Large-size orthorhombic phase bromine lead cesium single crystal and solution growth method and application thereof
By growing bromine-lead-cesium single crystals in a DMSO-H2O mixed solvent, the problems of complex equipment, pollution, and phase transition in existing technologies have been solved, and high-quality, large-size single crystals have been prepared, which are suitable for photovoltaic cells and light-emitting diodes.
Patent Information
- Authority / Receiving Office
- CN · China
- Patent Type
- Applications(China)
- Current Assignee / Owner
- SHANDONG UNIV
- Filing Date
- 2024-11-22
- Publication Date
- 2026-05-22
AI Technical Summary
Existing solutions for growing single crystals of bromine, lead, and cesium have problems such as high equipment requirements, complex growth processes, numerous byproducts, crystal phase transformation/cracking, and crystal surface contamination. In particular, the use of DMSO as a solvent leads to complex reactions and adhesion contamination.
Bromine-lead-cesium single crystals were grown using a DMSO-H2O mixed solvent. By controlling the solubility-temperature curve and reducing the viscosity of DMSO, positive temperature curve growth was achieved, avoiding the generation of by-products and crystal contamination. Crystal growth was controlled by slow cooling under low temperature conditions.
High-quality, large-size orthorhombic bromine-lead-cesium single crystals were obtained, solving the problems of phase transition and cracking, improving crystal surface quality, reducing production costs and reducing heavy metal waste pollution, and making them suitable for photovoltaic cells, light-emitting diodes and other fields.
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Abstract
Description
Technical Field
[0001] This invention relates to a large-size orthorhombic bromine-lead-cesium single crystal (CsPbBr3) and its solution growth method and application, belonging to the field of crystal material technology. Background Technology
[0002] Cesium bromine lead is one of the representative perovskite crystals. Its single crystals have excellent properties such as high transmittance, high carrier concentration, and high carrier mobility, and have important applications in many fields such as photovoltaic cells, light-emitting diodes, lasers, and X-ray photodetectors.
[0003] In recent years, various methods for growing bulk lead-cesium bromine single crystals have been studied, mainly including melt growth and solution growth methods. Melt growth is generally Bridgman growth, but this method requires sophisticated equipment and involves complex processes. Solution growth methods include anti-solvent diffusion, solvent evaporation, and reverse-temperature crystallization. While these methods are simple and low-cost, they present challenges such as complex phase regions, numerous byproducts, crystal phase transformation / cracking, and crystal surface contamination, which urgently need to be overcome.
[0004] The main reasons for the above-mentioned problems in the solution growth method of bromine-lead-cesium crystals are as follows: DMSO is usually used as the growth solvent for bromine-lead-cesium crystals, but the reaction of bromine-lead-cesium in DMSO is complex and produces many by-products; bromine-lead-cesium crystals exhibit reverse temperature crystallization properties in DMSO, which is not conducive to controlling crystal growth and obtaining high-quality crystals; DMSO solution has high viscosity and easily adheres to the crystal surface, contaminating the crystal and affecting the device properties.
[0005] Therefore, developing a novel growth method for large-size orthorhombic bromine-lead-cesium single crystal solutions to overcome the shortcomings of DMSO as a growth solvent for bromine-lead-cesium crystals will have great application prospects. Summary of the Invention
[0006] To address the shortcomings of existing technologies, this invention provides a large-size orthorhombic bromine-lead-cesium single crystal, its solution growth method, and its applications. Specifically, it describes a method for growing high-quality bromine-lead-cesium single crystals in a DMSO-H₂O mixed solvent and its applications in various fields such as photovoltaic cells, light-emitting diodes, lasers, and photodetectors.
[0007] The technical solution of the present invention is as follows:
[0008] A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals includes the following steps:
[0009] (1) Mix water and dimethyl sulfoxide thoroughly to obtain a mixed solvent; then add cesium bromide and lead bromide to the mixed solvent, heat and dissolve in a sealed state to obtain a clear cesium bromide-lead bromide solution;
[0010] (2) The bromine-lead-cesium solution obtained in step (1) is superheated at 70-80°C for 24-48 hours, filtered, and then cooled to 40-70°C to obtain the bromine-lead-cesium growth solution;
[0011] (3) Add bromine-lead-cesium crystal seeds to the bromine-lead-cesium growth solution obtained in step (2), and slowly cool down under a sealed state to grow large-size orthorhombic bromine-lead-cesium single crystals; or slowly cool down the bromine-lead-cesium growth solution obtained in step (2) under a sealed state to allow it to spontaneously nucleate and grow, and obtain large-size orthorhombic bromine-lead-cesium single crystals.
