Method for preparing perovskite light-emitting device by using transfer printing hole transport layer

Abstract

The invention belongs to the technical field of perovskite light-emitting devices, and particularly discloses a method for preparing a perovskite light-emitting device by utilizing a transfer printing hole transport layer, which comprises the following steps of: preparing a glass substrate; preparing a photoresist grating template; a polydimethylsiloxane grating template is prepared; preparing medicines required for preparing the perovskite light-emitting diode device; spin-coating a hole transport layer; a micro-nano grating is introduced into the transfer printing hole transport layer; spin-coating a perovskite precursor solution; and 2, 2 ', 2' '-(1, 3, 5-triyl)-tri (1-phenyl-1-H-benzimidazole), lithium fluoride and aluminum are evaporated by adopting a vacuum thermal evaporation system. According to the method for preparing the perovskite light-emitting device by using the transfer printing hole transport layer, the micro-nano structured metal electrode and the organic material interface effectively excite the SPPs mode to be coupled into light energy to be emitted from the device, the energy loss of the SPPs mode is reduced, and the light extraction efficiency of the device is improved.

Description

Technical Field

[0001] The present invention relates to the technical field of perovskite light-emitting devices, and particularly to a method for preparing a perovskite light-emitting device by transferring a hole transport layer. Background Art

[0002] Perovskite light-emitting diode (PeLEDs) devices have the characteristics of being lightweight, thin, flexible, and having high color purity, and are very promising for applications in next-generation flat panel displays and solid-state lighting technologies. In recent years, great progress has been made in the electroluminescence performance of perovskite light-emitting diodes, making people believe that they have great application potential in the fields of display and lighting. Although their external quantum efficiency has been increased to more than 20% in just a few years, it is still lower than that of currently commercially available inorganic LEDs S (EQE>50%) and organic LEDs S (EQE>30%).

[0003] In order to promote the commercial application of PeLEDs, it is crucial to improve their external quantum efficiency, which depends on the internal quantum efficiency and light extraction efficiency of the device. Researchers have proposed many methods to promote radiative recombination in perovskite thin films and suppress non-radiative recombination therein. Methods such as controlling the size of perovskite grains, introducing an interface layer, and adding a passivating agent have significantly improved the internal quantum efficiency of PeLEDs. However, due to the similar structure of PeLEDs devices to OLED devices, they also face problems of internal energy losses such as waveguide mode, substrate mode, and surface plasmon polariton (SPP) mode, resulting in only about 20% of the photons being extracted from the device interior finally, which greatly limits the commercial application prospects of PeLEDs devices.

[0004] Generally speaking, using other materials (such as graphene, conductive polymers, metal films or grids, etc.) to replace ITO as the electrode can effectively improve the influence of the waveguide mode formed by ITO and the organic layer. Preparing microstructures on the back of substrates such as glass can solve the energy loss caused by the substrate mode. Therefore, the energy loss caused by the surface plasmon polariton mode inside PeLEDs devices has become an urgent problem to be solved. Summary of the Invention

[0005] The object of the present invention is to provide a method for preparing a perovskite light-emitting device by using a transferred hole transport layer, reducing the energy loss of the SPPs mode and improving the light extraction efficiency of the device. The process of using the transferred hole transport layer introduces a micro-nano grating structure into the all-inorganic perovskite light-emitting diode. On the one hand, the grating structure of the hole transport layer can play a role in confining the growth of the perovskite spin-coated on the upper layer, and the obtained perovskite film has a better surface morphology and higher crystallinity. On the other hand, the interface between the micro-nano structured metal electrode and the organic material can effectively excite the SPPs mode to couple into light energy and emit from the device, reducing the energy loss caused by the SPPs mode in the light-emitting device and improving the light extraction efficiency of the device.

