Lead bromide-based perovskite single crystal grown by supplementing bromide ions as well as preparation method and application of lead bromide-based perovskite single crystal

Abstract

The invention discloses a lead bromide-based perovskite single crystal grown by supplementing bromide ions as well as a preparation method and application of the lead bromide-based perovskite single crystal, and relates to the technical field of perovskite crystal growth. The method comprises the following steps: dissolving CsBr, PbBr2 and NH4Br powder in dimethyl sulfoxide, and then adding cyclohexanol and dimethylformamide to obtain a precursor solution; the precursor solution is placed in a sealed container, heat preservation is conducted for 12-36 h at the temperature of 35-40 DEG C, the precursor solution is layered in the heat preservation process, and supernatant liquid is obtained; and placing the supernatant liquid in a sealed container, heating from 35-40 DEG C to 50-60 DEG C at a speed of 0.01-0.08 DEG C / h, and carrying out crystal growth to obtain the lead bromide-based perovskite single crystal grown by supplementing bromide ions. The crystal growth environment can be changed by adding NH4Br into the crystal growth precursor solution, and complicated operation is not needed, so that bromide ions in the crystal growth environment are increased, and the defects of PbBr, VBr and the like caused in a Pb-rich environment are reduced.

Description

Technical Field

[0001] The present invention relates to the technical field of perovskite crystal growth, and in particular to a lead-bromine-based perovskite single crystal grown by supplementing bromide ions, and a preparation method and application thereof. Background Art

[0002] Metal halide perovskite materials ABX3 (X = Cl, Br, I) have attracted widespread attention in recent years due to their unique electronic structure and excellent optoelectronic properties. Among them, cesium lead bromide (CsPbBr3), as an all-inorganic perovskite material, has a suitable band gap (2.25 eV), high light absorption coefficient, and excellent carrier transport properties. Its hole carrier mobility lifetime product can reach ~10 -3 cm 2 / V, resistivity can reach 10 9 It is on the order of Ω·cm and is therefore considered to be a suitable radiation detection material.

[0003] Inversion crystallization is currently the most commonly used method for preparing bulk CsPbBr3 single crystals from solution. In recent years, several research groups at home and abroad have successfully grown CsPbBr3 single crystals using this method. However, point defects during crystal growth affect crystal performance, making the crystals susceptible to ion migration, increasing leakage current in single crystal devices and limiting nuclear radiation detection sensitivity. Therefore, growing high-quality CsPbBr3 single crystals with low defect density remains a challenge.

[0004] The prior art discloses the relationship between the point defect type in CsPbBr3 and the crystal growth environment, which shows that lead-rich environment is prone to cause Pb Br The formation of deep defects such as Br-rich growth environment can reduce the generation of such defects. However, in the process of solution-based growth of CsPbBr3 crystals, since PbBr2 will combine with dimethyl sulfoxide molecules, pure CsPbBr3 phase can only be grown when there is a large excess of Pb.

[0005] The prior art also discloses V Br The defect is Br in CsPbBr3 - The migration provides a channel, and the V can be reduced by introducing Br2 vapor into the preparation of CsPbBr3 film. Br The density of defects improves ion migration in CsPbBr3 thin films, increasing the X-ray detection sensitivity of the films. However, unlike thin films, the growth environment of CsPbBr3 single crystals is more complex, the growth cycle is longer, and the closed growth system cannot achieve the replenishment of Br2 vapor.

[0006] Therefore, in order to reduce the concentration of point defects in the crystal and improve the nuclear radiation detection performance of the crystal, it is very necessary to develop a growth method for supplementing bromide ions during the crystal growth process. Summary of the Invention

[0007] Aiming at the deficiencies existing in the above-mentioned background technology, the present invention mainly solves the problem that when growing CsPbBr3 single crystals by the solution method in the prior art, due to the serious excess of Pb, defects such as Pb Br , V Br etc. are easily generated in the crystal. The present invention provides a method for growing lead bromide-based perovskite single crystals by supplementing bromide ions, and its preparation method and application. This method is simple to operate. Adding NH4Br to the crystal growth precursor solution can change the crystal growth environment, without complex operations, so that the bromide ions in the crystal growth environment increase, and reduce Pb Br , V Br and other defects caused by the Pb-rich environment.