[0012] According to a preferred embodiment of the present invention, in step (1), the mass ratio of water to dimethyl sulfoxide is (1-4):(6-9), such that the mass percentage of water in the mixed solvent is 10-40%.
[0013] More preferably, the mass ratio of water to dimethyl sulfoxide is 1:4, such that the mass percentage of water in the mixed solvent is 20%.
[0014] According to a preferred embodiment of the present invention, in step (1), the molar ratio of cesium bromide to lead bromide is (1-4):(1-2).
[0015] More preferably, the molar ratio of cesium bromide to lead bromide is 1:1.
[0016] According to a preferred embodiment of the present invention, in step (1), the mass ratio of the total mass of cesium bromide and lead bromide to the mass of the mixed solution is (1-5):(5-19), such that the mass percentage of the solute in the cesium bromide-lead-bromine solution is 5-50%.
[0017] More preferably, the mass ratio of the total mass of cesium bromide and lead bromide to the mass ratio of the mixed solution is 1.5:8.5, such that the mass percentage of solute in the cesium bromide-lead-bromine solution is 15%.
[0018] According to a preferred embodiment of the present invention, in step (1), the heating and dissolving process specifically involves stirring and heating at 70–80°C for 5–10 hours.
[0019] According to a preferred embodiment of the present invention, in step (2), the filtration is performed using an ultrafine water membrane with a diameter of 0.45 micrometers.
[0020] According to a preferred embodiment of the present invention, in step (3), the bromine-lead-cesium seed crystal is a cuboid bromine-lead-cesium orthorhombic single crystal with a side length of less than 3 mm.
[0021] According to a preferred embodiment of the present invention, in step (3), the specific process of growth under the sealed state is as follows: under the sealed conditions of an ambient relative humidity of 10 to 60%, the temperature is reduced from the initial temperature of 70 to 40°C to 30°C at a cooling rate of 0.2 to 2°C / day. The cooling rate can determine the growth rate of the bromine-lead-cesium single crystal.
[0022] More preferably, the specific process of growth under the sealed state is as follows: under sealed conditions with an ambient relative humidity of 30%, the temperature is reduced from an initial temperature of 60°C to 30°C at a cooling rate of 1°C / day.
[0023] A large-size orthorhombic bromine-lead-cesium single crystal was prepared according to the above method.
[0024] According to a preferred embodiment of the present invention, the large-size orthorhombic cesium bromine-lead-bromine single crystal has the molecular formula CsPbBr3, with a length of 17–17.5 mm, a width of 15–15.5 mm, and a height of 13–13.5 mm; the single crystal structure is orthorhombic, with the point group mmm and the space group Pnma. α = β = γ = 90°.
[0025] According to the present invention, the above-mentioned large-size orthorhombic bromine-lead-cesium single crystals are used in photovoltaic cells, light-emitting diodes, field-effect transistors, photocatalysis, LED lighting, photochemical cells, lasers, photodetectors (X-ray, gamma-ray, ultraviolet) and related imaging devices.
[0026] Technical features of the present invention:
[0027] This invention is the first to use a mixture of water and dimethyl sulfoxide as a solvent for cesium bromide and lead bromide, allowing water to participate in the growth of cesium bromide crystals. This alters the reverse-temperature crystallization property of CsPbBr3 crystals, changing its solubility curve from an inverse temperature curve to a positive temperature curve, thus achieving controlled crystal growth at a lower temperature. CsPbBr3 exhibits high solubility in the DMSO-H2O mixed solvent, and its solubility-temperature curve has a steep slope, making it suitable for the growth of large-size cesium bromide crystals. The use of the DMSO-H2O mixed solvent effectively reduces the viscosity of DMSO, preventing the mother liquor from remaining on the crystal surface and improving the surface quality of the crystals. This invention also solves the long-standing problem that the synthesis of cesium bromide crystals cannot be carried out according to a stoichiometric ratio (1:1). 1) The problem of feeding materials was solved, achieving stoichiometric synthesis and growth of crystals; the problem of phase deviation during the reaction process was resolved, avoiding the formation of byproducts such as Cs4PbBr6 and CsPb2Br5; after crystal growth, the mass ratio of cesium bromide and lead bromide in the dimethyl sulfoxide mother liquor remained at 1:1, and the mother liquor could be recycled, effectively reducing resource waste and pollution of the environment by heavy metal compounds; compared with the currently commonly used reverse temperature crystallization method, this patent uses low temperature (<60℃) to grow CsPbBr3 crystals, avoiding phase transformation and cracking phenomena in high temperature crystal growth (>100℃) methods, effectively improving crystal quality.