[0006] To achieve the above object, the present invention provides a method for preparing a perovskite light-emitting device by using a transferred hole transport layer, comprising the following steps:

[0007] S1. Preparation of the glass substrate, cleaning and drying the glass substrate required for preparing the grating template and the indium tin oxide glass substrate required for preparing the perovskite light-emitting diode;

[0008] S2. Preparation of the photoresist grating template, placing the glass substrate in an oxygen plasma cleaner for treatment, spin-coating a layer of photoresist on the glass substrate by using a spin coater, and then performing a two-beam interference experiment by using a laser. After exposure, development, rinsing, and drying, a photoresist template with a grating structure is obtained;

[0009] S3. Preparation of the polydimethylsiloxane grating template, pouring the prepared polydimethylsiloxane on the photoresist grating template, heating it in an oven and curing it through a curing agent, and finally peeling off the polydimethylsiloxane and rinsing it in an acetone solution to obtain a polydimethylsiloxane template with a micro-nano grating structure on the surface;

[0010] S4. Preparation of the drugs required for preparing the perovskite light-emitting diode device, the hole transport layers are poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] and polyvinylcarbazole respectively, and the perovskite precursor solution is cesium lead bromide solution;

[0011] S5. Spin-coating the hole transport layer poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], placing the dried indium tin oxide glass substrate in an oxygen plasma cleaner for treatment, and spin-coating the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] solution by using a spin coater in a vacuum glove box;

[0012] S6. Introduce micro-nano gratings into the hole transport layer of polyvinylcarbazole / 4,4',4'-tris(N-(3-methylphenyl)-N-phenylamino)triphenylamine. Place the polydimethylsiloxane grating template in an organic vacuum coating instrument, evaporate 1 nm of coupling agent and take it out. Spin-coat the polyvinylcarbazole / 4,4',4'-tris(N-(3-methylphenyl)-N-phenylamino)triphenylamine solution in a vacuum glove box. Invert and attach the spin-coated grating template to the surface of the indium tin oxide glass substrate spin-coated with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine]. Take it out of the vacuum glove box and place it in a hot embossing machine for embossing. Peel off the polydimethylsiloxane template in the vacuum glove box to obtain a polyvinylcarbazole / 4,4',4'-tris(N-(3-methylphenyl)-N-phenylamino)triphenylamine hole transport layer with a nano-grating structure;

[0013] S7. Spin-coat the perovskite precursor solution. Spin-coat the perovskite precursor solution on the glass substrate with the dried polyvinylcarbazole / 4,4',4'-tris(N-(3-methylphenyl)-N-phenylamino)triphenylamine hole transport layer with a nano-grating structure in a vacuum glove box using a spin coater, and perform spin coating by the two-step spin coating method;

[0014] S8. Evaporate 2,2′,2″-(1,3,5-triazine)-tris(1-phenyl-1H-benzimidazole), lithium fluoride, and aluminum using a vacuum thermal evaporation system. After spin-coating the perovskite precursor solution, transfer the glass substrate to the vacuum thermal evaporation system, and sequentially evaporate 2,2′,2″-(1,3,5-triazine)-tris(1-phenyl-1H-benzimidazole), lithium fluoride, and aluminum on the perovskite thin film surface.

[0015] Preferably, in step S2, the treatment time of the glass substrate in the oxygen plasma cleaner is 15 min, the rotation speed for spin-coating the photoresist is 3000 r / min, and the time is 30 s.

[0016] Preferably, in step S2, a 325 nm continuous laser is used, and a two-beam interference experiment is carried out to prepare the photoresist grating template under the conditions that the laser power is stable at 40 mw and the exposure time is 400 ms.

[0017] Preferably, in step S3, the mass ratio of polydimethylsiloxane rubber to the curing agent is 10:1.

[0018] Preferably, in step S4, the concentration of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] is 5 mg / ml, the solvent is chlorobenzene. After sealing, it is shaken on a shaker for 5 minutes. After complete dissolution, it is placed in a vacuum glove box for standby; polyvinylcarbazole and 4,4',4'-tris(N-3-methylphenyl-N-phenylamino)triphenylamine are mixed according to a mass ratio of 1:1, the concentration is 10 mg / ml, the solvent is chlorobenzene, and it is stirred at room temperature for 5 hours. After complete dissolution, it is placed in a vacuum glove box for standby; the concentration of the perovskite precursor solution is 0.3 mol / L, the solvent is dimethyl sulfoxide. Polyethylene oxide with a mass ratio of 0.086:1 to cesium lead bromide is added to the perovskite precursor solution to improve the film quality. The perovskite precursor solution is placed in a vacuum glove box and stirred at 60 °C for 24 hours, and then filtered using a 0.45 μm polypropylene filter head and sealed for standby.

