupling between the cell cells only through optical means; no carrier recombination layer or tunneling layer is provided between the cell cells. Each cell cell has its own pair of electrodes (positive and negative), and the entire tandem solar cell has four electrical output terminals, corresponding to the four electrodes. Two cell cells are isolated in the stacking direction by an insulating layer to prevent short circuits between the two cell cells.

[0386] In some implementations, the bandgap of the perovskite layer (i.e., the first light-absorbing layer) is Eg2, where 1.65 eV ≤ Eg2 ≤ 2.2 eV; the bandgap of the second light-absorbing layer is Eg1, where 1.1 eV ≤ Eg1 ≤ 1.6 eV. This bandgap configuration of the perovskite layer and the second light-absorbing layer effectively absorbs both short-wavelength and long-wavelength light, improving the photoelectric conversion efficiency of the multi-junction solar cell. In this implementation, the cell unit corresponding to the second light-absorbing layer is a narrow-bandgap solar cell, and the cell unit corresponding to the perovskite layer is a wide-bandgap solar cell.

[0387] In some embodiments, the second light-absorbing layer comprises a layer of compounds including: a second perovskite material, a silicon-containing semiconductor material, copper zinc tin sulfide, copper zinc tin selenide, copper zinc tin selenide sulfide, copper indium gallium selenide, copper indium gallium diselenide, copper indium selenide, cadmium telluride, gallium arsenide, and organic active materials. These materials can absorb light of different wavelengths with the perovskite layer, thereby broadening the spectral range of light absorption in the multi-junction solar cell and improving its photoelectric conversion efficiency. In some embodiments of this application, the definition of the second perovskite material is the same as that of the first perovskite material, but the composition differs to obtain a second light-absorbing layer with a different bandgap, used to absorb light of different wavelengths with the perovskite layer, broadening the absorption spectral range of the multi-junction solar cell and improving its photoelectric conversion efficiency. Exemplarily, the second light-absorbing layer comprises a second perovskite material, thereby obtaining a perovskite-perovskite multi-junction solar cell. In another example, the second light-absorbing layer comprises a crystalline silicon material, thereby obtaining a perovskite-crystalline silicon multi-junction solar cell.

[0388] Organic active materials are typically composed of blends of electron donor and electron acceptor materials. Common electron donor materials include poly(3-hexylthiophene) (P3HT), wide-bandgap polymer donor PM6, and high-efficiency polymer donor D18, while common electron acceptor materials include fullerene acceptors (such as PC). 61 BM, PC 71 BM, etc.), and non-fullerene acceptors (such as Y6 series materials, indendrothiophene derivatives, BTP series, etc.). Exemplary organic active materials include PM6:Y6 and P3HT:PC. 61 One of BM, D18:BTP-eC9, etc. can be used to obtain multiple types.

[0389] Silicon-containing semiconductor materials include, but are not limited to, crystalline silicon materials or amorphous silicon materials. Crystalline silicon materials can include monocrystalline silicon or polycrystalline silicon.

[0390] In some embodiments, a multi-junction solar cell includes a first electrode and a second electrode, with a first light-absorbing layer and a second light-absorbing layer both located between the first electrode and the second electrode, the first light-absorbing layer being closer to the first electrode and the second light-absorbing layer being closer to the second electrode.

[0391] In some implementations, the first electrode in a multi-junction solar cell is a transparent electrode. This allows light to enter the multi-junction solar cell from the first electrode. Furthermore, the band gap of the second light-absorbing layer is Eg1, 1.1 eV ≤ Eg1 ≤ 1.6 eV; the band gap of the perovskite layer is Eg2, 1.65 eV ≤ Eg2 ≤ 2.2 eV. Thus, light entering from the first electrode first passes through the perovskite layer, where it absorbs short-wavelength light (such as ultraviolet to visible light), and then enters the second light-absorbing layer, where it absorbs longer-wavelength light (such as near-infrared light). This allows for greater utilization of different wavelengths of light, improving the photoelectric conversion efficiency of the multi-junction solar cell. Furthermore, the perovskite layer, acting as the top light-absorbing layer, absorbs ultraviolet-visible light, protecting the second light-absorbing layer, which acts as the bottom light-absorbing layer.

[0392] In other embodiments, the bandgap of the second light-absorbing layer is Eg3, where 1.65 eV ≤ Eg3 ≤ 2.2 eV; and the bandgap of the perovskite layer is Eg4, where 1.1 eV ≤ Eg4 ≤ 1.6 eV. Thus, the bandgap settings of the second light-absorbing layer and the perovskite layer can absorb short-wavelength and long-wavelength light respectively, improving the photoelectric conversion efficiency of the multi-junction solar cell. In this embodiment, the cell unit corresponding to the second light-absorbing layer is a wide-bandgap solar cell, and the cell unit corresponding to the perovskite layer is a narrow-bandgap solar cell.

[0393] In other embodiments, the second light-absorbing layer comprises a third perovskite material. Thus, the resulting multi-junction solar cell is a perovskite-perovskite multi-junction solar cell. In some embodiments of this application, the third perovskite material is defined as the same type as the first perovskite material described above, but with a different composition to obtain a second light-absorbing layer with a different bandgap. This layer is used to absorb light of different wavelengths with the perovskite layer, broadening the absorption spectrum range of the multi-junction solar cell and improving its photoelectric conversion efficiency. Exemplarily, the third perovskite material includes APbI. z Br 3-z The material shown is defined as above, where 0 < z < 3.

[0394] In other embodiments, the second electrode in a multi-junction solar cell is a transparent electrode. This allows light to enter the multi-junction solar cell through the second electrode. Furthermore, the band gap of the second light-absorbing layer is Eg3, 1.65 eV ≤ Eg3 ≤ 2.2 eV; the band gap of the perovskite layer is Eg4, 1.1 eV ≤ Eg4 ≤ 1.6 eV. Thus, light entering from the second electrode first passes through the second light-absorbing layer, which absorbs short-wavelength light (such as ultraviolet to visible light), and then enters the perovskite layer, where it absorbs longer-wavelength light (such as near-infrared light). This allows for greater utilization of different wavelengths of light, improving the photoelectric conversion efficiency of the multi-junction solar cell. Furthermore, the second light-absorbing layer, acting as the top cell's light-absorbing layer, absorbs ultraviolet-visible light, protecting the perovskite layer as the bottom cell's light-absorbing layer.

[0395] In some embodiments, a multi-junction solar cell includes a first electrode, a perovskite layer, an interconnect layer, a second light-absorbing layer, and a second electrode stacked together, with the interconnect layer located between the perovskite layer and the second light-absorbing layer. The interconnect layer may include a carrier recombination layer or a tunneling layer. Thus, the multi-junction solar cell forms a monolithic integrated tandem cell, with two cell units connected by an interconnect layer (e.g., through a carrier recombination layer or a tunneling layer) to achieve current matching between the two cell units. It has a relatively smaller size, can absorb light of different wavelengths, broadens the absorption spectrum range of the multi-junction solar cell, and improves the photoelectric conversion efficiency of the multi-junction solar cell.

[0396] In some embodiments, a multijunction solar cell includes a first electrode, a perovskite layer, a tunneling layer, a second light-absorbing layer, and a second electrode stacked together, with the tunneling layer located between the perovskite layer and the second light-absorbing layer.

[0397] In some implementations, a multijunction solar cell includes a first charge transport layer, a second charge transport layer, a third charge transport layer, and a fourth charge transport layer.

[0398] In this application, the first charge transport layer, the second charge transport layer, the third charge transport layer, and the fourth charge transport layer are used to transport the first charge carrier, the second charge carrier, the third charge carrier, and the fourth charge carrier, respectively. One of the first charge carrier and the second charge carrier is an electron and the other is a hole. One of the third charge carrier and the fourth charge carrier is an electron and the other is a hole.

[0399] In some embodiments, a multi-junction solar cell includes a first electrode, an optional first charge transport layer, a perovskite layer, an optional second charge transport layer, a carrier recombination layer or tunneling layer, an optional third charge transport layer, a second light-absorbing layer, an optional fourth charge transport layer, and a second electrode, all stacked together. In some embodiments, the multi-junction solar cell includes at least one of the first and second charge transport layers, and also includes a hole transport layer. Further, when all four charge carriers are present, the first and third charge transport layers are identical and selected from one of the electron transport layer and the hole transport layer, and the second and fourth charge transport layers are identical and selected from the other of the electron transport layer and the hole transport layer. Thus, a first electrode, an optional first charge transport layer, a perovskite layer, and an optional second charge transport layer form a first battery cell; an optional third charge transport layer, a second light absorption layer, an optional fourth charge transport layer, and a second electrode form a second battery cell. A carrier recombination layer is used to recombine and annihilate electrons generated from the perovskite layer and holes generated from the second light absorption layer (or holes generated from the perovskite layer and electrons generated from the second light absorption layer) that are transported towards the carrier recombination layer, thereby achieving low-ohmic tunnel recombination between the first battery cell containing the perovskite layer and the second battery cell containing the second light absorption layer, ensuring the connectivity between the two battery cells. A tunneling layer is located between the two battery cells, and its main function is to achieve efficient transport of electrons and holes. Through the tunneling effect, the tunneling layer allows electrons and holes to be transported from the bottom battery to the top battery, thereby reducing energy loss due to electron thermal relaxation and improving the photoelectric conversion efficiency of the battery. Exemplarily, the second light absorption layer includes a second perovskite material, thus resulting in a perovskite-perovskite multi-junction solar cell. In another example, the second light-absorbing layer comprises crystalline silicon, thereby resulting in a perovskite-crystalline silicon multijunction solar cell.

[0400] In some embodiments of this application, multi-junction solar cells may include all four charge transport layers simultaneously, or may include only one or more of them; this is not limited here. The presence of charge transport layers helps to extract and transport electrons or holes generated by the perovskite layer or the second light-absorbing layer, enhancing the extraction and transport effect of electrons and holes and improving the performance of the multi-junction solar cell. The materials for the corresponding electron transport layer and hole transport layer are selected as defined above; the materials for the electron transport layer or hole transport layer corresponding to the first and second cell units may be the same or different.

[0401] In some embodiments, a multi-junction solar cell includes a first electrode, a hole transport layer, a perovskite layer, an electron transport layer, a carrier recombination layer or a tunneling layer, an optional hole transport layer, a second light absorption layer, an optional electron transport layer, and a second electrode, all stacked together.

[0402] In this application, the carrier recombination layer comprises one or more of the following: metallic materials, transparent conductive oxides, and carbon materials. Further, the transparent conductive oxide layer comprises, but is not limited to, one or more of the following: fluorine-doped tin oxide (FTO), indium tin oxide (ITO), aluminum-doped zinc oxide (AZO), boron-doped zinc oxide (BZO), indium zinc oxide (IZO), tungsten-doped indium oxide (IWO), indium gallium zinc oxide (IGZO), and antimony-doped tin oxide (ATO). Further, the metallic materials include, but are not limited to, one or more of the following: gold, copper, silver, platinum, aluminum, and iron. Further, the carbon materials include, but are not limited to, one or more of the following: graphite, graphene, and carbon nanotubes.

[0403] In some implementations, the thickness of the carrier recombination layer is 0.1 nm to 200 nm. For example, it can be 0.1 nm, 0.8 nm, 1 nm, 2 nm, 10 nm, 30 nm, 50 nm, 90 nm, 100 nm, 130 nm, 150 nm, 160 nm, 200 nm, or any two of the above values ​​as endpoints.

[0404] In some implementations, the components of the tunneling layer include, but are not limited to, PEDOT (poly-3,4-ethylenedioxythiophene), transparent metal oxides, etc.

[0405] In other embodiments, a multi-junction solar cell includes a first electrode, a perovskite layer, a third electrode, an insulating layer, a fourth electrode, a second light-absorbing layer, and a second electrode stacked together. The third electrode, insulating layer, and fourth electrode are stacked between the perovskite layer and the second light-absorbing layer. The third electrode is positioned on the side of the insulating layer facing the perovskite layer, and the fourth electrode is positioned on the side of the insulating layer facing the second light-absorbing layer. In this way, the multi-junction solar cell forms a mechanically stacked cell. The insulating layer isolates the two cell units, preventing direct parallel connection of charge carriers and eliminating the need for current matching. Furthermore, each cell unit has its own independent positive and negative electrodes for current extraction, allowing for flexible circuit adjustments.

[0406] In this application, the fifth charge transport layer, the sixth charge transport layer, the seventh charge transport layer, and the eighth charge transport layer are used to transport the fifth charge carrier, the sixth charge carrier, the seventh charge carrier, and the eighth charge carrier, respectively. One of the fifth and sixth charge carriers is an electron and the other is a hole. One of the seventh and eighth charge carriers is an electron and the other is a hole.