[0028] The beneficial effects of this invention are:
[0029] 1. The solution growth method for large-size orthorhombic bromine-lead-cesium single crystals provided by this invention allows for stoichiometric feeding, and there is no shift in the CsPbBr3 crystal phase region during crystal growth, effectively avoiding the formation of other byproducts of bromine-lead-cesium. Furthermore, CsPbBr3 has high solubility in DMSO-H2O, and large-size orthorhombic bromine-lead-cesium single crystals can be obtained through cooling growth.
[0030] 2. In the solution growth method for large-size orthorhombic bromine-lead-cesium single crystals provided by this invention, the solubility of bromine-lead-cesium in a mixed solvent of water and dimethyl sulfoxide exhibits a positive temperature curve, meaning that the solubility increases with increasing temperature. Single crystal growth can be achieved by cooling. The growth process is easy to control and has good repeatability.
[0031] 3. The solution growth method for large-size orthorhombic bromine-lead-cesium single crystals provided by this invention can obtain high-quality orthorhombic bromine-lead-cesium single crystals at or below 80℃. The crystal growth temperature is lower than the phase transition temperature of the orthorhombic phase (88℃), and no crystal phase transition occurs during the preparation process. Therefore, it effectively solves the phase transition cracking phenomenon existing in the existing preparation methods. At the same time, under the preferred growth conditions of a cooling rate of 1℃ / day, the maximum edge length of the obtained crystal can reach 2cm, with no solution residue on the single crystal surface and high crystal surface quality, which will greatly improve the performance of photovoltaic cells and photodetectors.
[0032] 4. The large-size orthorhombic bromine-lead-cesium single crystals prepared by this invention are square in shape, which facilitates device fabrication. Furthermore, the synthesis and growth methods are simple and easy to operate, showing great promise for widespread application. Simultaneously, the growth mother liquor can be recycled, reducing production costs, avoiding heavy metal waste pollution, and protecting the environment.
[0033] 5. The large-size orthorhombic bromine-lead-cesium single crystals prepared by this invention have excellent properties such as high carrier concentration and high carrier mobility, and can be applied to the preparation of photovoltaic cells, light-emitting diodes, field-effect transistors, photocatalysis, LED lighting, photochemical cells, lasers, photoelectric detection and imaging devices. Attached Figure Description
[0034] Figure 1 This is a photograph of the orthorhombic bromine-lead-cesium single crystal seed crystal in Example 1.
[0035] Figure 2 This is a growth photograph of lead-bromine cesium crystals seeded into the lead-bromine cesium growth solution in Example 1.
[0036] Figure 3 This is a photograph of the orthorhombic bromine-lead-cesium single crystal prepared in Example 1.
[0037] Figure 4 This is the X-ray diffraction pattern of the orthorhombic bromine-lead-cesium single crystal prepared in Example 1.
[0038] Figure 5 This is a photograph of the growth of single crystals in the bromine-lead-cesium solution in Example 3.
[0039] Figure 6 This is a photograph of the orthorhombic bromine-lead-cesium single crystal prepared by spontaneous nucleation in Example 3.
[0040] Figure 7 This is a photograph of the white crystal in Comparative Example 2.
[0041] Figure 8 This is a photograph of the green crystals prepared by the solvent evaporation method in Comparative Example 3.
[0042] Figure 9 This is a photograph of millimeter-sized bromine-lead-cesium single crystals prepared by the reverse temperature crystallization method in Comparative Example 4. Detailed Implementation
[0043] The present invention will be further illustrated below with reference to specific embodiments. It should be understood that these embodiments are for illustrative purposes only and are not intended to limit the scope of protection of the present invention.
[0044] The cesium bromide (CsBr) used in the examples was a high-purity microcrystalline powder (99.9% purity), the lead bromide (PbBr2) was a high-purity microcrystalline powder (99% purity), the ultrapure water resistivity was 18 MΩ·cm, and the DMSO purity was 99.9%.