[0019] Preferably, in step S5, the rotation speed of spin-coating the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] solution is 4000 r / min, the time is 60 s, and it is annealed on a hot plate at 110 °C for 15 min.

[0020] Preferably, in step S6, the polyvinylcarbazole / 4,4',4'-tris(N-3-methylphenyl-N-phenylamino)triphenylamine solution is spin-coated on the grating-structured polydimethylsiloxane, the rotation speed is 4000 r / min, the time is 60 s, and the imprinting pressure is 3 bar, the temperature is 110 °C, and the time is 20 min in a hot embossing machine.

[0021] Preferably, in step S7, spin-coating is carried out by a two-step spin-coating method. The rotation speed of the first step is 1000 r / min, the time is 5 s, the rotation speed of the second step is 4000 r / min, the time is 30 s, and it is annealed on a hot plate at 50 °C for 30 min.

[0022] Preferably, in step S8, the thickness of the evaporated 2,2′,2″-(1,3,5-triyl)-tris(1-phenyl-1-H-benzoimidazole) is 40 nm, and the film deposition rate is The thickness of lithium fluoride is 1 nm, and the deposition rate is The thickness of aluminum is 100 nm, and the deposition rate is

[0023] The advantages and beneficial effects of the present invention adopting the above method for preparing a perovskite light-emitting device by transferring a hole transport layer are:

[0024] 1. The present invention successfully introduces a periodic grating structure into a perovskite light-emitting device by spin-coating and transferring a hole transport layer on a polydimethylsiloxane (PMDS) with a periodic grating structure. The hole transport layer obtained by spin-coating on a micro-nano structured PDMS substrate can perfectly replicate the periodic grating structure of the template. Therefore, compared with the traditional nanoimprinting method, the present invention can control the depth of the periodic grating structure of the hole transport layer by regulating the depth of the template.

[0025] 2. The method of transferring the hole transport layer in the present invention introduces a micro-nano grating structure into a perovskite light-emitting device. Compared with the nanoimprinting method, the required imprinting pressure is smaller and the process is simpler.

[0026] 3. The present invention spin-coats a perovskite precursor solution on a hole transport layer with a micro-nano grating structure. Compared with a flat device, the micro-nano grating structure can play a role in confining the growth of perovskite nucleation and crystallization. The obtained perovskite thin film not only retains the micro-nano grating structure required for the device, but also has better crystallization quality of perovskite and fewer defects in the whole thin film, which is beneficial to the improvement of device performance.

[0027] 4. By introducing a periodic grating structure into a perovskite light-emitting diode, the energy of the SPPs mode at the interface between the grating metal electrode and the electron transport layer can be effectively coupled into light waves and emitted from the device, thereby reducing the SPPs energy loss of the perovskite light-emitting device and improving the light extraction efficiency.

[0028] The technical solutions of the present invention will be further described in detail below with reference to the accompanying drawings and embodiments. Description of the Drawings

[0029] Figure 1 is a flowchart for preparing a micro-nano grating perovskite light-emitting diode device of the present invention;

[0030] Figure 2 is the structural characterization of relevant functional layers in the device preparation process of the present invention. Among them, (a) is an atomic force microscope image of an S1805 photoresist grating template prepared by a two-beam interference experiment with a 325 nm continuous laser at a power of 40 mw. The period of the grating is 320 nm and the depth is about 50 nm. (b) is an atomic force microscope image of a transferred hole transport layer with a PVK / m-MTDATA micro-nano grating structure, and the depth is about 50 nm. (c) is an atomic force microscope image of a perovskite layer obtained by spin-coating a perovskite precursor solution on the hole transport layer with a grating structure and annealing and crystallizing. (d) is a scanning electron microscope image of a perovskite thin film of a flat comparison device; (e) is a scanning electron microscope image of a micro-nano grating perovskite thin film, and (f) is Glass / ITO / PTAA / PVK:m-MTDATA / CsPbBr 3Cross-sectional scanning electron microscope images;

[0031] Figure 3 These are the comparison diagrams of perovskite thin films between the nanograting device and the flat device, absorption spectra, and electromagnetic field distribution diagrams in the present invention. Among them, (a) is the X-ray diffraction (XRD) spectrum comparison diagram of the perovskite thin film of the nanograting device and the perovskite thin film of the flat device, (b) is the time-resolved PL (TRPL) decay spectrum comparison diagram of the perovskite thin film of the nanograting device and the perovskite thin film of the flat device, (c) is the absorption spectra of the perovskite light-emitting devices with gratings of 300 nm, 320 nm, 350 nm, and 380 nm, and (d) is the electromagnetic field distribution diagram in the PeLEDs device with a 320 nm grating period structure simulated by the finite-difference time-domain method FDTD;