[0008] The first object of the present invention is to provide a preparation method for growing lead bromide-based perovskite single crystals by supplementing bromide ions, including the following steps: Dissolve CsBr, PbBr2 and NH4Br powders in dimethyl sulfoxide, and then add cyclohexanol and dimethylformamide to obtain a precursor solution; Place the precursor solution in a sealed container and keep it warm at 35-40 °C for 12-36 h. During the heat preservation process, the precursor solution will be stratified to obtain the supernatant; Place the supernatant in a sealed container and heat it from 35-40 °C to 50-60 °C at a rate of 0.01-0.08 °C / h for crystal growth, and the lead bromide-based perovskite single crystal grown by supplementing bromide ions is obtained.

[0009] Preferably, the molar ratio of the CsBr, PbBr2 and NH4Br powders is 1:1.5-2:0.15-0.25.

[0010] Preferably, the molar concentration of the CsBr powder in dimethyl sulfoxide is 0.1-1.0 mol / L.

[0011] Preferably, the volume ratio of dimethyl sulfoxide, dimethylformamide and cyclohexanol is 2-2.8:1-1.8:1.

[0012] Preferably, during the process of obtaining the precursor solution, after dissolving the CsBr, PbBr2 and NH4Br powders in dimethyl sulfoxide, use an organic filter tip to filter and remove impurities, collect the filtrate, and then add cyclohexanol and dimethylformamide to the filtrate to prepare the precursor solution.

[0013] Preferably, the pore diameter of the organic filter tip is 0.22 μm.

[0014] Preferably, the heat preservation and the crystal growth are both performed in a crystal growth furnace; Among them, the crystals are taken out after 10 to 20 days of growth.

[0015] Preferably, the growth temperature of different crystals is selected, and the length, width and height of the grown CsPbBr3 crystals vary from millimeters to centimeters.

[0016] The second object of the present invention is to provide a lead-bromine-based perovskite single crystal grown by supplementing bromide ions.

[0017] The third object of the present invention is to provide an application of lead bromine-based perovskite single crystal grown by supplementing bromide ions in radiation detection materials.

[0018] Compared with the prior art, the present invention has the following beneficial effects: The present invention provides a lead bromide-based perovskite single crystal grown by supplementing bromide ions, and its preparation method and application. The present invention uses NH4Br to supplement bromide ions in the CsPbBr3 crystal growth precursor solution, thereby increasing the bromide ions in the crystal growth environment and reducing the Pb-rich environment. Br 、V Br This method can be used to obtain high-quality perovskite single crystals with lower defect concentration, and the crystal defect state density can be maintained at 10 9 cm -3 Order of magnitude; and further experimental verification, the Pb in the CsPbBr3 single crystal grown by the present invention Br 、V Br The defect density is significantly reduced by an order of magnitude; and the bulk resistivity of the crystal is also improved. It has been found that the resistivity of the CsPbBr3 single crystal grown by the bromide ion supplementation method can reach 10 9 Ω·cm level, good practicality.

[0019] The present invention is simple to operate. Adding NH4Br to the crystal growth precursor solution can change the crystal growth environment without the need for complex operations. NH4 ions in the crystal structure can only combine with Br ions through intermolecular forces and cannot form a stable three-dimensional crystal structure. Cs ions combine with Br ions through stronger chemical bonds. Therefore, NH4 ions will not replace Cs ions and enter the crystal structure, thereby causing other defects. BRIEF DESCRIPTION OF THE DRAWINGS

[0020] Figure 1 This is a photo of CsPbBr3 crystals grown by supplementing bromide ions in the present invention.

[0021] Figure 2It is a resistivity comparison diagram of CsPbBr3 crystals grown by the method of supplementing bromide ions and the method of not supplementing bromide ions.

[0022] Figure 3 It is a comparison diagram of the density of defect states of CsPbBr3 crystals grown by the method of supplementing bromide ions and the method of not supplementing bromide ions.

[0023] Figure 4 It is the defect type and defect density of CsPbBr3 crystals obtained by different growth methods measured by deep level transient spectroscopy. (a) is the deep level transient spectroscopy diagram of CsPbBr3 crystals grown without supplementing bromine, (b) is the deep level transient spectroscopy diagram of CsPbBr3 crystals grown with supplementing bromine, and (c) is the comparison diagram of defect density in CsPbBr3 crystals grown by different methods. Specific embodiments

[0024] In order to enable those skilled in the art to better understand and implement the technical solution of the present invention, the present invention will be further described below in conjunction with specific embodiments and drawings, but the specific embodiments cited do not limit the present invention.