[0045] Example 1
[0046] A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals includes the following steps:
[0047] (1) Mix 100 mL of water and 400 mL of dimethyl sulfoxide thoroughly to obtain 500 mL of mixed solvent; then add 34.4 g of cesium bromide and 59.3 g of lead bromide to the mixed solvent, heat and stir at 75 °C for 8 h to obtain a clear cesium bromide-lead bromide solution;
[0048] The mixed solvent contains 20% water by mass, cesium bromide and lead bromide by molar ratio of 1:1, and 15% solute by mass in the cesium bromide-lead-bromine solution.
[0049] (2) The clear bromine-lead-cesium solution obtained in step (1) was superheated at 70°C for 24 hours, filtered through a 0.45-micron ultrafine water membrane, and then cooled to 60°C to obtain the bromine-lead-cesium growth solution, which was kept warm.
[0050] (3) Transfer the bromine-lead-cesium growth solution obtained in step (2) to the growth tank, select a bromine-lead-cesium orthorhombic single crystal with a side length of less than 3 mm and a shape of approximately cuboid as a seed crystal, plant it in the bromine-lead-cesium growth solution, and grow it in a sealed state in the growth tank to obtain a large-size orthorhombic bromine-lead-cesium single crystal.
[0051] The specific process of growth under the sealed condition is as follows: under sealed conditions with an ambient relative humidity of 30%, the temperature is reduced from 60°C to 30°C at a cooling rate of 1°C / day.
[0052] The large-size orthorhombic bromine-lead-cesium single crystal prepared in this embodiment has a length of 17.16 mm, a width of 15.14 mm, and a height of 13.18 mm.
[0053] The photograph of the orthorhombic bromine-lead-cesium single crystal seed crystal in this embodiment is shown below. Figure 1 As shown.
[0054] In this embodiment, the growth photograph shows the seeding of lead bromine and cesium cesium crystals into the lead bromine and cesium cesium growth solution. Figure 2 As shown.
[0055] The photograph of the orthorhombic lead-cesium bromide single crystal prepared in this embodiment is shown below. Figure 3 As shown.
[0056] Depend on Figure 3 It can be seen that the orthorhombic bromine-lead-cesium single crystal prepared in this embodiment has a smooth and flat surface, clear edges and corners, good quality, and high transparency.
[0057] Depend on Figures 1-3 It can be seen that the orthorhombic bromine-lead-cesium single crystal was successfully prepared in this embodiment.
[0058] The X-ray diffraction pattern of the lead-cesium bromine single crystal prepared in this embodiment is as follows: Figure 4 As shown.
[0059] Depend on Figure 4 It can be seen that the orthorhombic bromine-lead-cesium single crystal prepared in this embodiment has good single crystallization properties. Its structure is an orthorhombic phase, free of impurities, and the single crystal structure is an orthorhombic crystal system with the mmm point group and Pnma space group. α = β = γ = 90°.
[0060] Example 2
[0061] A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals includes the following steps:
[0062] (1) Mix 20 mL of water and 80 mL of dimethyl sulfoxide thoroughly to obtain 100 mL of mixed solvent; then add 6.9 g of cesium bromide and 11.9 g of lead bromide to the mixed solvent, stir and heat at 80 °C for 5 h to obtain a clear cesium bromide-lead bromide solution;
[0063] The mixed solvent contains 20% water by mass, the molar ratio of cesium bromide to lead bromide is 1:1, and the solute in the cesium bromide-lead-bromine solution is 15% by mass.
[0064] (2) The clear bromine-lead-cesium solution obtained in step (1) was superheated at 70°C for 24 hours, filtered through a 0.45-micron ultrafine water membrane, and then cooled to 60°C to obtain the bromine-lead-cesium growth solution, which was kept warm.
[0065] (3) The bromine-lead-cesium growth solution obtained in step (2) is transferred to the growth tank, and spontaneous nucleation and growth are carried out in the sealed state of the growth tank to obtain a large-size orthorhombic bromine-lead-cesium single crystal.
[0066] The specific process of growth under the sealed condition is as follows: under sealed conditions with an ambient relative humidity of 30%, the temperature is reduced from 60°C to 30°C at a cooling rate of 1°C / day.