[0032] Figure 4 These are the comparison diagrams between the nanograting perovskite light-emitting device and the flat perovskite light-emitting device in the present invention. Among them, (a) is the comparison diagram of the current density-voltage curve, (b) is the comparison diagram of the luminance-current density curve, (c) is the comparison diagram of the current efficiency-voltage curve, and (d) is the comparison diagram of the EL spectral curve. Detailed implementation manners

[0033] The technical solutions of the present invention will be further described below with reference to the accompanying drawings and embodiments.

[0034] Unless otherwise defined, the technical terms or scientific terms used in the present invention shall have the ordinary meanings understood by those of ordinary skill in the field to which the present invention belongs.

[0035] Unless otherwise defined, the reagents, equipment, etc. used in the present invention are all obtained from conventional commercial sources.

[0036] Example 1

[0037] A method for preparing a perovskite light-emitting device by transferring a hole transport layer, comprising the following steps:

[0038] S1. Preparation of glass substrates. The glass substrates required for preparing the grating templates and the indium tin oxide (ITO) glass substrates required for preparing the perovskite light-emitting diodes are subjected to standardized cleaning treatment. The glass substrates required for preparing the grating templates and the indium tin oxide (ITO) glass substrates required for preparing the perovskite light-emitting diodes (PeLEDs) are ultrasonically cleaned in acetone, anhydrous ethanol, and deionized water for 60 minutes, and then wiped with medical cotton balls containing anhydrous ethanol, and then washed with deionized water. The water droplets on the surface of the glass substrates required for preparing the grating templates and the indium tin oxide glass substrates required for preparing the perovskite light-emitting diodes are blown dry with nitrogen, and then the cleaned glass substrates required for preparing the grating templates and the indium tin oxide glass substrates required for preparing the perovskite light-emitting diodes are placed in a constant temperature oven of 95°C and baked for 20 minutes.

[0039] S2, preparation of photoresist grating template, the clean glass substrate required for preparing the grating template is placed in an oxygen plasma cleaning machine for 15 minutes to make the surface hydrophilic, and then a layer of S1805 photoresist is spin-coated on the glass substrate using a spin coater in a light-proof environment for standby use, the spin coating speed is 3000r / min, and the time is 30s. Subsequently, a 325nm laser is used to perform a laser double-beam interference experiment to prepare a grating template, and the parameters are calculated and the optical path is designed according to the wavelength of the laser and the period of the required grating template; the laser is turned on and preheated for 30 minutes, and the power is observed using a power meter, and the power is waited for to stabilize at 40mw; the glass sheet with the S1805 photoresist spin-coated is attached to the light screen, and the timing opening time of the light gate is adjusted to 400ms for exposure; the exposed photoresist glass sheet is developed in a developer for 2s, and then rinsed and dried with deionized water to obtain a photoresist template with a grating structure.

[0040] S3, preparation of PDMS grating template, use a syringe to take an appropriate amount of PDMS glue and curing agent in a mass ratio of 10:1, add it to the centrifuge tube, use a stirring rod to stir thoroughly to fully blend the curing agent and glue, put it into a centrifuge for centrifugation at a speed of 6000rpm for 6 minutes. Then cast the centrifuged PDMS on the photoresist grating template, let it stand for 30 minutes to wait for the bubbles to disappear, put it in an oven at a constant temperature of 95°C and heat it for 4 hours, and finally peel off the PDMS. Because it is placed in an acetone solution to rinse and remove the residual S1805 photoresist on the surface, a PDMS template with a micro-nano grating structure is obtained.