[0407] In some embodiments, a multi-junction solar cell includes a first electrode, an optional fifth charge transport layer, a perovskite layer, an optional sixth charge transport layer, a third electrode, an insulating layer, a fourth electrode, an optional seventh charge transport layer, a second light-absorbing layer, an optional eighth charge transport layer, and a second electrode, all stacked together. In some embodiments, the multi-junction solar cell includes at least one of the fifth and sixth charge transport layers, and also includes a hole transport layer. Further, when all five to eight charge carriers are present, the fifth charge transport layer is selected from either a hole transport layer or an electron transport layer; the sixth charge transport layer is selected from either a hole transport layer or an electron transport layer different from the fifth charge transport layer; the seventh charge transport layer is selected from either a hole transport layer or an electron transport layer; and the eighth charge transport layer is selected from either a hole transport layer or an electron transport layer different from the seventh charge transport layer. The definitions and material selections of the corresponding hole transport layers or electron transport layers are as described above and will not be repeated here. Thus, a first electrode, optionally a fifth charge transport layer, a perovskite layer, optionally a sixth charge transport layer, and a third electrode form a first battery cell; a fourth electrode, optionally a seventh charge transport layer, a second light-absorbing layer, optionally an eighth charge transport layer, and a second electrode form a second battery cell. The first and second battery cells are electrically isolated by an insulating layer. Each battery cell has two electrodes, for a total of four electrodes. The circuits of the two battery cells are independent of each other, forming a four-terminal multi-junction solar cell. This allows for adjustment of the current in the multi-junction solar cell. Exemplarily, the second light-absorbing layer comprises a second perovskite material, resulting in a perovskite-perovskite multi-junction solar cell. In another example, the second light-absorbing layer comprises crystalline silicon, resulting in a perovskite-crystalline silicon multi-junction solar cell.

[0408] Furthermore, since the third and fourth electrodes are located in the middle of the multi-junction solar cell, in order to further increase the light energy utilization of the multi-junction solar cell and enable the remaining light after absorption by one cell to enter the next cell, the third and fourth electrodes can be set as light-transmitting electrodes, and the materials can be selected from one or more of the above-mentioned transparent conductive oxides.

[0409] In some embodiments, the material of the insulating layer includes, but is not limited to, glass or an insulating adhesive. Further, the glass is transparent glass; further, the insulating adhesive is a transparent adhesive.

[0410] In some embodiments, the multi-junction solar cell may also include multi-junction solar cells composed of 3, 4, or 5 cells, such as 3-junction solar cells, 4-junction solar cells, 5-junction solar cells, etc., and may be mechanically stacked cells, monolithically integrated stacked cells, or hybrid stacked cells composed of both, without limitation here.

[0411] Without limitation, the hole transport material in the hole transport layer may include, but is not limited to, one or more of the following materials and their derivatives: hole transport organic materials and hole transport inorganic materials.

[0412] In some embodiments of this application, the hole transport material includes hole transport organics. Without limitation, the hole transport organics may include, but are not limited to, poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA), poly(3,4-ethylenedioxythiophene)-polystyrene sulfonic acid (PEDOT:PSS), 2,2',7,7'-tetratetra[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene, poly-3-hexylthiophene, methoxytriphenylamine-fluoroformamidinium, triphenylamine with a triphenylene core, 3,4-ethylenedioxythiophene-methoxytriphenylamine, N-(4-aniline)carbazole-spirobifluorene, polythiophene, carbazole-based monomers or polymers (such as [4-(3,6-dimethoxy-9H-carbazole-9-yl)butyl]phosphonic acid (MeO-4PACz), [4-(3,6-dimethyl-9H-carbazole]... [4-(9H-carbazole-9-yl)butyl]phosphonic acid (Me-4PACz), [4-(3,6-dibromo-9H-carbazole-9-yl)butyl]phosphonic acid (4PACz), [4-(3,6-dibromo-9H-carbazole-9-yl)butyl]phosphonic acid (Br-4PACz), [2-(3,6-dimethoxy-9H-carbazole-9-yl)ethyl]phosphonic acid (MeO-2PACz), [2-(3,6-dimethyl-9H-carbazole-9-yl)ethyl]phosphonic acid (Me-2PACz), [2-(9H-carbazole-9-yl)ethyl]phosphonic acid (2PACz), [2-(3,6-dibromo-9H-carbazole-9-yl)ethyl]phosphonic acid (Br-2PACz), etc., triphenylamine monomers or polymers, aromatic monomers or polymers, etc. In some embodiments of this application, the hole transport material includes hole transport inorganic materials. Non-limitingly, the hole transport inorganic material may include, but is not limited to, one or more of metal oxides (which may be referred to as the first metal oxide), cuprous iodide and cuprous thiocyanate, molybdenum sulfide, etc.; wherein, the metal oxide in the hole transport material may include, but is not limited to, one or more of nickel oxide, molybdenum oxide, cuprous oxide, vanadium oxide, and tungsten oxide. As a non-limiting example, in the hole transport material, the metal element in the first metal oxide may include one or more of nickel (Ni), molybdenum (Mo), copper (Cu), vanadium (V), and tungsten (W).

[0413] It is understood that the electron transport layer includes electron transport materials. Without limitation, the electron transport materials in the electron transport layer may include, but are not limited to, one or more of the following materials and their derivatives, impurities, and passivated materials: fullerenes and their derivatives, imide compounds, metal oxides, metal sulfides, metal fluorides, cyano-containing polyphenylacetylene, boron-containing polymers, copper bath, red phenanthroline, hydroxyquinoline aluminum, oxadiazole compounds, quinone compounds, etc.; exemplarily, fullerenes and their derivatives include, but are not limited to, [6,6]-phenyl-C 61 methyl butyrate (PC) 61 BM), [6,6]-phenyl-C 71 methyl butyrate (PC) 71 BM), Fullerene C 60 Fullerene C 61 Fullerene C 70 The imide compounds include, but are not limited to, one or more of perylene imide materials, naphthalene imide materials, phthalimide, succinimide, N-bromosuccinimide, glutarimide, or maleimide; metal oxides (which may be referred to as second metal oxides), perylene imide materials, naphthalene imide materials, etc. Among these, the metal oxides in the electron transport materials may include one or more of tin oxide, zinc oxide, etc. As a non-limiting example, in the electron transport materials, the metal element in the second metal oxide may include one or more of tin (Sn), magnesium (Mg), indium (In), molybdenum (Mo), titanium (Ti), and zinc (Zn). Metal sulfides include indium sulfide or zinc sulfide; metal fluorides include one or more of lithium fluoride (LiF), sodium fluoride, magnesium fluoride (MgF2), and calcium fluoride (CaF2).

[0414] Without limitation, the metal oxide in the first charge transport layer may refer to a first metal oxide (in which case the first charge transport layer is a hole transport layer) or a second metal oxide (in which case the first charge transport layer is an electron transport layer).

[0415] In some embodiments of this application, the first charge transport layer is a hole transport layer. In this case, in addition to the first metal oxide, the first charge transport layer may also include one or more other types of hole transport materials, as described above.

[0416] In some embodiments of this application, the first charge transport layer is an electron transport layer. In this case, in addition to the second metal oxide, the first charge transport layer may also include one or more other types of electron transport materials, as described above.

[0417] In this application, the terms "first metal oxide" and "second metal oxide" are used for descriptive purposes only and should not be construed as indicating or implying relative importance or quantity, nor should they be construed as implicitly indicating the importance or quantity of the indicated technical features.

[0418] In this application, unless otherwise specified, "perovskite material" refers to a class of semiconductor materials having a crystal structure similar to that of the natural mineral calcium titanate (CaTiO3). Typically, perovskite materials comprise a first cation, a second cation, and an anion. The anion and the second cation together form an octahedral structure, with the anion located at the body center of the octahedron and the second cation located at the six vertices. The first cation fills the voids between the octahedra to achieve charge balance and maintain crystal structure stability. Adjacent octahedral structures are connected by sharing vertices, thus forming a continuous crystal lattice structure. Unless otherwise specified, the first cation may be denoted as A and referred to as an A-site ion or A-site cation; the second cation may be denoted as B and referred to as a B-site ion or B-site cation; and the anion may be denoted as X and referred to as an X-site ion or X-site anion.

[0419] In some embodiments of this application, the first cation is relatively large and the second cation is relatively small.

[0420] In some embodiments of this application, the perovskite tolerance factor is in the range of 0.85 to 1.0. This is advantageous for obtaining a more stable perovskite crystal structure.

[0421] In this application, "perovskite tolerance factor (t)" has a meaning known in the art, and its calculation formula is as follows: , where R A R is the ionic radius of the A-site ion. B R is the ionic radius of the B-site ion. X Let X be the ionic radius of the ion at the X site.

[0422] The first cation in a perovskite material can be an organic cation, an inorganic cation, or a mixture of organic and inorganic cations; it is understood that the first cation in a perovskite material can be one or more types. In some embodiments of this application, the first cation includes a monovalent cation, and more specifically, it can be a monovalent cation.

[0423] The second cation in the perovskite material can be an organic cation, an inorganic cation, or a mixture of organic and inorganic cations; it is understood that the type of the second cation in the perovskite material can be one or more. In some embodiments of this application, the second cation includes a divalent cation, and more specifically, it can be a divalent cation.

[0424] In some embodiments of this application, the anions in the perovskite material include one or more of halogens and pseudohalogens.

[0425] It is understood that pseudohalogens present in perovskite materials can act as X-site ions. In some embodiments of this application, the X-site anion is a monovalent anion.

[0426] In some embodiments of this application, the perovskite material includes perovskite-type metal halides.

[0427] Unless otherwise stated in this application, the anions in perovskite materials or perovskite-type metal halides may include one or more of halogen anions and pseudohalogen anions.

[0428] In some embodiments of this application, the anion in the perovskite material or perovskite-type metal halide is selected from one or more of halogen anions and pseudohalogen anions.

[0429] In some embodiments of this application, the perovskite material or perovskite-type metal halide may include the material shown in ABX3; wherein A is a monovalent cation, B is a divalent cation, and X is a monovalent anion.

[0430] Without limitation, in perovskite-type metal halides, A can be a monovalent inorganic cation, a monovalent organic cation, or a mixed cation of monovalent organic and monovalent inorganic cations.

[0431] In some embodiments of this application, in the perovskite material or perovskite-type metal halide, A is a monovalent inorganic cation; optionally, A includes Li. + Na + K + 、Rb + and Cs + One or more of them.

[0432] In some embodiments of this application, in the perovskite material or perovskite-type metal halide, A is a monovalent organic cation. Optionally, A includes at least one of methylamino, ethylamino, propylamino, butylamino, pentamino, hexamino, formamidinyl, and imidazolyl.

[0433] Without limitation, the A in perovskite materials or perovskite-type metal halides may include Cs. + K + 、Rb + Li + One or more of monovalent organic cations, etc.

[0434] Non-limiting examples of monovalent organic cations include (NR) 31 R 32 R 33 R34 ) + 、(R 31 R 32 N=CR 33 R 34 ) + 、(R 31 R 32 NC(R 35 )=NR 33 R 34 ) + or (R) 31 R 32 NC(NR 35 R 36 )=R 33 R 34 ) + , where R 31 R 32 R 33 R 34 R 35 and R 36 Each is independently selected from H and C. 1-20 Alkyl, aryl, substituted C 1-20 Alkyl or substituted aryl; wherein, C 1-20 Alkyl and substituted C 1-20 The "C" in alkyl 1-20 Each alkyl group can be independently selected as C. 1-15 Alkyl, further optionally C 1-10 Alkyl, and further optionally C 1-8 Alkyl, and further optionally C 1-6 Alkyl, and further optionally C 1-4 Alkyl, and further optionally C 1-3 Alkyl groups, and further optionally methyl groups. The "aryl" in aryl groups and substituted aryl groups can each independently be C10. 6-20 Aryl, further optionally C 6-12 Aryl, and further alternatively C 6-10 Aryl, further optionally phenyl or naphthyl, and further optionally phenyl. Substituted C 1-20 In alkyl and substituted aryl groups, each substituent is independently C1. 1-10 Hydrocarbon group, further optionally C 1-6 Alkyl or C 6-10 Aryl, and may further be methyl or phenyl.

[0435] Non-limiting examples of monovalent organic cations include CH3NH3 + (Methylamine, MA) + ), NH2CH=NH2 + (Formamidin, can be written as FA) +), dimethylamine cation, ethylamine cation, propylamine cation, butylamine cation, pentamine cation, hexamine cation, imidazole cation.

[0436] In some embodiments of this application, in the perovskite-type metal halide, A includes a monovalent organic cation and Cs. + One or more of them.

[0437] In some embodiments of this application, in the perovskite material or perovskite-type metal halide, B includes divalent cations of one or more of the following elements: lead, tin, zinc, titanium, antimony, bismuth, nickel, iron, cobalt, silver, copper, gallium, germanium, magnesium, calcium, indium, aluminum, manganese, chromium, molybdenum, and europium.