[0067] In this embodiment, several single crystals with an average length of 6 mm, a width of 5 mm, and a height of 3.5 mm were obtained at the bottom of the growth tank.
[0068] The growth photographs of orthorhombic cesium bromine-lead-bromine single crystals in the cesium bromine-lead-bromine solution in this embodiment are shown below. Figure 5 As shown.
[0069] The photograph of the orthorhombic lead-cesium bromide single crystal prepared in this embodiment is shown below. Figure 6 As shown.
[0070] Depend on Figures 5-6 As can be seen, this embodiment successfully obtained orthorhombic bromine-lead-cesium single crystals through spontaneous nucleation growth, and the obtained single crystals have the crystal structure of the single crystals prepared in Example 1.
[0071] Comparative Example 1
[0072] A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals, the specific steps of which are as described in Example 1, except that in step (1): 50 mL of water and 450 mL of dimethyl sulfoxide are thoroughly mixed to obtain 500 mL of mixed solvent, and the mass percentage of water in the mixed solvent is 10%.
[0073] This comparative example was unable to successfully prepare large-size orthorhombic bromine-lead-cesium single crystals (CsPbBr3), as no crystals precipitated during the cooling process from 60°C to 30°C.
[0074] Comparative Example 2
[0075] A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals, the specific steps are as described in Example 1, except that in step (1): 200 mL of water and 300 mL of dimethyl sulfoxide are thoroughly mixed to obtain 500 mL of mixed solvent, and the mass percentage of water in the mixed solvent is 40%.
[0076] This comparative example failed to successfully prepare large-size orthorhombic single-crystal CsPbBr3. During the cooling process from 60℃ to 30℃, white crystals precipitated; however, these white crystals were not orthorhombic single-crystal CsPbBr3. (Specific details are as follows...) Figure 7 As shown.
[0077] Comparative Example 3
[0078] A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals, the specific steps of which are as follows.
[0079] (1) Add 4.5g of cesium bromide and 7.8g of lead bromide to 27mL of dimethyl sulfoxide without adding water, and heat and stir at 60℃ for 5-10h to obtain a cesium bromide-lead solution;
[0080] The mass percentage of solute in the cesium bromide-lead bromide solution was 45.6%; the molar ratio of cesium bromide to lead bromide was 1:1.
[0081] (2) The clear bromine-lead-cesium solution obtained in step (1) is filtered through a 0.45-micron ultrafine water membrane to obtain the bromine-lead-cesium growth solution, and kept at 60℃.
[0082] (3) The bromine-lead-cesium growth solution obtained in step (2) is transferred to a hot plate for heating and volatilization growth, and crystals are prepared by solvent evaporation.
[0083] This comparative example failed to successfully prepare large-size orthorhombic single-crystal CsPbBr3. During the volatilization and growth process under heating on a hot plate, green crystals precipitated. These green crystals were not orthorhombic single-crystal CsPbBr3. Specifically, as shown below... Figure 8 As shown.
[0084] Comparative Example 4
[0085] A solution growth method for orthorhombic bromine-lead-cesium single crystals, the specific steps of which are as follows.
[0086] (1) Add 4.5g of cesium bromide and 15.5g of lead bromide to 27mL of dimethyl sulfoxide without adding water, and heat and stir at 60℃ for 5-10h to obtain a clear cesium bromide-lead-bromine solution;
[0087] The mass percentage of solute in the cesium bromide-lead bromide solution was 74.1%; the molar ratio of cesium bromide to lead bromide was 1:2.
[0088] (2) The clear bromine-lead-cesium solution obtained in step (1) is filtered through a 0.45-micron ultrafine water membrane to obtain the bromine-lead-cesium growth solution, and kept at 60℃.
[0089] (3) The bromine-lead-cesium growth solution obtained in step (2) is transferred to the growth tank. Under the sealed state of the growth tank, the temperature is slowly increased at a rate of 1℃ / day to grow the millimeter-scale orthorhombic bromine-lead-cesium single crystals by the reverse temperature crystallization method.
[0090] The specific process of growth under the sealed condition is as follows: under sealed conditions with an ambient relative humidity of 30%, the temperature is increased from 60℃ to 120℃ at a rate of 1℃ / day, taking advantage of the crystal's reverse temperature crystallization property.