[0041] S4. Preparation of the chemicals required for perovskite light-emitting diode devices. The hole transport layers are poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] (PTAA) and polyvinylcarbazole (PVK), and the perovskite precursor solution is cesium lead bromide solution. The concentration of PTAA is 5 mg / ml. The preparation method is to put a certain mass of PTAA into a glass vial, add chlorobenzene as the solvent, seal it, and shake it on a shaker for 5 minutes. After complete dissolution, it is placed in a vacuum glove box for standby. The hole mobility of PVK is relatively low. To improve its mobility, the hole injection material m-MTDATA is introduced into the PVK solution. PVK and m-MTDATA are mixed in a mass ratio of 1:1, and the concentration is 10 mg / ml. Weigh PVK and m-MTDATA respectively, then add the solvent chlorobenzene and a stirring rotor, and place it on a stirring table to stir at room temperature for 5 hours. After complete dissolution, it is placed in a vacuum glove box for standby.

[0042] The concentration of the perovskite precursor solution is 0.3 mol / L, and the molar ratio of CsBr and PbBr 2 is 1.2:1. During the experiment, 2 ml of the perovskite precursor solution is prepared. Weigh 0.1532 g of the mass of CsBr and 0.2202 g of the mass of PbBr 2 and then add them to the solvent DMSO. To improve the quality of the film, polyethylene oxide (PEO) is added to the precursor solution, and the mass ratio of PEO to the prepared CsPbBr 3 is 0.086:1. The precursor solution is stirred in a vacuum glove box at 60 °C for 24 hours, and then filtered through a 0.45 μm polypropylene filter head and sealed for standby.

[0043] S5. Spin-coat the hole transport layer poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine]. Place the dried indium tin oxide glass substrate in an oxygen plasma cleaner for 10 min, and spin-coat the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] solution in a vacuum glove box using a spin coater. The spinning speed of the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] solution is 4000 r / min, and the time is 60 s. Then anneal it on a hot plate at 110 °C for 15 min.

[0044] S6. Introduce a micro-nano grating into the hole transport layer of polyvinylcarbazole (PVK) / 4,4',4'-tris(N-(3-methylphenyl)-N-phenylamino)triphenylamine (m-MTDATA). Place the polydimethylsiloxane grating template in an organic vacuum coating instrument, evaporate 1 nm of coupling agent, and then take it out. Spin-coat the PVK / m-MTDATA solution in a vacuum glove box at a spinning speed of 4000 r / min for 60 s. Invert and attach the spin-coated PDMS to the surface of the ITO glass spin-coated with PTAA, take it out of the glove box, and place it in a hot embossing machine for embossing at a pressure of 3 bar, a temperature of 110 °C, and a time of 20 min. After embossing, take it out and remove the PDMS template in the glove box to obtain a PVK / m-MTDATA hole transport layer with a periodic grating structure, successfully introducing the periodic grating structure into the perovskite light-emitting device.

[0045] S7. Spin-coat the perovskite precursor solution. Spin-coat the perovskite precursor solution on the glass substrate with the dried PVK / 4,4',4'-tris(N-(3-methylphenyl)-N-phenylamino)triphenylamine hole transport layer with a nano-grating structure in a vacuum glove box using a spin coater. Use a two-step spin-coating method. The spinning speed in the first step is 1000 r / min for 5 s, and the spinning speed in the second step is 4000 r / min for 30 s. Then place it on a 50 °C hot stage for annealing for 30 min.

[0046] S8. Deposit 2,2′,2″-(1,3,5-triazine)-tris(1-phenyl-1H-benzimidazole) (TPBI), lithium fluoride (LiF), and aluminum (Al) using a vacuum thermal evaporation system. After spin-coating the perovskite precursor solution, in a vacuum pressure of 5×10 -4 Pa, sequentially deposit the electron transport layer TPBi, the cathode modification layer LiF, and the cathode Al in a high-vacuum multi-source thermal evaporation system. The thickness of TPBi is 40 nm, and the film deposition rate is The thickness of LiF is 1 nm, and the deposition rate is The thickness of Al is 100 nm, and the deposition rate is

[0047] By Figure 1It is known that the preparation process of the micro-nano grating perovskite light-emitting diode device is as follows. First, a PDMS template with a micro-nano grating structure is obtained by the casting method. ITO is selected as the anode of the device, and PTAA hole transport layer is spin-coated on the ITO glass substrate. Then, PVK / m-MTDATA is spin-coated on the PDMS template and transferred to the substrate. PVK / m-MTDATA can well replicate the micro-nano grating structure, and a double hole transport layer is formed by the micro-nano grating PVK / m-MTDATA and PTAA. Subsequently, CsPbBr 3 precursor solution is spin-coated on the micro-nano grating PVK / m-MTDATA layer. After annealing and crystallization, a perovskite thin film is obtained as the light-emitting layer, and the micro-nano grating structure is retained to a certain extent. Then, 40 nm of TPBi is evaporated on its surface as the electron transport layer, 1 nm of LiF is used as the cathode modification layer, and 100 nm of Al is used as the cathode. Since the evaporated layer will replicate the structure of the substrate, a micro-nano grating Al electrode can be obtained.