[0438] In some embodiments of this application, X represents a halide anion; optionally, X includes F. - Cl - ,Br - and I - One or more of them, and optionally, X includes Cl - ,Br - and I - One or more of them.

[0439] In some embodiments of this application, the perovskite material includes perovskite-type metal halides, and the monovalent cation of the perovskite material includes FA. + and Cs + .

[0440] In some embodiments of this application, the perovskite material includes perovskite-type metal halides, and the monovalent cation of the perovskite material includes FA. + MA + and Cs + .

[0441] In some embodiments of this application, FA + The molar percentage of monovalent cations in perovskite materials is 0.8~1.0.

[0442] In some embodiments of this application, MA + The molar percentage of monovalent cations in perovskite materials is 0 to 1.0.

[0443] In some embodiments of this application, Cs + The molar percentage of monovalent cations in perovskite materials is 0~1.0.

[0444] In some embodiments of this application, the perovskite material includes perovskite-type metal halides, and the divalent cation of the perovskite material includes Pb. 2+ Furthermore, it can be used for Pb 2+ .

[0445] In some embodiments of this application, the perovskite material includes perovskite-type metal halides, and the monovalent anions of the perovskite material include iodide anions and bromide anions.

[0446] In some embodiments of this application, the molar percentage of iodine anions in the monovalent anions of the perovskite material is 0.1 to 1.0.

[0447] In some embodiments of this application, the molar percentage of bromide anions in the monovalent anions of the perovskite material is 0 to 0.9.

[0448] In this application, unless otherwise specified, the term "aryl" refers to an aromatic hydrocarbon group derived from an aromatic cyclic hydrocarbon compound by losing one hydrogen atom, that is, forming a monovalent linking site directly on the ring. It can be a monocyclic aryl, a fused-ring aryl, or a polycyclic aryl; for polycyclic rings, at least one is an aromatic ring system. For example, "C6- 10 "Aryl" refers to an aryl group containing 6 to 10 carbon atoms. Each time it appears, it can be independently C6 aryl, C8 aryl, C9 aryl, or C6 aryl. 10 Aryl. For example, "C6- 20 "Aryl" refers to an aryl group containing 6 to 20 carbon atoms. Each time it appears, it can be independently, but is not limited to, C6 aryl (such as phenyl), C8 aryl (such as benzocyclobutenyl), C9 aryl (such as indenyl), C6 aryl, C8 aryl, C9 ... 10 Aryl (such as naphthyl), C 12 Aryl (such as acenaphthene, biphenyl), C 13 Aryl (such as fluorene), C 14 Aryl (such as anthracene, phenanthrene), C 18 Aryl (such as phenylene) or C 20 Aryl groups (such as dinaphthalene-based phenyl groups). Examples of suitable aromatic cyclic hydrocarbons that can be derived to form aryl groups include, but are not limited to: benzene, benzocyclobutene, biphenyl, indene, naphthalene, acenaphthene, fluorene, anthracene, phenanthrene, triphenylene, dinaphthalene-based phenyl groups and their derivatives.

[0449] Without limitation, in perovskite-type metal halides, B can be an inorganic cation.

[0450] In some embodiments of this application, in the perovskite-type metal halide, B includes a divalent cation. Optionally, B includes a divalent cation of one or more of the following elements: lead, tin, zinc, titanium, antimony, bismuth, nickel, iron, cobalt, silver, copper, gallium, germanium, magnesium, calcium, indium, aluminum, manganese, chromium, molybdenum, europium, etc.

[0451] Without limitation, B in perovskite-type metal halides may include Pb. 2+ Sn 2+ Fe 2+Mn 2+ Ni 2+ 、Ge 2+ Co 2+ and Sb 2+ One or more of them.

[0452] In perovskite-type metal halides, X can be an inorganic anion, an organic anion, or a mixture of organic and inorganic anions.

[0453] In some embodiments of this application, in the perovskite-type metal halide, X is a halide anion; optionally, X includes F. - Cl - ,Br - and I - One or more of them, and optionally, X includes Cl - ,Br - and I - One or more of the following. In some embodiments, X in the perovskite metal halide can be I. - ,Br - and Cl - One or more of them.

[0454] Without limitation, X in perovskite-type metal halides may include I. - ,Br - One or two of them. X can be I. - ,Br - Or a combination thereof. In some embodiments, X is I. - .

[0455] In some embodiments of this application, the perovskite material accounts for more than or equal to 95% of the mass of the perovskite layer, and can be selected as 95% to 100%.

[0456] Non-limiting, the first electrode and the second electrode may each independently comprise a conductive material. The conductive material in the first electrode and the conductive material in the second electrode may each independently comprise an organic conductive material, an inorganic conductive material, or an organic-inorganic mixed conductive material.

[0457] As an example, organic-inorganic hybrid conductive materials include both organic and inorganic conductive components.

[0458] As a non-limiting example, organic conductive materials may include conductive polymers, wherein non-limiting examples of conductive polymers may include one or more of PEDOT (poly-3,4-ethylenedioxythiophene), polythiophene, polyacetylene, etc.

[0459] As a non-limiting example, inorganic conductive materials may include one or more of transparent conductive oxides, metallic conductive materials, and carbon conductive materials. Non-limiting examples of transparent conductive oxides may include one or more of fluorine-doped tin oxide (FTO), indium tin oxide (ITO), aluminum-doped zinc oxide (AZO), boron-doped zinc oxide (BZO), indium zinc oxide (IZO), tungsten-doped indium oxide (IWO), indium gallium zinc oxide (IGZO), and antimony-doped tin oxide (ATO). Metallic conductive materials may include one or more of gold (Au), silver (Ag), copper (Cu), aluminum (Al), nickel (Ni), chromium (Cr), bismuth (Bi), platinum (Pt), magnesium (Mg), molybdenum (Mo), and tungsten (W).

[0460] In some embodiments of this application, non-limiting examples of inorganic conductive materials include metallic conductive materials. Further, metallic conductive materials may include any one of gold (Au), silver (Ag), copper (Cu), aluminum (Al), nickel (Ni), chromium (Cr), bismuth (Bi), platinum (Pt), magnesium (Mg), or any suitable mixture of the aforementioned elements.

[0461] It is understood that transparent electrodes comprise transparent conductive materials. In some embodiments of this application, the transparent conductive material contained in the transparent electrode may include conductive oxides. Non-limitingly, the conductive oxide in the transparent electrode may include one or more of indium tin oxide, fluorine-doped tin oxide, indium-doped tungsten oxide, indium-doped zinc oxide, and aluminum-doped zinc oxide. In some embodiments of this application, the transparent conductive material in the transparent electrode may be exemplified, but is not limited to, one or more of the following materials: fluorine-doped tin oxide (FTO), indium tin oxide (ITO), aluminum-doped zinc oxide (AZO), boron-doped zinc oxide (BZO), indium zinc oxide (IZO), tungsten-doped indium oxide (IWO), indium gallium zinc oxide (IGZO), and antimony-doped tin oxide (ATO), etc.

[0462] In some embodiments of this application, one of the first electrode and the second electrode is a metal electrode. The metal electrode may include one or more metallic elements selected from gold (Au), silver (Ag), copper (Cu), aluminum (Al), nickel (Ni), chromium (Cr), bismuth (Bi), platinum (Pt), magnesium (Mg), molybdenum (Mo), tungsten (W), etc.

[0463] In some embodiments of this application, the electrode material of the first electrode includes at least one of indium tin oxide (ITO), lanthanide-doped indium oxide, fluorine-doped tin oxide (FTO), antimony-doped tin oxide (ATO), boron-doped zinc oxide (BZO), aluminum-doped zinc oxide (AZO), indium zinc oxide (IZO), gallium zinc oxide (GZO), tungsten-doped indium oxide (IWO), Au, Ag, Cu, Al, Ni, Cr, Bi, Pt, Mg, Mo, W and their alloys, graphite, graphene, and carbon nanotubes; optionally, it includes at least one of Ag, Cu, C, Au, Al, ITO, AZO, BZO or IZO, and further optionally, it includes at least one of Cu, Ag, and Au.

[0464] In some embodiments of this application, the second electrode is a back electrode. The back electrode may include one or more of indium tin oxide (ITO), lanthanide-doped indium oxide, fluorine-doped tin oxide (FTO), antimony-doped tin oxide (ATO), boron-doped zinc oxide (BZO), aluminum-doped zinc oxide (AZO), indium zinc oxide (IZO), gallium zinc oxide (GZO), and tungsten-doped indium oxide (IWO), and the metal may include one or more metallic elements selected from Au, Ag, Cu, Al, Ni, Cr, Bi, Pt, and Mg.

[0465] The substrate layer involved in the embodiments or examples of this application can be, but is not limited to, a rigid substrate layer or a flexible substrate layer. A non-limiting example of a rigid substrate layer is a glass substrate layer. In some embodiments, the rigid substrate layer is transparent glass. In some embodiments, the substrate layer is provided by a transparent conductive oxide film glass (TCO glass), wherein the glass serves as the substrate layer, and the TCO is a transparent conductive oxide film material; non-limiting examples of TCO materials include ITO, FTO, etc.

[0466] In some embodiments of this application, the material of the flexible substrate layer may be, for example, but not limited to, organic polymer materials. Furthermore, it may be composed of one or more of the following materials mixed in different proportions: including but not limited to polyvinyl alcohol (PVA), polyester (PET), polyimide (PI), polyethylene naphthalate (PEN), polydimethylsiloxane (PDMS), etc.

[0467] It is understood that the structure of the photovoltaic device involved in this application is not limited to the structural layers listed above. Other functional layers or interface layers, such as buffer layers and insertion layers, can also be introduced as needed. In some embodiments, a buffer layer with appropriate energy levels can be provided in the photovoltaic device, which can play one or more of the following roles: reducing energy level barriers, promoting energy level matching, improving carrier extraction efficiency, passivating interface defect states, protecting the light-absorbing layer, inhibiting the oxidation and decomposition of water molecules and oxygen on the battery, improving energy conversion efficiency, and improving device stability. Depending on the location of the buffer layer, the type of buffer layer can include four types: a buffer layer between the hole transport layer and the anode, a buffer layer between the electron transport layer and the cathode, a buffer layer between the hole transport layer and the light-absorbing layer, and a buffer layer between the electron transport layer and the light-absorbing layer. Materials that can be used for buffer layers in photovoltaic devices can include, but are not limited to, Cu2O, NiO, AZO, TiO2, etc. In some embodiments, an insertion layer can be provided between the electron transport layer and the second electrode. This insertion layer is used to block the transport of holes and can also be called a hole blocking layer. Examples of materials for the insertion layer include bath copper phosphate (BCP) and tin oxide.

[0468] In some embodiments of this application, the photovoltaic device includes the following stacked structure: a transparent conductive glass substrate layer, a hole transport layer, a perovskite layer, an electron transport layer, a hole blocking layer (optional), and a back electrode (the back electrode can be a metal electrode or a transparent conductive electrode).

[0469] In this application, unless otherwise specified, "sequentially stacked" refers to the direction of stacking between layered structures and does not constitute a limitation on the structural composition of the stacked body. For example, "including stacked structural layer A and structural layer B" means that the stacking direction of structural layer A and structural layer B is along their respective thickness directions; that is, the thickness direction of structural layer A is consistent with or substantially consistent with the thickness direction of structural layer B. It is understood that other intermediate structural layers are allowed to be set between structural layer A and structural layer B.

[0470] In some embodiments of this application, the photovoltaic device 20 includes Figure 14 The structure shown ( Figure 14The structure shown is a schematic cross-sectional view of the device along its thickness direction. The photovoltaic device 10 includes a substrate layer 500, a first electrode 410, a first transport layer 310, a perovskite layer 100, a second transport layer 320, and a second electrode 420, all stacked together. Further, the photovoltaic device 10 has three cross-layered channel regions: a first channel region P1, a second channel region P2, and a third channel region P3. Using the channel group formed by the first channel region P1, the second channel region P2, and the third channel region P3, the solar cell is divided into several series-connected sub-cells. Each sub-cell includes a first channel region P1, a second channel region P2, and a third channel region P3 arranged sequentially, with the second channel region P2 located between the first channel region P1 and the third channel region P3. The first channel region P1, the second channel region P2, and the third channel region P3 can be connected to the spaced-apart structural layers, thereby connecting the circuit between the first electrode of one sub-cell and the second electrode of an adjacent sub-cell, forming a series structure. The first channel region P1, the second channel region P2, and the third channel region P3 can each be an independent linear channel region, formed by laser etching or a photomask. The number of each of the first channel region P1, the second channel region P2, and the third channel region P3 can be one or more. The number of the first channel region P1, the second channel region P2, and the third channel region P3 corresponds to the number of sub-cells. Non-limitingly, the first channel region P1, the second channel region P2, and the third channel region P3 can be configured as follows: the first channel region P1 is used to divide the first electrode 410 to prevent short circuits between adjacent sub-cells; the second channel region P2 is used to penetrate and divide the second charge transport layer 320, the perovskite layer 100, and the first charge transport layer 310, and the second channel region is filled with a conductive material such that both ends of the conductive material are connected to the second electrode 420 and the first electrode 410, respectively. The material of this conductive material can be the same as the material of the second electrode 420 to achieve integral fabrication during the fabrication process of the second electrode 420, or it can be different from the material of the second electrode 420; no limitation is made here; the third channel region P3 is used to penetrate and at least divide the second electrode 420, in Figure 14 In the example, the third channel region P3 is used to penetrate and divide the second electrode 420, the second charge transport layer 320, the perovskite layer 100, and the first charge transport layer 310. One end of the third channel region P3 is connected to the surface of the first electrode 410, and the other end extends out of the outer surface of the second electrode 420. The purpose is to isolate the second electrode between two adjacent sub-cells to prevent short circuits. In this way, a series connection between adjacent sub-cells is achieved.