[0025] The purpose of the present invention is to provide a method for growing lead bromide-based perovskite single crystals by supplementing bromide ions, and its preparation method and application, so as to solve the problem that when growing CsPbBr3 single crystals by the solution method, due to severe Pb excess, defects such as Pb Br and V Br are easily generated in the crystal.

[0026] In order to achieve the above purpose, the first aspect of the present invention provides a preparation method for growing lead bromide-based perovskite single crystals by supplementing bromide ions, including the following steps: Dissolve CsBr, PbBr2 and NH4Br powders in dimethyl sulfoxide, and then add cyclohexanol and dimethylformamide to obtain a precursor solution; Place the precursor solution in a sealed container and keep it at 35-40 °C for 12-36 h. During the heat preservation process, the precursor solution will be layered to obtain the upper clear liquid; Place the upper clear liquid in a sealed container and heat it from 35-40 °C to 50-60 °C at a rate of 0.01-0.08 °C / h for crystal growth, and thus obtain lead bromide-based perovskite single crystals grown by supplementing bromide ions.

[0027] The present invention dissolves NH4Br in the dimethyl sulfoxide solution of PbBr2 and CsBr, supplements Br ions in the precursor solution, and due to the change of the crystal growth environment, reduces the deep level Pb Br defects and V Br as the ion migration channel in CsPbBr3 crystals.Defects are reduced to improve the crystal properties. This method is applicable to perovskites where PbBr2 is in excess and dimethyl sulfoxide is used as the solvent in a solution-based crystal growth environment.

[0028] Among them, the molar ratio of the CsBr, PbBr2, and NH4Br powders is 1:1.5 - 2:0.15 - 0.25.

[0029] The molar concentration of the CsBr powder in dimethyl sulfoxide is 0.1 - 1.0 mol / L.

[0030] The volume ratio of the dimethyl sulfoxide, dimethylformamide, and cyclohexanol is 2 - 2.8:1 - 1.8:1.

[0031] During the process of obtaining the precursor solution, after dissolving the CsBr, PbBr2, and NH4Br powders in dimethyl sulfoxide, an organic filter tip is used for filtration to remove impurities, and the filtrate is collected. Subsequently, cyclohexanol and dimethylformamide are added to the filtrate to prepare the precursor solution.

[0032] The pore diameter of the organic filter tip is 0.22 μm.

[0033] Both the heat preservation and the crystal growth are carried out in a crystal growth furnace; Among them, the crystal is taken out after 10 - 20 days of growth.

[0034] According to the present invention, by selecting different crystal growth temperatures, the length, width, and height of the grown CsPbBr3 crystal sizes vary from millimeter scale to centimeter scale.

[0035] Exemplarily, a preparation method for supplementing bromide ions to grow lead bromide-based perovskite single crystals includes: 1) Dissolve the PbBr2, CsBr, and NH4Br powders in dimethyl sulfoxide, and use an organic filter tip for filtration to remove impurities. Collect the filtrate, and then add cyclohexanol and dimethylformamide to the filtrate to prepare the precursor solution; In step 1), the molar ratio of the PbBr2 powder, CsBr powder, and NH4Br powder is 1.5 - 2:1:0.15 - 0.25; The molar concentration of the CsBr powder in dimethyl sulfoxide is 0.5 mol / L; The volume ratio of the dimethyl sulfoxide, dimethylformamide, and cyclohexanol is: 2 - 2.8:1 - 1.8:1.

[0036] The diameter of the organic filter tip is 0.22 μm.

[0037] 2) Place the precursor solution prepared in step 1) in conical flask A and seal the mouth of conical flask A with a rubber stopper; 3) Connect the sealed conical flask A in step 2) to a four-jaw clamp, and connect the four-jaw clamp to a crystal growth furnace, and place the conical flask A in water for heat preservation; Place the conical flask A in water at 35 - 40 °C for heat preservation for 24 h.

[0038] It should be noted that 1) The main purpose of selecting a temperature of 35 - 40 °C is that the concentration of the initial precursor solution is relatively high. First, the precursor solution is heat-preserved to nucleate the solution. When the solution concentration reaches below the supersaturation, crystal growth is carried out to avoid a large number of nucleations during the crystal growth process, resulting in the formation of polycrystals.