[0091] Although this comparative example successfully prepared millimeter-scale orthorhombic cesium bromine-lead-bromine single crystals, a white substance precipitated on the crystal surface during the removal of the crystals from the solution. This white substance was not an orthorhombic cesium bromine-lead-bromine single crystal (CsPbBr3). Specifically, as shown below... Figure 9 As shown in the figure. This indicates that the surface of the bromine-lead-cesium crystals generated under the solution conditions of Comparative Example 3 has white contamination.
[0092] Finally, it is necessary to further clarify that the above embodiments are merely further illustrations of the present invention and should not be construed as limiting the scope of protection of the present invention. Any non-substantial improvements and adjustments made by those skilled in the art based on the above description of the present invention are within the scope of protection of the present invention.
Claims
1. A solution growth method for large-size orthorhombic bromine-lead-cesium single crystals, characterized in that, The steps include the following: (1) Mix water and dimethyl sulfoxide thoroughly to obtain a mixed solvent; then add cesium bromide and lead bromide to the mixed solvent, heat and dissolve in a sealed state to obtain a clear cesium bromide-lead bromide solution; (2) The bromine-lead-cesium solution obtained in step (1) is superheated at 70-80°C for 24-48 hours, filtered, and then cooled to 40-70°C to obtain the bromine-lead-cesium growth solution; (3) Add bromine-lead-cesium crystal seeds to the bromine-lead-cesium growth solution obtained in step (2), and grow it under a sealed state by cooling down to obtain a large-size orthorhombic bromine-lead-cesium single crystal; or cool down the bromine-lead-cesium growth solution obtained in step (2) under a sealed state to allow it to spontaneously nucleate and grow, thereby obtaining a large-size orthorhombic bromine-lead-cesium single crystal.
2. The solution growth method as described in claim 1, characterized in that, In step (1), the mass ratio of water to dimethyl sulfoxide is (1-4):(6-9), such that the mass percentage of water in the mixed solvent is 10-40%. More preferably, the mass ratio of water to dimethyl sulfoxide is 1:4, such that the mass percentage of water in the mixed solvent is 20%.
3. The solution growth method as described in claim 1, characterized in that, In step (1), the molar ratio of cesium bromide to lead bromide is (1-4):(1-2); More preferably, the molar ratio of cesium bromide to lead bromide is 1:
1.
4. The solution growth method as described in claim 1, characterized in that, In step (1), the total mass of cesium bromide and lead bromide and the mass ratio of the mixed solution are (1-5):(5-19), so that the mass percentage of solute in the cesium bromide-lead-bromine solution is 5-50%. More preferably, the mass ratio of the total mass of cesium bromide and lead bromide to the mass of the mixed solution is 1.5:8.5, such that the mass percentage of solute in the cesium bromide-lead-bromine solution is 15%.
5. The solution growth method as described in claim 1, characterized in that, In step (1), the heating and dissolving process specifically involves stirring and heating at 70-80°C for 5-10 hours.
6. The solution growth method as described in claim 1, characterized in that, In step (2), the filtration is performed using an ultrafine water membrane with a diameter of 0.45 micrometers.
7. The solution growth method as described in claim 1, characterized in that, In step (3), the bromine-lead-cesium seed crystal is a cuboid bromine-lead-cesium orthorhombic single crystal with a side length of less than 3 mm; The specific process of growth under the sealed condition is as follows: under sealed conditions with an ambient relative humidity of 10-60%, the temperature is reduced from the initial temperature of 70-40℃ to 30℃ at a cooling rate of 0.2-2℃ / day. The cooling rate can determine the growth rate of bromine-lead-cesium single crystals.
8. The solution growth method as described in claim 7, characterized in that, The specific process of growth under the sealed condition is as follows: under sealed conditions with an ambient relative humidity of 30%, the temperature is reduced from the initial temperature of 60°C to 30°C at a cooling rate of 1°C / day.
9. A large-size orthorhombic bromine-lead-cesium single crystal, characterized in that, The large-size orthorhombic cesium bromine-lead-bromine single crystal was prepared according to the method described in any one of claims 1 to 8; the molecular formula of the single crystal is CsPbBr3, the single crystal structure is orthorhombic, the point group is mmm, and the space group is Pnma. α = β = γ = 90°.
10. The application of the large-size orthorhombic bromine-lead-cesium single crystal as described in claim 9 in the preparation of photovoltaic cells, light-emitting diodes, field-effect transistors, photocatalysis, LED lighting, photochemical cells, lasers, photodetectors and related imaging devices.