[0471] In some embodiments of this application, Figure 14 The substrate 500 in the structure shown is a light-incident glass substrate.

[0472] In some embodiments of this application, the filling material in the first channel region P1 of the photovoltaic device can be the same as the first charge transport layer, or it can be filled with insulating material, as long as it can prevent short circuits between adjacent series-connected sub-cells.

[0473] In some embodiments of this application, the filling material in the second channel region P2 of the photovoltaic device may be consistent with the second electrode.

[0474] In some embodiments of this application, the width of the first channel region P1 is 10~50μm, such as 15μm, 25μm, 30μm, etc.

[0475] In some embodiments of this application, the width of the second channel region P2 is 10~200μm, for example 50μm, 60μm, 150μm. Further, the interval between the second channel region P2 and the first channel region P1 can be 20~100μm, for example 20μm, 30μm, 50μm, 100μm, etc.

[0476] In some embodiments of this application, the width of the third channel region P3 is 10~50μm, such as 15μm, 25μm, 50μm, etc. Further, the interval between the third channel region P3 and the second channel region P2 can be 20~100μm, such as 30μm, 50μm, 80μm.

[0477] In some embodiments of this application, the photovoltaic device includes an encapsulating adhesive layer.

[0478] The encapsulating adhesive layer can be used to protect the stability of photovoltaic devices, for example, by isolating them from water, oxygen, and other corrosive substances.

[0479] In some embodiments of this application, the encapsulating adhesive layer includes one or more of the following: epoxy encapsulating adhesive, silicone encapsulating adhesive, polyurethane encapsulating adhesive, UV-curable encapsulating adhesive, ethylene-vinyl acetate copolymer, polyvinyl butyral, ethylene octene copolymer, polyisobutylene, and polyolefin encapsulating adhesive.

[0480] The encapsulating adhesive layer can be stacked using existing techniques in the field. After the photovoltaic device is fabricated, the encapsulating adhesive layer can be stacked at the final structural layer of the solar cell device. In some embodiments of this application, the final structural layer can be a second electrode. For example, lamination technology can be used to laminate the arranged photovoltaic devices or components including photovoltaic devices with the encapsulating adhesive film, thereby creating an encapsulating adhesive layer on the side of the second electrode opposite to the light-absorbing layer.

[0481] Unless otherwise stated, the encapsulating film and encapsulating layer in this application are transparent materials.

[0482] In some embodiments of the second aspect of this application, a method for fabricating a photovoltaic device is provided, which can be used to fabricate the photovoltaic device of the first aspect of this application.

[0483] In some embodiments of this application, a method for fabricating an optoelectronic device is provided, which includes the following steps:

[0484] S100: The perovskite precursor liquid containing perovskite precursor material and first solvent is coated and dried to remove part of the first solvent, thus preparing a perovskite intermediate phase film layer.

[0485] Optionally, drying is performed on a stage at 0°C to 70°C to remove part of the first solvent;

[0486] S200: The additive solution is sprayed onto the surface of the perovskite mesophase film layer, and then annealed with a solvent, wherein the solvent for solvent annealing is chlorobenzene, to form a perovskite layer; wherein the additive solution includes a first additive and a second solvent, and the first additive is an organic material.

[0487] The formed perovskite layer can be found in the description of the first aspect of this application.

[0488] In this application, unless otherwise specified, "perovskite precursor solution" is in solution form and is also referred to as perovskite precursor solution.

[0489] In this application, unless otherwise specified, "precursor material for perovskite materials" refers to a material used to form the perovskite crystal structure, capable of providing the basic elements in the perovskite crystal structure. Typically, the elemental composition of the precursor material for perovskite materials matches the chemical elemental composition of the target perovskite material. For example, the target perovskite material can adopt the general structural formula ABX3, in which case the corresponding raw materials may include AX, BX2, etc., and divalent metal cations (such as Pb). 2+ The sum of the atomic ratios of the components is 1; for example, the target perovskite material can be FA. 0.95 MA 0.05 Pb(I 0.95 Br 0.05 3. At this time, the divalent metal cation is Pb. 2+ .

[0490] In step S100, during the drying process to remove part of the first solvent, the stage temperature is denoted as T1. Unless otherwise specified, T1 is lower than the perovskite crystallization temperature.

[0491] Unless otherwise stated in this application, "perovskite crystallization temperature" refers to the initial crystallization temperature of perovskite, which is the lowest temperature at which the perovskite precursor begins to undergo a phase transition and transform into perovskite crystals.

[0492] In some embodiments of this application, the drying temperature is lower than the perovskite crystallization temperature, and in some embodiments, a perovskite intermediate phase film layer with no significant crystallinity can be obtained.

[0493] Unless otherwise specified, the perovskite mesophase film is a wet film, meaning that some solvent remains.

[0494] In some embodiments of this application, the formed perovskite layer includes a first perovskite material containing Pb and I elements; the thickness direction of the perovskite layer is denoted as the Z direction; the perovskite layer has a first surface and a second surface opposite to each other in the Z direction, the first surface corresponding to the surface coated with the additive solution; a first region with a thickness of 5nm to 10nm exists within a range extending 20nm from the first surface along the Z direction toward the interior of the perovskite layer; the thickness of the perovskite layer is denoted as H0; a second region with a thickness of 5nm to 10nm exists within a range extending (1 / 40)·H0 from 1 / 2·H0 of the perovskite layer toward the first surface and the second surface, respectively; the first region is located between the first surface and the second region; the first region contains lead (Pb) elements. 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+ The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region... - The binding energy of 3d orbital electrons is denoted as J3, and the I of iodine in the second region is... - The binding energy of the 3d orbital electron is denoted as J4; where the perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

[0495] Unless otherwise stated in this application, "the mass percentage of solvent residue in the perovskite mesophase film (F)" S Using the initial solvent content before vacuum drying as a baseline, the following method can be used to confirm the solvent content: TOF-SIMS detection is used to perform in-depth analysis of the dried perovskite mesophase film layer, and the solvent molecule signal intensity (I1) at different depths is monitored. This is then compared with the signal intensity (I0) in the coated perovskite mesophase film layer before VCD treatment to obtain the solvent mass M1 in the dried sample and the solvent mass M0 in the coated sample before VCD treatment. This yields the percentage of residual solvent F in the perovskite mesophase film layer. S =M1 / M0×100%.

[0496] In this application, unless otherwise stated, "perovskite mesophase film without significant crystallinity" means that the perovskite mesophase film has no obvious perovskite crystal phase.

[0497] In some embodiments of this application, the X-ray diffraction pattern of the perovskite mesophase film does not show the characteristic peaks of the perovskite crystalline phase; this characteristic can be used to confirm the "non-significant crystallinity" property of the perovskite mesophase film.

[0498] Unless otherwise stated, X-ray diffraction (XRD) is used in this application to analyze the crystallization of the perovskite phase. The XRD pattern of the perovskite intermediate phase film in this application does not show obvious characteristic peaks of the perovskite phase. After annealing, sharp diffraction peaks of the perovskite phase can be observed in the XRD pattern of the obtained perovskite layer.

[0499] Unless otherwise specified in this application, XRD testing can be performed using the following instruments and methods: an X-ray source of Cu Kα1 (wavelength 1.54056 Å), a scanning range (2θ) of 0–80°, and a scanning rate of 10° / min. Furthermore, a TWIST-TUBE light source and an EIGER2 detector can be selected. Even further, a Bruker D8 DISCOVER instrument can be used. The incident angle can be selected from 2° to 90°. See also the test methods in the Examples section below.

[0500] It is understandable that the temperature for laser annealing is higher than or equal to the crystallization temperature of perovskite.

[0501] A perovskite mesophase film with non-significant crystallinity can be obtained by drying at a low temperature (e.g., 0℃~70℃) below the crystallization temperature of perovskite. Then, a uniform first additive film is introduced by spraying, which helps the first additive to achieve maximum physical contact with defects on the perovskite surface, thereby effectively passivating the defects to the greatest extent. Furthermore, by combining a solvent annealing process, using chlorobenzene as the solvent for annealing helps to extract the first solvent in the perovskite mesophase film, allowing the perovskite mesophase film to quickly reach a highly supersaturated state, inducing rapid and uniform nucleation of perovskite in large quantities. This can promote the first additive to have a large-area uniform coverage characteristic on the crystallized perovskite film while inducing effective crystallization of perovskite, thereby achieving large-area, long-term effective, and specific interface element binding energy regulation. The optoelectronic device described in the first aspect can be prepared. Furthermore, high energy conversion efficiency and long-term operational reliability can be achieved on large-area devices.

[0502] The above-mentioned preparation process has good versatility. It can utilize the binding energy peak position control of Pb, I and optional Br elements by the first additive. It is applicable to perovskite materials with different types and crystallographic properties, and can universally and effectively achieve the control of the binding energy shift vector by defect passivation. In addition, it has good process stability and can significantly improve the batch consistency of high-efficiency devices.

[0503] Furthermore, given the effect of the first additive on the large area (e.g., ≥1m) of the crystallized perovskite film... 2 Its uniform coverage characteristic enables effective and uniform control of the bonding energy of interface elements.

[0504] The preparation method described above can achieve large-area uniform interfacial element binding energy modulation on the surface of perovskite films with different types of perovskite materials and different crystallographic properties.

[0505] The preparation methods described above can use a variety of first additives, all of which can effectively and uniformly control the interfacial element binding energy by virtue of their large-area and uniform coverage of the crystallized perovskite film.

[0506] In some embodiments of this application, the target perovskite material includes divalent metal cations. Further, the concentration of the divalent metal cations in the perovskite precursor solution can be 0.5 mol / L to 3 mol / L, optionally 1 mol / L to 2 mol / L, or any of the following concentrations or a range selected from any two of the following concentrations: 0.5 mol / L, 0.6 mol / L, 0.8 mol / L, 0.9 mol / L, 1 mol / L, 1.2 mol / L, 1.4 mol / L, 1.5 mol / L, 1.6 mol / L, 1.8 mol / L, 2 mol / L, 2.2 mol / L, 2.4 mol / L, 2.5 mol / L, 3 mol / L, etc.

[0507] In some embodiments of this application, the solvent for the perovskite precursor solution may include one or more of dimethylformamide (DMF), dimethyl sulfoxide (DMSO), and N-methylpyrrolidone (NMP).

[0508] In some embodiments of this application, the solvent for the perovskite precursor solution can be a mixture of dimethylformamide (DMF) and dimethyl sulfoxide (DMSO). In some embodiments, the volume ratio of DMF to DMSO is 2 to 6, and exemplary volume ratios can be 2, 2.5, 3, 3.5, 4, 4.5, 5, 5.5, 6, etc., but are not limited thereto.

[0509] In some embodiments of this application, the second solvent includes one or more of chloroform, isopropanol, and ethanol.

[0510] In some embodiments of this application, in step S100, the stage temperature (T1) is 0℃~70℃, optionally 20℃~35℃, further optionally 20℃~30℃, and may also be any of the following temperatures or a range selected from any two of the following temperatures: 0℃, 2℃, 4℃, 5℃, 6℃, 8℃, 10℃, 15℃, 20℃, 25℃, 30℃, 35℃, 40℃, 45℃, 50℃, 55℃, 60℃, 65℃, 70℃, etc.

[0511] In some embodiments of this application, drying to remove a portion of the first solvent can be performed at room temperature. In some embodiments of this application, the drying time for removing a portion of the first solvent is 1 s to 120 s, optionally 60 s to 90 s, or any of the following durations, or a range selected from any two of the following: 1 s, 2 s, 4 s, 5 s, 6 s, 8 s, 10 s, 12 s, 14 s, 15 s, 16 s, 18 s, 20 s, 25 s, 30 s, 35 s, 40 s, 45 s, 50 s, 55 s, 60 s, 80 s, 100 s, 120 s, etc.

[0512] In some embodiments of this application, in step S100, the drying process to remove part of the first solvent is carried out by air knife purging. Drying by air knife purging is more conducive to obtaining a perovskite intermediate phase film layer with no significant crystallinity and uniform in-plane structure, which is beneficial to improving the crystallization quality of perovskite.