[0039] 2) Considering the temperature conditions in the laboratory in summer, if the heat preservation temperature is lower than 35 °C, it may be difficult to control because the actual temperature of the growth furnace may be higher than 35 °C due to the high ambient temperature. If the heat preservation temperature is higher than 40 °C, too much mass may precipitate in the solution, resulting in a slow crystal growth rate and small crystal size.

[0040] 4) Take out the conical flask A after heat preservation in step 3), pour the supernatant in the conical flask A into the conical flask B, seal the mouth of the conical flask B with a rubber stopper, and place the sealed conical flask B in the crystal growth furnace, and carry out crystal growth by heating; Slowly heat the crystal growth furnace from 35 - 40 °C to 50 - 60 °C at a rate of 0.05 °C / h for crystal growth.

[0041] Among them, slowly heating from 35 - 40 °C to 50 - 60 °C at a rate of 0.05 °C / h, the crystal growth takes about 15 - 20 days, and then it is taken out to obtain CsPbBr3 single crystals.

[0042] It should be noted that since the solubility and supersaturation of CsPbBr3 in the solution decrease with increasing temperature, a relatively fast heating rate may cause the solution concentration to remain higher than the supersaturation and generate nucleation, which is not conducive to obtaining high-quality single crystals. In addition, a high heating rate will lead to a faster crystal growth rate, which is likely to increase the crystal defects. Therefore, a slow heating rate of 0.05 °C / h is selected for heating.

[0043] For the CsPbBr3 single crystals, depending on the different growth temperature ranges, the length, width, and height of the grown CsPbBr3 crystal sizes vary from millimeter scale to centimeter scale.

[0044] The second aspect of the present invention provides a method for growing lead bromide-based perovskite single crystals by supplementing bromide ions.

[0045] The second aspect of the present invention provides an application of a method for growing lead bromide-based perovskite single crystals by supplementing bromide ions in radiation detection materials.

[0046] It should be noted that, unless otherwise specified, the experimental methods used in the present invention are all conventional methods; the reagents and materials used, unless otherwise specified, can all be purchased on the market.

[0047] Example 1 A preparation method of growing lead bromide-based perovskite single crystals by supplementing bromide ions, comprising: Dissolving NH4Br powder in the CsPbBr3 crystal growth precursor solution and growing in a crystal growth furnace for 15 days. The specific steps are as follows. 1) Dissolve 12.4 g of PbBr2, 6 g of CsBr and 0.33 g of NH4Br powder in 45 mL of dimethyl sulfoxide, and filter to remove impurities using a 0.22 μm organic filter tip, collect the filtrate, and then add 22.5 mL of cyclohexanol and 22.5 mL of dimethylformamide to the filtrate to prepare the precursor solution; 2) Place the precursor solution prepared in step 1) in conical flask A and seal the mouth of conical flask A with a rubber stopper; 3) Connect the sealed conical flask A in step 2) to a four-jaw clamp, and connect the four-jaw clamp to the crystal growth furnace, and place conical flask A in water at 35 °C for heat preservation for 24 h; 4) Take out conical flask A after heat preservation in step 3), pour the upper clear liquid in conical flask A into conical flask B, seal the mouth of conical flask B with a rubber stopper, and place the sealed conical flask B in the crystal growth furnace, and slowly heat from 35 °C to 50 °C at a heating rate of 0.05 °C / h for crystal growth.

[0048] The grown CsPbBr3 single crystal is as Figure 1 shown, and the crystal size is about 10×10×2 mm in length×width×height 3 , and the crystal has good permeability. In order to verify what differences exist between the CsPbBr3 single crystals grown by supplementing bromide ions and those grown without supplementing bromide ions, the present invention also compared the defect state density, resistivity, and specific defect types and densities in the crystals grown by the two methods, as Figure 2 , 3 and shown in 4. The results show that the crystal grown by supplementing bromide ions has a lower defect density and a higher resistivity, indicating that the crystal quality has been significantly improved.

[0049] Figure 2 are the resistivities of the CsPbBr3 crystals grown with and without adding NH4Br (wo-NH4Br). It can be seen that the resistivity of the crystal grown by adding NH4Br is significantly increased, indicating that the impurity concentration in the crystal is small and the defect energy levels within the crystal band gap are few.