[0048] It can be seen from Figure 2 that through the transfer process, a hole transport layer with a well-shaped grating structure can be prepared, so that the micro-nano grating structure can be introduced into the device. After the perovskite precursor solution is spin-coated and nucleated and crystallized, the overall structure of the grating can be completely retained. Compared with the flat perovskite thin film, the perovskite thin film nucleated and crystallized on the grating structure hole transport layer has a dense surface and very few pinholes. This can be attributed to the fact that the grating structure hole transport layer can play a role in confining the growth of the nucleation and crystallization of CsPbBr 3 , thereby regulating the grain size of the CsPbBr 3 thin film to be more uniform and the surface coverage to be higher. The SEM cross-sectional image proves that the grating structure of the CsPbBr 3 layer is intact, further indicating that the strategy of introducing the grating structure into the device by transferring the hole transport layer is highly feasible.

[0049] It can be seen from Figure 3 that compared with the flat perovskite thin film, the diffraction peak corresponding to the (101) crystal plane of the grating structure perovskite thin film is enhanced and the full width at half maximum becomes narrower, indicating that the crystal quality of the grating perovskite thin film is improved; the obvious increase in the excited state lifetime of the grating CsPbBr 3 further confirms the improvement of the crystal quality and the reduction of defects of the grating perovskite thin film; when the grating period is 320 nm, there is a strong absorption peak near 520 nm, confirming that the grating structure can induce the coupling of the SPPs mode energy and the light wave, and the grating period of 320 nm coincides with the center wavelength (520 nm) of the emission peak of the PeLEDs device in the present invention, which is beneficial to the optimization of the light extraction efficiency of the device.

[0050] It can be seen from Figure 4It can be seen that, compared with flat-panel devices, the brightness and efficiency of the PeLEDs device with a periodic grating structure are increased by 35.67% and 64.38% respectively.

[0051] Therefore, the method for preparing a perovskite light-emitting device by using a transferred hole transport layer according to the present invention has a simple process, is easy to operate, and significantly improves the external quantum efficiency of the device.

[0052] Finally, it should be noted that the above embodiments are only used to illustrate the technical solutions of the present invention and are not intended to limit them. Although the present invention has been described in detail with reference to the preferred embodiments, those of ordinary skill in the art should understand that they can still modify or equivalently replace the technical solutions of the present invention, and these modifications or equivalent replacements cannot make the modified technical solutions deviate from the spirit and scope of the technical solutions of the present invention.