[0513] In some embodiments of this application, the mass percentage of residual solvent is controlled to be 12% to 20%, or it can be any of the following percentages or a range selected from any two of the following percentages: 12%, 14%, 15%, 16%, 18%, 20%, etc., based on the initial solvent content before drying. Those skilled in the art can control the amount of residual solvent by controlling the parameters of the air knife purging (the purging gas pressure can be selected as 0.1-0.5 MPa, and the purging gas can be nitrogen or argon, etc.) or the stage temperature and time, etc., which will not be elaborated here.

[0514] In some embodiments of this application, the method for fabricating the optoelectronic device satisfies one or more of the following features:

[0515] (d1) The stage temperature is 20℃~35℃, and the drying time is 1s~120s, which can be selected as 30s~90s;

[0516] Optionally, drying is performed using an air knife purging method;

[0517] (d2) The first additive is the first additive in the optoelectronic device described in the first aspect of this application.

[0518] (d3) The concentration of the first additive in the additive solution is 2 mg / mL to 8 mg / mL, which can be selected as 2 mg / mL to 6 mg / mL, or it can be any of the following concentrations followed by a range of any two of the following concentrations: 2 mg / mL, 2.2 mg / mL, 2.4 mg / mL, 2.5 mg / mL, 2.6 mg / mL, 2.8 mg / mL, 3 mg / mL, 3.2 mg / mL, 3.4 mg / mL, 3.5 mg / mL, 3.6 mg / mL, 3.8 mg / mL, 4 mg / mL, 4.5 mg / mL, 5 mg / mL, 5.5 mg / mL, 6 mg / mL, 6.5 mg / mL, 7 mg / mL, 7.5 mg / mL, 8 mg / mL, etc.;

[0519] (d4) The second solvent includes at least one of chloroform, isopropanol and ethanol;

[0520] (d5) In the step of spraying the additive solution onto the surface of the perovskite mesophase film, a film with a thickness of 1 nm to 10 nm is formed by spraying.

[0521] Optionally, the spraying parameters include: a flow rate of 5 sccm to 30 sccm, a spraying air pressure range of 0.3 MPa to 0.5 MPa, a distance of 15 cm to 20 cm between the spray gun and the surface of the perovskite film, and a spray gun moving speed of 5 cm / s to 60 cm / s;

[0522] (d6) Solvent annealing adopts a gradient annealing method; optionally, solvent annealing includes performing a first stage annealing at a first temperature and then performing a second stage annealing at a second temperature, wherein the first temperature is lower than the second temperature;

[0523] Optionally, the first temperature is 85℃~95℃, and the second temperature is 100℃~120℃;

[0524] Optionally, the annealing time at the first temperature is 1 min to 3 min, and the annealing time at the second temperature is 5 min to 10 min;

[0525] Optionally, the volume percentage of chlorobenzene in the annealing atmosphere is 5% to 20%.

[0526] By controlling the spraying parameters, it is beneficial to enable the first additive to make greater physical contact with the defects on the perovskite surface, thereby achieving more effective passivation of defects.

[0527] During the first-stage annealing process at a relatively low temperature, the perovskite can be induced to nucleate uniformly and achieve pre-crystallization even with a relatively high amount of solvent residue. Then, the second-stage annealing is carried out at a relatively high temperature to induce the formation of high-quality perovskite crystals, which helps to reduce defects and improve the energy conversion efficiency of the device.

[0528] In some embodiments of this application, the annealing time at the first temperature is shorter than the annealing time at the second temperature.

[0529] In some embodiments of this application, the photovoltaic device prepared is as described in the first aspect of this application.

[0530] In some embodiments of this application, the first additive satisfies one or more of the following characteristics (any numerical parameter of the following characteristics may also be selected from any suitable value or range in the context):

[0531] (e1) The number of carbon atoms in the hydrocarbon haloamine is 6 to 20, which can be selected as 6 to 10, or any of the following values ​​or a range selected from any two of the following values: 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, 20, etc.

[0532] (e2) The hydrocarbon group in the hydrocarbon halide amine is at least one of aliphatic hydrocarbon group and aromatic hydrocarbon group, and may be alkyl, alkenyl or aralkyl;

[0533] (e3) The first additive includes one or more of octylamine chloride, alkenylamine bromide, octadecenylamine chloride, phenethylamine chloride, phenethylamine iodide (PEACl), PACl, etc.

[0534] In optoelectronic devices, structural layers other than the perovskite layer can be prepared using one or more of the following methods, including but not limited to: chemical bath deposition, electrochemical deposition, chemical vapor deposition, thermal evaporation, atomic layer deposition, magnetron sputtering, precursor liquid spin coating, precursor liquid slot coating, precursor liquid blade coating, and mechanical pressing. Appropriate methods can be selected to stack the structural layers with adjacent structural layers based on the material properties of each layer. In some embodiments of this application, structural layers in optoelectronic devices can be prepared using one or more of the following methods, including but not limited to: thermal evaporation, precursor liquid coating, etc., wherein the precursor liquid coating method can be precursor liquid spin coating, precursor liquid blade coating, precursor liquid spraying, etc.

[0535] In some embodiments of this application, the method for fabricating a photovoltaic device includes the following steps:

[0536] S10: Perform P1 etching on the first electrode: Perform P1 etching on the first electrode stacked on the substrate layer to form a P1 etching line, exposing the substrate layer to obtain the first substrate, which is then cleaned for later use. The first electrode can be a transparent electrode. The location of the formed P1 etching line can be found in [reference needed]. Figure 14 .

[0537] S20: A first charge transport layer is formed on the first electrode.

[0538] In some implementations, the first charge transport layer may be a hole transport layer.

[0539] S30: A perovskite layer is formed on the first charge transport layer. See the context for photovoltaic device fabrication methods.

[0540] S40: Form a second charge transport layer on the perovskite layer. Perform P2 etching to the depth of the first electrode near the hole transport layer surface. (See reference...) Figure 14 .

[0541] When the first charge transport layer is a hole transport layer, the second charge transport layer is an electron transport layer; when the first charge transport layer is an electron transport layer, the second charge transport layer is a hole transport layer.

[0542] S50: Form a second electrode on the second charge transport layer, perform P3 etching, and etch to the surface of the first electrode near the hole transport layer, then clean the edges. The location of the formed P3 etching line can be found in [reference needed]. Figure 14 .

[0543] In some embodiments of the third aspect of this application, an electrical device is provided, which includes at least one of the optoelectronic devices described in the first aspect of this application and optoelectronic devices prepared by the preparation method of the optoelectronic devices described in the second aspect of this application.

[0544] In some embodiments of the fourth aspect of this application, a power generation device is provided, which includes at least one of the optoelectronic devices described in the first aspect of this application and optoelectronic devices prepared by the preparation method of the optoelectronic devices described in the second aspect of this application.

[0545] Both the power-consuming devices and power-generating devices containing the aforementioned optoelectronic devices can leverage the advantages of optoelectronic devices.

[0546] In some embodiments, the aforementioned optoelectronic devices or optoelectronic components can be power generation devices or power generation apparatuses that function as electrical devices. The type of power generation device or power generation apparatus may include, but is not limited to, integrated power generation. The location of the power generation device or power generation apparatus may include, but is not limited to, the roof or back panel of a vehicle.

[0547] Furthermore, the aforementioned electrical devices may include mobile devices, such as mobile phones and laptops, electric vehicles, electric trains, ships and satellites, power generation systems, etc., but are not limited to these.

[0548] Figure 15 This is an example of an electrical device. The electrical device 6 is a car, and can further be a pure electric vehicle, a hybrid electric vehicle, or a plug-in hybrid electric vehicle, etc.

[0549] Another example of an electrical device could be a mobile phone, tablet, laptop, calculator, etc.

[0550] Another example of an electrical device could be a wearable device, such as a watch.

[0551] Non-limiting examples of light-emitting devices may include light-emitting diodes (LEDs), laser diodes (LDs), etc. Applications of power-generating devices may include, but are not limited to, lighting and display applications.

[0552] In some embodiments, the aforementioned optoelectronic devices or optoelectronic components can be used as light-emitting devices in a display device. Non-limiting examples of display devices include displays, photodetectors, etc.

[0553] The following describes some embodiments of this application. The embodiments described below are exemplary and are only used to explain this application, and should not be construed as limiting this application. Where the technology or conditions are not specified in the embodiments, they are performed according to the description above, or according to the technology or conditions described in the literature in the art, or according to the product instructions. Reagents or instruments whose manufacturers are not specified are all conventional products that can be obtained commercially, or can be synthesized from commercially available products using conventional methods.

[0554] In the following examples, unless otherwise specified, room temperature refers to 20°C to 30°C, and more specifically 25°C.

[0555] In the testing methods section, photovoltaic devices are used as an example of performance testing for optoelectronic devices. It can be understood that optoelectronic devices can be used to perform relevant tests on light-emitting devices.

[0556] For test results where specific test methods are not specified below, please refer to the descriptions above, such as the band gap test method for perovskite layers.

[0557] Hole transport materials: PTAA is poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine]; FAI is formamidinium iodide (CAS No.: 879643-71-7), MABr is methylamine bromide (CAS No.: 6876-37-5), MACl is methylamine chloride (CAS No.: 593-51-1); OACl is octylamine chloride, OABr is octylamine bromide, OAMCl is 9-octadecenylamine chloride (oleylamine chloride), PEACl is phenylethylamine iodide, PACl is propylamine chloride; PCBM is [6,6]-phenyl C61 butyrate methyl ester; BCP is 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline (bath copper); OACl is octylamine chloride (CAS: 1838-08-0), OABr is octylamine bromide (CAS: 1838-08-0), OABr is octylamine bromide (CAS: 1838-08-0), OABr is octylamine bromide (CAS: 1838-08-5), OACl is octylamine chloride (CAS: 1838-08-5 ... bromide (CAS: 1838-08-5), OACl is octyl 14846-47-0), OAmCl is 9-octadecenylamine chloride (oleoamine chloride, CAS: 41130-29-4), PEAI is phenylethylamine iodide (CAS: 151059-43-7), and PEACl is phenylethylamine chloride (CAS: 156-28-5).

[0558] The perovskite layers of the optoelectronic devices prepared in the following embodiments are all in the range of 1.2 eV to 2.2 eV.

[0559] I. Fabrication of optoelectronic devices (which can be used as photovoltaic devices for fabricating solar cells)

[0560] Example 1. The photovoltaic device has an inverted structure.

[0561] Step S1: Take a set of fluorine-doped tin oxide substrates (FTO conductive glass electrodes, first electrode / glass substrate) with dimensions of 1m×2m, and use an infrared laser to etch P1. The width of P1 is about 25μm. Divide the entire glass into 161 sub-cells. The series resistance of different sub-cells is greater than 10MΩ (i.e., 1×10). 7 The etched conductive glass surface was cleaned by ultrasonic cleaning with deionized water, acetone, ethanol, and isopropanol for 15 minutes each, and then placed in a 70°C drying oven for 120 minutes to remove residual organic impurities, resulting in a clean and dry substrate material. This substrate was then treated with UV-ozone for 15 minutes and transferred to a nitrogen-filled glove box. The thickness of the first electrode was 500 nm.

[0562] Step S2, preparation of the hole transport layer: PTAA is used as the hole transport material. PTAA is dissolved in toluene to form a 2 mg / mL solution. This solution is coated onto an FTO substrate and then annealed at 100°C for 10 min to obtain a thin and flat hole transport layer (approximately 20 nm thick). The hole transport layer is used to extract photogenerated holes and block electrons.

[0563] Step S3, Preparation of the perovskite layer:

[0564] Step S3-1: Using a slit coating method, PbI2, FAI, PbBr2, MABr, CsI, and MACl (MACl with a molar percentage of 20 mol% relative to Pb, used as an additive) are dissolved in a mixed solvent of dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) at a volume ratio of 5.5:1, according to CsI... 0.05 (FA 0.92 MA 0.08 ) 0.95 Pb(I 0.92 Br 0.08 The elements in the chemical formula were mixed to prepare a basic solution of perovskite precursor with a molar ratio of 1.4 mol / L. The solution was stirred overnight in a glove box filled with nitrogen to obtain the perovskite precursor solution.

[0565] Step S3-2: The perovskite precursor solution obtained in step S3-1 is filtered using a polytetrafluoroethylene (PTFE) filter. The filtered precursor solution is then coated onto the hole transport layer. At room temperature, an air knife is used to purge the perovskite precursor solution to remove some of the solvent (stage temperature 25°C, duration 60 s), obtaining a perovskite mesophase film layer (or referred to as the perovskite precursor film, with a solvent residue mass percentage of 14%). Octylamine chloride (OACl, the first additive) is dissolved in chloroform at a concentration of 4 mg / mL to obtain an additive solution. This additive solution is then sprayed onto the perovskite mesophase film to form an additive film with a thickness of approximately 5 nm.