[0050] SeeFigure 3 As shown, the density of defect states of CsPbBr3 crystals grown by the space charge confinement method with and without the addition of NH4Br (wo-NH4Br) was measured. The density of defect states of the crystals grown with the addition of NH4Br decreased significantly, indicating that the addition of Br ions can effectively reduce the crystal defect concentration.

[0051] See Figure 4 As shown, for the defect types and concentrations in the crystal, the test results of deep level transient spectroscopy show that after adding NH4Br to supplement Br ions, the density of V Br - and Pb Br 2+ in the crystal both decreased by an order of magnitude, indicating that Br ions effectively filled the vacancy defects and reduced the generation of deep level anti-site defects.

[0052] Example 2 A preparation method for growing lead bromide-based perovskite single crystals by supplementing bromide ions, comprising: Dissolving NH4Br powder in the CsPbBr3 crystal growth precursor solution and growing in a crystal growth furnace for 17 days. The specific steps are as follows. 1) Dissolve 14.45 g of PbBr2, 6 g of CsBr, and 0.44 g of NH4Br powder in 45 mL of dimethyl sulfoxide, and filter to remove impurities using a 0.22 μm organic filter tip. Collect the filtrate, and then add 18.8 mL of cyclohexanol and 26.3 mL of dimethylformamide to the filtrate to prepare the precursor solution; 2) Place the precursor solution prepared in step 1) in conical flask A and seal the mouth of conical flask A with a rubber stopper; 3) Connect the sealed conical flask A in step 2) to a four-jaw clamp, and connect the four-jaw clamp to the crystal growth furnace, and place conical flask A in water at 38 °C for heat preservation for 24 h; 4) Take out conical flask A after heat preservation in step 3), pour the upper clear liquid in conical flask A into conical flask B, seal the mouth of conical flask B with a rubber stopper, and place the sealed conical flask B in the crystal growth furnace, and slowly heat from 38 °C to 55 °C at a heating rate of 0.05 °C / h for crystal growth. The finally grown crystal size is about 12×12×2.5 mm in length×width×height 3 .

[0053] Example 3 A preparation method for growing lead bromide-based perovskite single crystals by supplementing bromide ions, comprising: Dissolving NH4Br powder in the CsPbBr3 crystal growth precursor solution and growing in a crystal growth furnace for 20 days. The specific steps are as follows, 1) Dissolve 16.52 g of PbBr2, 6 g of CsBr and 0.55 g of NH4Br powders in 45 mL of dimethyl sulfoxide, and filter to remove impurities using a 0.22 μm organic filter tip. Collect the filtrate, and then add 28.9 mL of cyclohexanol and 16.1 mL of dimethylformamide to the filtrate to prepare a precursor solution; 2) Place the precursor solution prepared in step 1) in conical flask A, and seal the mouth of conical flask A with a rubber stopper; 3) Connect the sealed conical flask A in step 2) to a four-jaw clamp, and connect the four-jaw clamp to a crystal growth furnace, and place conical flask A in water at 40 °C for heat preservation for 24 h; 4) Take out conical flask A after heat preservation in step 3), pour the supernatant in conical flask A into conical flask B, seal the mouth of conical flask B with a rubber stopper, and place the sealed conical flask B in a crystal growth furnace, and slowly heat from 40 °C to 60 °C at a heating rate of 0.05 °C / h for crystal growth. The finally grown crystal size is about 15×15×3 mm in length×width×height 3 The present invention also further verifies the crystals grown by different methods in Examples 2 to 3, and obtains the same results as in Example 1. Thus, it can be determined that adding bromide ions by using NH4Br in the CsPbBr3 single crystal growth precursor solution can change the crystal growth environment, significantly reduce the defect density of the obtained CsPbBr3 single crystal, and improve the crystal quality.