Claims

1. A method for preparing a perovskite light-emitting device by transferring a hole transport layer, characterized in that: The steps include: S1. Preparation of glass substrates: cleaning and drying the glass substrates required for preparing grating templates and the indium tin oxide glass substrates required for preparing perovskite light-emitting diodes; S2, preparation of a photoresist grating template, placing a glass substrate in an oxygen plasma cleaning machine for treatment, using a spin coater to spin coat a layer of photoresist on the glass substrate, then using a laser to perform a double-beam interference experiment, and obtaining a photoresist template with a grating structure after exposure, development, washing, and drying; S3, preparation of a polydimethylsiloxane grating template, pouring the prepared polydimethylsiloxane on the photoresist grating template, placing it in an oven for heating and curing with a curing agent, and finally peeling off the polydimethylsiloxane and rinsing it in an acetone solution to obtain a polydimethylsiloxane template with a micro-nano grating structure on the surface; S4. Preparation of chemicals required for perovskite light-emitting diode devices. The hole transport layers are poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] and polyvinylcarbazole, and the perovskite precursor solution is cesium lead bromide solution. S5, spin coating the hole transport layer poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], placing the dried indium tin oxide glass substrate in an oxygen plasma cleaning machine for treatment, and spin coating the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] solution using a spin coater in a vacuum glove box; S6, transfer hole transport layer polyvinyl carbazole / 4,4',4'-tri(N-3-methylphenyl-N-phenylamino)triphenylamine to introduce micro-nano grating, place polydimethylsiloxane grating template in organic vacuum coating instrument, evaporate 1nm coupling agent, take it out, spin-coat polyvinyl carbazole / 4,4',4'-tri(N-3-methylphenyl-N-phenylamino)triphenylamine solution in vacuum glove box, invert and attach the spin-coated grating template to the surface of indium tin oxide glass substrate spin-coated with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], take it out of vacuum glove box, place it in hot stamping machine for stamping, peel off polydimethylsiloxane template in vacuum glove box, and obtain polyvinyl carbazole / 4,4',4'-tri(N-3-methylphenyl-N-phenylamino)triphenylamine hole transport layer with nano grating structure; S7, spin coating the perovskite precursor solution, spin coating the dried glass substrate with the hole transport layer of polyvinyl carbazole / 4,4',4'-tri(N-3-methylphenyl-N-phenylamino)triphenylamine with the nano-grating structure by using a spin coater in a vacuum glove box, and performing the spin coating by a two-step spin coating method; S8. Use a vacuum thermal evaporation system to evaporate 2,2′,2″-(1,3,5-triyl)-tri(1-phenyl-1-H-benzimidazole), lithium fluoride, and aluminum. After spin coating the perovskite precursor solution, transfer the glass substrate to the vacuum thermal evaporation system, and evaporate 2,2′,2″-(1,3,5-triyl)-tri(1-phenyl-1-H-benzimidazole), lithium fluoride, and aluminum on the surface of the perovskite film in sequence.

2. A method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S2, the glass substrate is treated in the oxygen plasma cleaning machine for 15 minutes, and the rotation speed used for spin coating the photoresist is 3000 r / min for 30 seconds.

3. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S2, a 325 nm continuous laser is used to perform a double-beam interference experiment under the conditions of a stable laser power of 40 mW and an exposure time of 400 ms to prepare a photoresist grating template.

4. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S3, the mass ratio of polydimethylsiloxane glue to curing agent is 10:

1.

5. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S4, the concentration of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] is 5 mg / ml, the solvent is chlorobenzene, and after sealing, it is placed on an oscillator for 5 minutes, and after being completely dissolved, it is placed in a vacuum glove box for standby use; polyvinyl carbazole and 4,4',4'-tri(N-3-methylphenyl-N-phenylamino)triphenylamine are mixed in a mass ratio of 1:1, with a concentration of 10 mg / ml, and the solvent is chlorobenzene. Stir at room temperature for 5 hours, and after being completely dissolved, it is placed in a vacuum glove box for standby use; the concentration of the perovskite precursor solution is 0.3 mol / L, and the solvent is dimethyl sulfoxide. Polyethylene oxide with a mass ratio of 0.086:1 to cesium lead bromine is added to the perovskite precursor solution to improve the quality of the film. The perovskite precursor solution is placed in a vacuum glove box and stirred at 60°C for 24 hours, and then filtered using a 0.45 μm polypropylene filter head, and sealed for standby use.

6. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S5, the poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine] solution is spin-coated at a rotation speed of 4000 r / min for 60 s, and annealed on a hot plate at 110° C. for 15 min.

7. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S6, polyvinyl carbazole / 4,4',4'-tri(N-3-methylphenyl-N-phenylamino)triphenylamine solution is spin-coated on the grating structure polydimethylsiloxane at a rotation speed of 4000 r / min for 60 s, and the hot stamping pressure is 3 bar, the temperature is 110° C., and the time is 20 min.

8. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S7, the spin coating is performed by a two-step spin coating method, the first step has a rotation speed of 1000 r / min and a time of 5 s, the second step has a rotation speed of 4000 r / min and a time of 30 s, and annealing is performed on a hot plate at 50°C for 30 min.

9. The method for preparing a perovskite light-emitting device by transferring a hole transport layer according to claim 1, characterized in that: In step S8, 2,2′,2″-(1,3,5-triyl)-tri(1-phenyl-1-H-benzimidazole) is evaporated to a thickness of 40 nm, and the film deposition rate is The thickness of lithium fluoride is 1nm and the deposition rate is The aluminum thickness is 100nm and the deposition rate is

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