[0566] The spraying parameters are as follows: spraying flow rate is 15 sccm, spraying air pressure range is 0.4 MPa, distance between spray gun and perovskite film surface is 15 cm, and spray gun moving speed is 30 cm / s.

[0567] In step S3-3, the perovskite mesophase film layer with additive film is solvent annealed. The perovskite precursor film layer obtained in step S3-2 is transferred to an oven, and chlorobenzene diluted with dry air is set as the annealing atmosphere (chlorobenzene volume ratio is 10%). It is first annealed at 90℃ for 2 min, and then the temperature is raised to 110℃ and annealed at 110℃ for 8 min to form a perovskite film (i.e., perovskite layer) with a thickness of about 440 nm.

[0568] Step S4, preparation of the electron transport layer: PCBM is dissolved in chlorobenzene at 20 mg / mL, coated on the perovskite layer, and then annealed on a heating stage at 70°C for 10 minutes to form an electron transport layer with a thickness of about 60 nm.

[0569] Step S5, preparation of the interface layer: Dissolve BCP in methanol to form a 0.5 mg / mL solution, coat it on the electron transport layer, and then anneal it on a heating stage at 70°C for 10 minutes to form an interface layer (here, a hole blocking layer) with a thickness of about 5 nm.

[0570] P2 is laser-etched, with a width of 60 μm and a depth reaching the FTO layer. The spacing between P2 and P1 is 100 μm.

[0571] Step S6, Fabrication of the back electrode (second electrode): Using a vacuum thermal evaporation deposition apparatus, deposit a 100 nm thick copper electrode on the interface layer obtained in step S5. Laser etch P3, with a width of 50 μm, to a depth down to the FTO layer. The spacing between P3 and P2 is 80 μm (the etching lines are positioned sequentially as P1 / P2 / P3, see reference). Figure 14 Then, infrared edge cleaning is used on the component. An optoelectronic device with an inverted structure is fabricated.

[0572] The prepared optoelectronic devices can be used as photovoltaic devices for device performance testing.

[0573] Examples 2-9 were prepared using essentially the same method as in Example 1 to fabricate optoelectronic devices including a perovskite layer. The differences lay in the type, concentration, spraying parameters, and annealing conditions of the first additive in the additive solution, as shown in Table 1. The remaining operational steps were the same as in Example 1.

[0574] Example 2: The concentration of OACl in step S3-2 was adjusted to 2 mg / mL, and the remaining operation steps were the same as in Example 1;

[0575] Example 3: The concentration of OACl in step S3-2 was adjusted to 8 mg / mL, and the remaining operation steps were the same as in Example 1;

[0576] Example 4: In step S3-2, OACl is replaced with OABr, and the remaining operation steps are the same as in Example 1;

[0577] Example 5: In step S3-2, OACl is replaced with OAmCl, and the remaining operation steps are the same as in Example 1;

[0578] Example 6: In step S3-2, OACl is replaced with PEACl, and the solvent annealing parameters in step S3-3 are adjusted as follows: Chlorobenzene diluted with dry air is set as the annealing atmosphere (chlorobenzene volume percentage is 8%), annealing is first performed at 85°C for 5 min, then the temperature is raised to 120°C and annealed at 120°C for 6 min, and the remaining operation steps are the same as in Example 1.

[0579] Example 7: In step S3-2, OACl is replaced with pyridine, and the solvent annealing parameters in step S3-3 are adjusted as follows: chlorobenzene diluted with dry air is set as the annealing atmosphere (chlorobenzene volume percentage is 20%), and the remaining operation steps are the same as in Example 1.

[0580] Example 8: In step S3-2, OACl was replaced with polymethyl methacrylate, and the spraying parameters were adjusted as follows: spraying flow rate was 10 sccm, spraying air pressure range was 0.5 MPa, the distance between the spray gun and the perovskite film surface was 20 cm, and the spray gun moving speed was 20 cm / s. The remaining operation steps were the same as in Example 1.

[0581] Example 9: In step S3-2, OACl was replaced with polyacrylonitrile, the stage temperature for air knife purging was set to 30°C, and the duration was 40s (the mass percentage of solvent residue in the perovskite mesophase film was 16%). The remaining operation steps were the same as in Example 1.

[0582] Example 10 uses the same method as Example 1 to prepare an optoelectronic device including a perovskite layer. The difference is that the composition of the perovskite precursor material in step S3-1 is different. The other steps are the same as in Example 1. Please refer to Table 1.

[0583] In step S3-1 of Example 8, a slit coating method was used to dissolve PbI2, FAI, CsI, and MACl (MACl molar percentage relative to Pb is 20 mol%) in a mixed solvent of dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) with a volume ratio of 5.5:1, according to FAI... 0.09 Cs 0.05 A basic solution of perovskite precursor was prepared by mixing elements with the chemical formula of PbI3 at a molar ratio of 1.4 mol / L. The solution was stirred overnight in a glove box filled with nitrogen to obtain the perovskite precursor solution.

[0584] Example 11. Photovoltaic devices have a formal structure.

[0585] In the following formal structure,

[0586] Step S1, Fabrication of the transparent electrode (first electrode): A fluorine-doped tin oxide substrate (FTO conductive glass electrode, first electrode / glass substrate) with dimensions of 1m × 2m is selected. P1 is etched using an infrared laser. The width of P1 is approximately 25μm. The entire glass is sequentially divided into 161 sub-cells. The series resistance of different sub-cells is greater than 10MΩ (i.e., 1×10⁻⁶). 7 The etched FTO substrate surface was cleaned by ultrasonic cleaning with deionized water, acetone, ethanol, and isopropanol for 15 minutes each, followed by incubation in a 70°C drying oven for 120 minutes to remove residual organic impurities, resulting in a clean and dry FTO substrate. This substrate was then treated with UV-ozone for 15 minutes and transferred to a nitrogen-filled glove box. The thickness of the first electrode was approximately 550 nm.

[0587] Step S2, preparation of the electron transport layer: A tin oxide nanoparticle aqueous dispersion (the volume ratio of tin oxide nanoparticles to water is 1:9.5, and the average particle size of tin oxide nanoparticles is about 2 nm) is spin-coated onto the FTO conductive layer at a speed of 3000 rpm for 30 s; then, it is transferred to a hot plate and annealed at a temperature of 150 °C for 30 min, followed by ultraviolet ozone treatment at a wavelength of 185 nm, a power of 2250 W, and an irradiation time of 20 min to obtain an electron transport layer with a thickness of about 20 nm.

[0588] Step S3-1: Dissolve PbI2, FAI, PbBr2, MABr, CsI, and MACl (MACl with a molar percentage of 20 mol% relative to Pb, used as an additive) in a mixed solvent of dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) at a volume ratio of 5.5:1 (first solvent), according to CsI... 0.05 (FA 0.92 MA 0.08 ) 0.95 Pb(I 0.92 Br 0.08 The elements in the chemical formula were mixed to prepare a basic solution of perovskite precursor with a molar ratio of 1.4 mol / L. The solution was stirred overnight in a glove box filled with nitrogen to obtain the perovskite precursor solution.

[0589] Step S3-2: Using a slit coating method, the perovskite precursor solution obtained in step S3-1 is filtered through a polytetrafluoroethylene filter. The filtered perovskite precursor solution is then coated onto the hole transport layer. A gas knife is used to remove some of the first solvent (stage temperature 25℃, duration 60s) to obtain the perovskite mesophase film. Octylamine chloride (OACl, the first additive) is dissolved in chloroform at a concentration of 4 mg / mL to obtain an additive solution. This additive solution is then sprayed onto the perovskite mesophase film. The chloroform evaporates quickly, forming a uniform additive film with a thickness of approximately 5 nm.

[0590] The spraying parameters are as follows: spraying flow rate is 15 sccm, spraying air pressure range is 0.4 MPa, distance between spray gun and perovskite film surface is 15 cm, and spray gun moving speed is 30 cm / s.

[0591] In step S3-3, the perovskite mesophase film layer with additive film is solvent annealed. The perovskite precursor film layer obtained in step S3-2 is transferred to an oven, and chlorobenzene diluted with dry air is set as the annealing atmosphere (chlorobenzene volume ratio is 10%). It is first annealed at 90℃ for 2 min, and then the temperature is raised to 110℃ and annealed at 110℃ for 7 min to form a perovskite film (i.e., perovskite layer) with a thickness of about 440 nm.

[0592] Step S4, preparation of the hole transport layer: 1.811 mmol of lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) was dissolved in 1 mL of acetonitrile to obtain the first raw material solution; 72.3 mg of 2,2',7,7'-tetratetra[N,N-di(4-methoxyphenyl)amino]-9,9'-spirodifluorene was dissolved in 1 mL of chlorobenzene, and then mixed with 17.5 μL of the first raw material solution and 28.8 μL of 4-tert-butylpyridine (tBP) to obtain the doped raw material solution; the doped raw material solution was spin-coated onto the perovskite layer at a speed of 3000 rpm for 30 s to obtain the hole transport layer with a thickness of approximately 150 nm.

[0593] Perform laser scribing on P2, with a width of 60 μm, and etch to the upper interface of the FTO layer. The spacing between P2 and P1 is 100 μm.

[0594] Step S6, fabrication of the back electrode (second electrode): A 100 nm thick gold (Au) electrode is deposited on the interface layer obtained in step S5 using a vacuum thermal evaporation coating instrument. The electrode is then removed after vacuum removal, and P3 is laser-etched. P3 has a width of 50 μm and a depth reaching the upper interface of the FTO layer. The spacing between P3 and P2 is 80 μm, and the etching lines are positioned sequentially as P1 / P2 / P3. Infrared edge cleaning is then performed. A photoelectric device with a formal structure is thus fabricated. The fabricated photoelectric device can then be used as a photovoltaic device for performance testing.

[0595] Example 12 uses essentially the same method as Example 1 to prepare an inverted optoelectronic device including a perovskite layer, except that step S3 is different, omitting the preparation and spraying steps of the additive solution. The remaining steps are the same as in Example 1, and can also be found in Table 1.

[0596] Step S3-1 is the same as in Example 1.

[0597] Step S3-2: Filter the solution obtained in step S3-1 using a polytetrafluoroethylene filter. Coat the filtered perovskite precursor solution onto the hole transport layer. Use an air knife to purge and extract the solvent from the perovskite precursor solution to obtain the perovskite intermediate phase film layer. The step of coating the additive solution is omitted.

[0598] Step S3-3: Transfer the perovskite intermediate phase film to a heating stage and anneal at 100°C for 10 minutes to obtain a fully crystallized perovskite layer.

[0599] Example 13. An optoelectronic device comprising a perovskite layer was prepared using a method essentially the same as that in Example 1, except that the method for preparing the perovskite layer was different; the first additive was directly added to the perovskite precursor solution, as shown below. The remaining operating steps were the same as in Example 1, and can also be found in Table 1.

[0600] S3 uses the following method to prepare the perovskite layer:

[0601] S3-1: Dissolve PbI₂, FAI, PbBr₂, MABr, CsI, and MACl (MACl is used as an additive with a molar percentage of 20 mol% relative to Pb) in a mixed solvent of dimethylformamide (DMF) and dimethyl sulfoxide (DMSO) at a volume ratio of 5.5:1 (first solvent), and proceed according to CsI. 0.05 (FA 0.92 MA 0.08 ) 0.95 Pb(I 0.92 Br 0.08 A basic perovskite precursor solution was prepared by mixing the elements in the chemical formula with a molar ratio of 1.4 mol / L. Then, octylamine chloride (OACl) was added to the basic solution at a concentration of 4 mg / mL. The solution was then stirred overnight in a glove box filled with nitrogen to obtain the perovskite precursor solution.

[0602] Step S3-2: Using the slit coating method, the perovskite precursor liquid obtained in step S3-1 is filtered with a polytetrafluoroethylene filter head. The filtered precursor liquid is then coated onto the hole transport layer, and air knife is used to remove part of the first solvent (the stage temperature and duration are the same as in Example 1) to obtain the perovskite intermediate phase film layer.

[0603] Step S3-3: Transfer the perovskite intermediate phase film layer to a heating stage and anneal at 100°C for 10 minutes to form a perovskite thin film.

[0604] Example 14 prepared an optoelectronic device including a perovskite layer using essentially the same method as in Example 1, the difference being that the first additive was different; KCl was dissolved in chloroform at a concentration of 2 mg / mL to obtain an additive solution. The remaining operating steps were the same as in Example 1, and can also be found in Table 1.

[0605] Example 15 uses essentially the same method as Example 11 to prepare a formal optoelectronic device including a perovskite layer, except that step S3 is different, omitting the preparation step of the additive solution and the spraying step of the additive solution. The remaining operation steps are the same as in Example 12, and can also be found in Table 1.

[0606] Step S3-1 is the same as in Example 1.