[0054] Comparative Example 1 Do not add NH4Br to the crystal growth precursor solution, and grow in a crystal growth furnace for 15 days. The specific steps are as follows, 1) Dissolve 12.4 g of PbBr2 and 6 g of CsBr powders in 45 mL of dimethyl sulfoxide, and filter to remove impurities using a 0.22 μm organic filter tip. Collect the filtrate, and then add 22.5 mL of cyclohexanol and 22.5 mL of dimethylformamide to the filtrate to prepare a precursor solution; 2) Place the precursor solution prepared in step 1) in conical flask A, and seal the mouth of conical flask A with a rubber stopper; 3) Connect the sealed conical flask A in step 2) to a four-jaw clamp, and connect the four-jaw clamp to a crystal growth furnace, and place conical flask A in water at 35 °C for heat preservation for 24 h; 4) Take out the conical flask A after heat preservation in step 3), pour the upper clear liquid in the conical flask A into the conical flask B, seal the mouth of the conical flask B with a rubber stopper, and place the sealed conical flask B in a crystal growth furnace, and slowly heat it from 35 °C to 50 °C at a heating rate of 0.05 °C / h for crystal growth.

[0055] In Comparative Example 1, without adding NH4Br (wo-NH4Br), the resistivity, defect state density, and deep level transient spectroscopy of the grown CsPbBr3 crystals were tested, and the results are as Figure 2 , Figure 3 and Figure 4 shown. It can be seen that the crystals grown without supplementing Br ions have a low resistivity, a high defect state density, and the densities of V Br - and Pb Br 2+ defects, which are all higher and are not conducive to obtaining high-quality CsPbBr3 single crystals.

[0056] As described above, it is only the specific implementation manner of the present invention, but the protection scope of the present invention is not limited thereto. Any person skilled in the art within the technical scope disclosed by the present invention can easily think of various equivalent modifications or substitutions, and these modifications or substitutions should all be covered within the protection scope of the present invention.

Claims

1. A preparation method of a lead bromide-based perovskite single crystal grown by supplementing bromide ions, characterized in that, It includes the following steps: After dissolving CsBr, PbBr2 and NH4Br powders in dimethyl sulfoxide, cyclohexanol and dimethylformamide are added to obtain a precursor solution; The precursor solution is placed in a sealed container and kept at 35 - 40 °C for 12 - 36 h. During the heat preservation process, the precursor solution will be stratified to obtain the supernatant; The supernatant is placed in a sealed container and heated from 35 - 40 °C to 50 - 60 °C at a rate of 0.01 - 0.08 °C / h for crystal growth, and the lead bromide-based perovskite single crystal grown by supplementing bromide ions is obtained.

2. The preparation method of supplementing bromide ions to grow lead bromide-based perovskite single crystals according to claim 1, characterized in that, The molar ratio of the CsBr, PbBr2 and NH4Br powders is 1:1.5 - 2:0.15 - 0.

25.

3. The preparation method of growing lead bromide-based perovskite single crystals by supplementing bromide ions according to claim 1, wherein, The molar concentration of the CsBr powder in dimethyl sulfoxide is 0.1 - 1.0 mol / L.

4. The preparation method of supplementing bromide ions to grow lead bromide perovskite single crystals according to claim 1, characterized in that, The volume ratio of the dimethyl sulfoxide, dimethylformamide and cyclohexanol is 2 - 2.8:1 - 1.8:

1.

5. The preparation method of supplementing bromide ions to grow lead bromide-based perovskite single crystals according to claim 1, characterized in that, During the process of obtaining the precursor solution, after dissolving CsBr, PbBr2 and NH4Br powders in dimethyl sulfoxide, an organic filter tip is used for filtration to remove impurities, the filtrate is collected, and then cyclohexanol and dimethylformamide are added to the filtrate to prepare the precursor solution.

6. The preparation method of supplementing bromide ions to grow lead bromide-based perovskite single crystals according to claim 5, characterized in that, The pore diameter of the organic filter tip is 0.22 μm.

7. The preparation method of supplementing bromide ions to grow lead bromide-based perovskite single crystals according to claim 1, characterized in that, Both the heat preservation and the crystal growth are carried out in a crystal growth furnace; Among them, the crystal is taken out after 10 - 20 days of crystal growth.

8. The method for preparing a lead-bromine-based perovskite single crystal grown by supplementing bromide ions according to claim 1, wherein: By selecting different crystal growth temperatures, the lengths, widths and heights of the grown CsPbBr3 crystal sizes vary from millimeter level to centimeter level.

9. A lead bromide-based perovskite single crystal grown by supplementing bromide ions prepared by the method according to any one of claims 1 - 8.

10. An application of the lead bromide-based perovskite single crystal grown by supplementing bromide ions according to claim 9 in radiation detection materials.

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