[0607] Step S3-2: Filter the solution obtained in step S3-1 using a polytetrafluoroethylene filter. Coat the filtered precursor solution onto the hole transport layer. Use an air knife to purge and extract the solvent from the perovskite precursor solution to obtain the perovskite intermediate phase film layer. The step of coating the passivation precursor solution is omitted.

[0608] Step S3-3: Transfer the perovskite intermediate phase film to a heating stage and anneal at 100°C for 10 minutes to obtain a fully crystallized perovskite layer.

[0609] Example 16 uses essentially the same method as Example 1 to fabricate an optoelectronic device including a perovskite layer, the difference being that...

[0610] Step S3-2: Air knife purging is used to remove most of the solvent in the perovskite precursor solution (stage temperature 45°C, duration 60s). The obtained perovskite precursor film has a solvent residue mass percentage of less than 5%. The additive solution is coated onto the perovskite precursor film using a slit coating method to form an additive film with a thickness of about 5nm.

[0611] In step S3-3, the perovskite intermediate phase film layer with additive film is solvent annealed. The perovskite precursor film layer obtained in step S3-2 is transferred to an oven, and chlorobenzene diluted with dry air is set as the annealing atmosphere (chlorobenzene volume ratio is 10%). It is first annealed at 90°C for 10 min to form a perovskite film (i.e., perovskite layer) with a thickness of about 440 nm.

[0612] II. Testing Methods

[0613] (a) Testing of materials, membrane samples, and samples obtained from disassembly, etc.

[0614] 1. X-ray diffraction (XRD) for detecting the crystallization of perovskite mesophase films.

[0615] Test instrument: Bruker D8 Advance.

[0616] XRD test parameters: The X-ray source was Cu Kα1 (wavelength 1.54056 Å), the scanning range (2θ) was 0~80°, the scanning rate was 10° / min, and the incident angle (2θ) ranged from 2° to 90°. The X-ray tube was set to TWIST-TUBE, and the detector was EIGER2.

[0617] The X-ray diffractometer is started to begin measurements. X-rays pass through the sample, interact with the crystal, and produce diffracted light, which is then received and recorded by the detector to obtain the XRD data of the perovskite layer. First, background is subtracted by linear or polynomial fitting, and then the target peaks are marked with their ranges.

[0618] 2. X-ray photoelectron spectroscopy (XPS): Analysis of the binding energies of Pb, I, and Br orbital electrons in the perovskite layer.

[0619] (1) Preparation of perovskite thin film samples (taking Example 1 as an example): In a low humidity (relative humidity less than 2%) or inert gas environment, the perovskite optoelectronic device is cut open with a diamond glass cutter. At this time, the backplate glass, along with the adhesive film and the second electrode, is separated from the perovskite layer. The side with the perovskite layer is picked up with tweezers. Using a pipette or dropper, a small amount of chlorobenzene and o-xylene solvent is allowed to partially and briefly contact the exposed perovskite layer. The surface of the perovskite layer is repeatedly rinsed to remove the electron transport layer material on the surface of the perovskite layer, thus obtaining the bare perovskite thin film;

[0620] (2) The perovskite film is placed in an XPS instrument and the sample surface is irradiated with X-rays to excite orbital electrons of Pb, I, and Br. The binding energy of the corresponding elements can be calculated by measuring the kinetic energy of the photoelectrons using an energy analyzer and combining the instrument work function with the incident electron energy.

[0621] The greater the chemical shift of the binding energy of the orbital electrons in the first region relative to the second region, the greater the bond energy formed with the first additive.

[0622] (II) Measurement and analysis of electric potential distribution

[0623] 1. KPFM test

[0624] KPFM testing instrument: Bruker FastScan Bio.

[0625] KPFM test analysis: By measuring the change in electrostatic force between the probe and the sample, when the probe approaches the surface to be tested, due to the difference in their work functions, electrons will flow from the high Fermi level to the low Fermi level until the Fermi level is flattened. The contact potential difference can be deduced from the work function difference in this process, thereby obtaining potential data. By further combining in-plane scanning, the potential distribution data of the surface to be tested can be obtained.

[0626] 2. Moran Index Analysis

[0627] (1) Parameters to be analyzed at different locations: obtain the values ​​of the parameters to be analyzed at different locations within the region to be analyzed.

[0628] (2) Calculate the Moran index (I) using the selected statistical formula:

[0629]

[0630] Where n is the number of data points; W is the sum of all weights; ij x is an element in the spatial weight matrix; i and x j These are the parameter values ​​for the i-th and j-th positions; This is the average value of all position parameter values.

[0631] (3) Setting the spatial weight matrix:

[0632] The spatial weight matrix uses inverse distance weights, i.e. ,in The distance between the i-th and j-th positions is... Here is the distance attenuation parameter, and p is 2.

[0633] (4) Statistical area and sampling interval of data points: The statistical area is 10 μm × 10 μm, and the sampling interval of data points is 50 nm.

[0634] The Moran index for the potential distribution at the first surface (first region) can be found in Table 2.

[0635] (III) Device Performance Testing

[0636] 1. Initial performance of the device (optoelectronic devices used in solar cells)

[0637] Under normal temperature and pressure (25℃, 1 atmosphere), a standard light source with AM1.5G was used to simulate sunlight, conforming to the national standard IEC61215. The light intensity was corrected using crystalline silicon solar cells to achieve the intensity of one solar cell. The current-voltage characteristic curve (i.e., current-voltage curve) of the solar cell under the illumination of the light source was measured using a four-channel digital source meter (Keithley 2440). The open-circuit voltage (Voc), short-circuit current density (Jsc), fill factor (FF), and photoelectric conversion efficiency (PCE) of the solar cell were obtained.

[0638] The photoelectric conversion efficiency (PCE) is calculated as follows:

[0639] PCE = Pout / Pin

[0640] = Voc×Jsc×[(Vmpp×Jmpp) / (Voc×Jsc)] / Pin

[0641] = Voc×Jsc×FF / Pin

[0642] Wherein, Pout, Pin, Voc, Jsc, Vmpp, Jmpp, and FF represent the battery's operating output power, incident light power, open-circuit voltage, short-circuit current, maximum power point voltage, maximum power point current, and fill factor, respectively. The incident light power is 100 mW / cm². 2 .

[0643] 2. Device stability determination (aging test)

[0644] After the initial performance test of the device is completed, the cell under test is placed in an atmospheric environment (relative humidity of 65%-85%, ambient temperature of about 15℃-40℃) and left in the dark for 1000 hours. The energy conversion efficiency is then tested again (each test continues until there is no hysteresis in the forward and reverse scans, and the photoelectric conversion efficiency is recorded). The ratio of the photoelectric conversion efficiency after 1000 hours of atmospheric placement to the initial efficiency is calculated and used as the normalized efficiency of the solar cell after 1000 hours of placement, which can be denoted as "1000h retention rate".

[0645] 1000h retention rate = retest efficiency / initial efficiency × 100%. The higher the initial normalized efficiency, the better the device stability.

[0646] III. Test Result Analysis

[0647] Based on the XPS test results, the binding energy data of orbital electrons of Pb, I, and Br at the first surface (upper interface, corresponding to the first region) and the bulk phase portion of the perovskite layer (corresponding to the second region) can be obtained, thereby obtaining J1, J2, J3, J4, J5, J6, and J1-J2, J4-J3, J6-J5. See Table 1. For example, the XPS test data of Example 1 can be found in... Figure 16-17 .

[0648] The optoelectronic devices prepared in Examples 1-11, which can be used as photovoltaic devices, all have high photoelectric conversion efficiency and high device stability.

[0649] For example, in the optoelectronic device prepared in Example 1, the J1-J2 and J4-J3 layers of the perovskite layer are controlled within a specific range, satisfying J1-J2 ≥ 0.15 eV and J4-J3 ≥ 0.15 eV; while the optoelectronic devices of Examples 12-15 do not satisfy "J1-J2 ≥ 0.15 eV and J4-J3 ≥ 0.15 eV"; the optoelectronic device of Example 1 has a higher photoelectric conversion efficiency than that of Example 12. Furthermore, the optoelectronic device prepared in Example 1 also exhibits higher device stability. See Tables 1-2 for details.

[0650] In Example 11, the J1-J2 and J4-J3 values ​​of the perovskite layer in the optoelectronic device are controlled within a specific range, satisfying J1-J2 ≥ 0.15 eV and J4-J3 ≥ 0.15 eV; while the optoelectronic devices in Example 15 do not satisfy "J1-J2 ≥ 0.15 eV and J4-J3 ≥ 0.15 eV"; the optoelectronic device in Example 11 has a higher photoelectric conversion efficiency than that in Example 15. Furthermore, the optoelectronic device prepared in Example 11 also exhibits higher device stability. See Tables 1-2 for details.

[0651] In the optoelectronic devices of all embodiments 1-11, the Moran's index of the potential distribution in the first region is relatively small, much lower than that of embodiments 12 and 15. This shows that embodiments 1-11 achieve more uniform in-plane control. See Table 1 for details.

[0652] Taking Example 1 as an example, according to the XRD test results of the perovskite mesophase film, no obvious characteristic diffraction peaks of the perovskite crystal phase were observed, and the perovskite mesophase film showed no significant crystallinity. However, after annealing, stronger diffraction peaks of the perovskite crystal phase could be observed in the XRD spectrum of the formed perovskite layer. For example, perovskite crystal phase diffraction peaks near 13°~15° (2θ) could be observed, indicating the formation of high-quality perovskite crystals.

[0653] Example 12 uses a trans structure, but the additive solution treatment is omitted, i.e., the first additive is not introduced. The binding energies of Pb, I, and Br in the first region do not shift compared to the binding energies of Pb, I, and Br in the perovskite phase. In Example 13, the first additive is directly added to the perovskite precursor solution; in Example 14, the first additive (OACl) in the additive solution is replaced with the inorganic material KCl; and in Example 16, the process parameters are changed. The shift in the binding energies of Pb, I, and Br in the first region of the perovskite layer corresponding to Examples 12-14 compared to the binding energies of Pb, I, and Br in the perovskite phase is relatively low or nonexistent.

[0654] Example 15 uses the formal structure. Compared to Example 11, Example 15 omits the additive solution treatment, that is, the first additive is not introduced, and the binding energies of Pb, I, and Br do not shift.

[0655] After testing, the Moran index of J1-J2, J4-J3 and J6-J5 (if any) corresponding to Examples 1-11 is greater than 0 and less than or equal to 0.25. Furthermore, the Moran index of J1-J2, J4-J3 and J6-J5 (if any) corresponding to Examples 1-2 and Examples 4-11 is less than or equal to 0.15.

[0656] Table 1.

[0657]

[0658] In Table 1, the optoelectronic devices in Examples 11 and 15 are the formal structures, while the remaining Examples 1-10, 12-14, and 16 are the inverse structures.

[0659] In Table 1, the chemical formula of the perovskite materials in Examples 1-9 and 11-16 is Cs. 0.05 (FA 0.92 MA 0.08 ) 0.95 Pb(I 0.92 Br 0.08 )3; The chemical formula of the perovskite material in Example 10 is FA 0.09 Cs 0.05 PbI3.

[0660] Table 2.

[0661]

[0662] It is understood that the above embodiments and examples are merely illustrative. Those skilled in the art may also use other preparation methods to obtain the optoelectronic device of the first aspect of this application. For example, the first additive may not be added, but other process parameters may be adjusted to obtain the optoelectronic device of the first aspect of this application. This application does not limit the preparation method of the optoelectronic device protected by the first aspect.

[0663] The descriptions of the various implementation methods and embodiments above tend to emphasize the differences between them. Similarities or resemblances can be referenced interchangeably, and for the sake of brevity, they will not be repeated here. The technical features of the implementation methods and embodiments described above can be combined arbitrarily. For the sake of brevity, not all possible combinations of the technical features in the above embodiments have been described. However, as long as the combinations of these technical features do not contradict each other, they should be considered within the scope of this specification.

[0664] It should be noted that this application is not limited to the above-described embodiments and examples. The above-described embodiments and examples are merely examples, and any embodiments and examples that have the same structure and achieve the same effect as the technical concept within the scope of this application are included in the technical scope of this application. The embodiments and examples described above only illustrate several embodiments and examples of this application, and although the descriptions are relatively detailed, they should not be construed as limiting the scope of the patent. Furthermore, various modifications that can be conceived by those skilled in the art to the embodiments or examples, and other ways of constructing embodiments or examples by combining some of the constituent elements of the embodiments or examples, are also included in the scope of this application without departing from the spirit of this application.

Claims

1. An optoelectronic device, characterized in that, The perovskite layer includes a first perovskite material containing lead and iodine; the thickness direction of the perovskite layer is denoted as the Z-direction; the perovskite layer has a first surface and a second surface that are opposite to each other in the Z-direction. There exists a first region with a thickness of 5nm to 10nm extending 20nm from the first surface along the Z direction toward the interior of the perovskite layer; The thickness of the perovskite layer is denoted as H0; A second region with a thickness of 5 nm to 10 nm exists within a range extending (1 / 2)·H0 from the perovskite layer toward the first surface and the second surface, respectively; the first region is located between the first surface and the second region. Pb of lead in the first region 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+ The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region - The binding energy of the 3d orbital electrons is denoted as J3, and the I of the iodine element in the second region is... - The binding energy of 3d orbital electrons is denoted as J4; The perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

2. The optoelectronic device according to claim 1, characterized in that, The perovskite layer satisfies one or more of the following characteristics: (t1) 0.15 eV ≤ J1-J2 ≤ 0.3 eV, optionally, 0.16 eV ≤ J1-J2 ≤ 0.28 eV, further optionally, 0.20 eV ≤ J1-J2 ≤ 0.25 eV; (t2) 0.15 eV ≤ J4-J3 ≤ 0.45 eV, optionally, 0.20 eV ≤ J4-J3 ≤ 0.45 eV, further optionally, 0.35 eV ≤ J4-J3 ≤ 0.42 eV.

3. The optoelectronic device according to claim 1 or 2, characterized in that, The perovskite layer satisfies one or more of the following characteristics: (z1) J2 is 138 eV~139 eV; (z2)J4 is 619 eV~620 eV.

4. The optoelectronic device according to any one of claims 1 to 3, characterized in that, The first perovskite material also includes bromine; the Br content of bromine in the first region... - Let J5 be the binding energy of the 3d orbital electrons, and let Br be the Br of bromine in the second region. - The binding energy of 3d orbital electrons is denoted as J6; where J6-J5>0eV.

5. The optoelectronic device according to any one of claims 1 to 4, characterized in that, 0.2 eV≤J6-J5≤0.5 eV, optionally, 0.28 eV≤J6-J5≤0.5 eV, further optionally, 0.35 eV≤J6-J5≤0.46 eV.

6. The optoelectronic device according to any one of claims 1 to 5, characterized in that, The thickness of the perovskite layer is 200nm~1500nm, and can be selected as 400nm~1000nm.

7. The optoelectronic device according to any one of claims 1 to 6, characterized in that, In a direction perpendicular to the thickness of the perovskite layer, the perovskite layer satisfies one or more of the following characteristics: (a1) The Moran index of J1-J2 is less than or equal to 0.25, and optionally less than or equal to 0.15; (a2) The Moran index of J4-J3 is less than or equal to 0.25, and optionally less than or equal to 0.15; (a3) The perovskite layer includes bromine; the Br content of bromine in the first region... - Let J5 be the binding energy of the 3d orbital electrons, and let Br be the Br of bromine in the second region. - The binding energy of the 3d orbital electron is denoted as J6; wherein the Moran index of J6-J5 is less than or equal to 0.25, and optionally less than or equal to 0.

15.

8. The optoelectronic device according to any one of claims 1 to 7, characterized in that, The Moran index of the potential distribution of the first surface is less than or equal to 0.2, and optionally less than or equal to 0.12; wherein the potential of the first surface is obtained by measuring the potential of the first surface using a Kelvin atomic force microscope.

9. The optoelectronic device according to any one of claims 1 to 8, characterized in that, The band gap of the perovskite layer is 1.2 eV to 2.2 eV.

10. The optoelectronic device according to any one of claims 1 to 9, characterized in that, The perovskite layer includes a first additive located in a region of the perovskite layer near the first surface; the first additive is an organic material. Optionally, the first additive comprises at least one of a hydrocarbon halide amine or its corresponding salt, a heteroaryl Lewis base, a polar polymer, polystyrene, and polyethylene glycol, wherein the polar polymer contains a polar group located on its side chain, and the polar group includes a carboxylic acid C. 1-4 One or more of alkyl esters and cyano groups; Further optionally, the first additive includes C 6-20 The alkyl halogenated amine, wherein the halogen in the alkyl halogenated amine or its corresponding salt includes at least one of chlorine, bromine, and iodine; the heteroaryl Lewis base contains at least one of a pyridine ring and a thiophene ring; and the polar polymer includes polymethacrylic acid C. 1-3 Alkyl esters, polyacrylic acid C 1-3 One or more of alkyl esters and polyacrylonitrile.

11. The optoelectronic device according to claim 10, characterized in that, The first additive comprises a hydrocarbon-based haloamine or its corresponding salt, and the perovskite layer satisfies any one of the following characteristics: (i) The halogen in the alkyl halogenated amine or its corresponding salt includes one or more of chlorine and bromine; Optionally, the second surface is used for light incident, and the first surface is used for electron transport; (ii) The halogen in the alkyl halogenated amine or its corresponding salt includes iodine; Optionally, the second surface is used for light incident, and the first surface is used for transmitting holes.

12. The optoelectronic device according to claim 10 or 11, characterized in that, The first region contains the first additive.

13. The optoelectronic device according to any one of claims 1 to 12, characterized in that, The first perovskite material includes halogens; The perovskite layer satisfies one or more of the following characteristics: (b1) The molar percentage of iodine in the halogens of the perovskite layer is 10% to 100%, and can be selected as 80% to 100%; (b2) The molar percentage of bromine in the halogens of the perovskite layer is 0% to 90%, and can be selected as 0% to 20%; (b3) Let the molar ratio of lead to halogen in the perovskite layer be q:3, then q is 0.5~1, and can be selected as 0.9~1.

14. The optoelectronic device according to any one of claims 1 to 13, characterized in that, On a projection plane perpendicular to the Z-direction, the area of ​​the perovskite layer is greater than or equal to 0.09 cm². 2 Optionally, greater than or equal to 1m 2 .

15. The optoelectronic device according to any one of claims 1 to 14, characterized in that, The optoelectronic devices include photovoltaic devices or light-emitting devices.

16. The optoelectronic device according to any one of claims 1 to 15, characterized in that, The optoelectronic devices include photovoltaic devices; The optoelectronic device satisfies one or more of the following characteristics: (c1) The perovskite layer is contained in the inverse or formal structure of the optoelectronic device; (c2) The optoelectronic device includes a first charge transport layer and a second charge transport layer, wherein the perovskite layer is disposed between the first charge transport layer and the second charge transport layer, the first surface faces the first charge transport layer, and the second surface faces the second charge transport layer; wherein, one of the first charge transport layer and the second charge transport layer is a hole transport layer and the other is an electron transport layer; (c3) The optoelectronic device includes a first electrode and a second electrode, the perovskite layer is disposed between the first electrode and the second electrode, the first surface faces the first electrode, and the second surface faces the second electrode.

17. The optoelectronic device according to any one of claims 15-16, characterized in that, The optoelectronic device includes a photovoltaic device, and the second surface is located on the light-incident side of the perovskite layer.

18. The optoelectronic device according to any one of claims 15 to 17, characterized in that, The optoelectronic device includes a photovoltaic device. When the first surface is used to transport electrons, the photovoltaic device includes an electron transport layer stacked with the perovskite layer, and the first surface faces the electron transport layer. or, When the first surface is used for hole transport, the photovoltaic device includes a hole transport layer stacked with the perovskite layer, with the first surface facing the hole transport layer.

19. The optoelectronic device according to any one of claims 15 to 17, characterized in that, The optoelectronic device includes a photovoltaic device; the photovoltaic device includes a solar cell, and the solar cell includes the perovskite layer.

20. The optoelectronic device according to any one of claims 1 to 19, characterized in that, The optoelectronic device includes a solar cell, which is a multi-junction solar cell. The multi-junction solar cell includes a first cell unit, which includes the perovskite layer.

21. The optoelectronic device according to claim 20, characterized in that, The multijunction solar cell further includes a second cell stacked with the first cell; the second cell and the first cell are connected by an interconnect layer, or the second cell and the first cell are isolated by an insulating layer; the second cell includes a second light-absorbing layer, and the band gap of the second light-absorbing layer is different from that of the perovskite layer.

22. The optoelectronic device according to claim 21, characterized in that, The second light-absorbing layer in the second battery cell includes a semiconductor active material, which includes one or more of the following: a second perovskite material, a silicon-containing semiconductor material, copper zinc tin sulfide, copper zinc tin selenide, copper zinc tin selenide sulfide, copper indium gallium selenide, copper indium gallium diselenide, copper indium selenide, cadmium telluride, gallium arsenide, and organic active materials.

23. The optoelectronic device according to claim 21 or 22, characterized in that, The multi-junction solar cell includes a first electrode, a perovskite layer, an interconnect layer, a second light-absorbing layer, and a second electrode stacked together; wherein the interconnect layer is located between the perovskite layer and the second light-absorbing layer; the first electrode is located on the side of the perovskite layer opposite to the interconnect layer, and the second electrode is located on the side of the second light-absorbing layer opposite to the interconnect layer; or, The multi-junction solar cell includes a first electrode, a perovskite layer, a third electrode, an insulating layer, a fourth electrode, a second light-absorbing layer, and a second electrode stacked together; wherein the third electrode, the insulating layer, and the fourth electrode are stacked between the perovskite layer and the second light-absorbing layer, the third electrode is disposed on the side of the insulating layer facing the perovskite layer, the fourth electrode is disposed on the side of the insulating layer facing the second light-absorbing layer, the first electrode is located on the side of the perovskite layer away from the third electrode, and the second electrode is located on the side of the second light-absorbing layer away from the fourth electrode.

24. A method for fabricating an optoelectronic device, characterized in that, Includes the following steps: A perovskite precursor liquid containing perovskite precursor material and a first solvent is coated and dried on a stage at 0℃~70℃ to remove part of the first solvent, thus preparing a perovskite intermediate phase film layer. An additive solution is sprayed onto the surface of the perovskite mesophase film layer, and then annealed with a solvent, wherein the solvent for solvent annealing is chlorobenzene, to form a perovskite layer; wherein the additive solution includes a first additive and a second solvent, and the first additive is an organic material; The formed perovskite layer comprises a first perovskite material containing lead and iodine. The thickness direction of the perovskite layer is denoted as the Z-direction. The perovskite layer has a first surface and a second surface opposite to each other in the Z-direction, the first surface corresponding to the surface coated with the additive solution. A first region with a thickness of 5 nm to 10 nm exists extending 20 nm from the first surface along the Z-direction into the perovskite layer. The thickness of the perovskite layer is denoted as H0. A second region with a thickness of 5 nm to 10 nm exists extending (1 / 2)·H0 from the perovskite layer towards both the first and second surfaces, each extending (1 / 40)·H0. The first region is located between the first surface and the second region. The first region contains lead (Pb). 2+ The binding energy of the 4f orbital electron is denoted as J1, and the Pb of lead in the second region is... 2+ The binding energy of the 4f orbital electrons is denoted as J2; the I of iodine in the first region - The binding energy of the 3d orbital electrons is denoted as J3, and the I of the iodine element in the second region is... - The binding energy of the 3d orbital electron is denoted as J4; wherein the perovskite layer satisfies J1-J2≥0.15 eV and J4-J3≥0.15 eV.

25. The method for fabricating an optoelectronic device according to claim 24, characterized in that, The method for fabricating the optoelectronic device satisfies one or more of the following characteristics: (d1) The stage temperature is 20℃~35℃, and the drying time is 1s~120s, which can be selected as 30s~90s; Optionally, the drying process employs an air knife purging method; (d2) The first additive is the first additive in the optoelectronic device according to claim 10 or 11. (d3) The concentration of the first additive in the additive solution is 2 mg / mL to 8 mg / mL, and can be selected as 2 mg / mL to 6 mg / mL; (d4) The second solvent includes at least one of chloroform, isopropanol and ethanol; (d5) In the step of spraying the additive solution onto the surface of the perovskite mesophase film, a film with a thickness of 1 nm to 10 nm is formed by spraying. Optionally, the spraying parameters include: a flow rate of 5 sccm to 30 sccm, a spraying air pressure range of 0.3 MPa to 0.5 MPa, a distance of 15 cm to 20 cm between the spray gun and the surface of the perovskite film, and a spray gun moving speed of 5 cm / s to 60 cm / s; (d6) The solvent annealing adopts a gradient annealing method; optionally, the solvent annealing includes performing a first stage annealing at a first temperature and then performing a second stage annealing at a second temperature, wherein the first temperature is lower than the second temperature; Optionally, the first temperature is 85℃~95℃, and the second temperature is 100℃~120℃; Optionally, the annealing time at the first temperature is 1 min to 3 min, and the annealing time at the second temperature is 5 min to 10 min; Optionally, the volume percentage of chlorobenzene in the annealing atmosphere is 5% to 20%.

26. An electrical appliance, characterized in that, It includes at least one of the optoelectronic devices according to any one of claims 1 to 23 and optoelectronic devices prepared by the preparation method of any one of claims 15 to 15.

27. A power generation device, characterized in that, It includes at least one of the optoelectronic devices according to any one of claims 1 to 23 and optoelectronic devices prepared by the preparation method of any one of claims 15 to 15.

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