Dynamic molecule regulated metal halide single crystal growth method and application

Abstract

The invention provides a dynamic molecule regulated metal halide single crystal growth method and application. Dynamic molecules are used as an additive of a metal halide single crystal precursor to synchronously regulate and control the nucleation and growth steps of the single crystal. The dynamic molecules generate reversible structure and performance changes under external stimulation such as light irradiation or temperature change. Before external stimulation such as light irradiation or temperature change is received, the micelle diameter of the metal halide is increased by adding the dynamic molecules, so that the nucleation number of the metal halide single crystal is reduced. After external stimulation, the interaction between the dynamic molecules and the metal halide micelles is reduced, and the original large micelles are dissociated into small micelles, so that the diffusion rate of the metal halide precursor micelles is increased, and the growth rate of the bulk single crystal or single crystal film is improved. Compared with the prior art, the on-off response of the dynamic molecules enables the nucleation number of the metal halide single crystal to be obviously reduced, and the growth rate and the final single crystal size are greatly improved.

Description

Technical Field

[0001] The present invention belongs to the technical field of metal halide single crystal material preparation, and relates to a metal halide single crystal growth method and application controlled by dynamic molecules. Background Art

[0002] Metal halide perovskites are a new class of semiconductor materials with excellent optoelectronic properties that can be prepared in solution. They show promising applications in solar cells, light-emitting diodes, and radiation detection, and have become the target of intense research and development in academia and industry in areas such as new energy and the environment. Currently, these devices primarily use polycrystalline thin films as photoactive materials. Defects such as dangling bonds and unsaturated bonds at the surface and interface significantly reduce device performance and lifetime. In contrast, metal halide single crystals have extremely low defect densities (approximately one hundred thousandth of those in polycrystalline thin films) while possessing excellent light absorption and carrier transport properties, making them ideal candidates for high-performance optoelectronic devices.

[0003] In recent years, metal halide bulk single crystals and thin films have been primarily prepared using methods such as cooling acid, reverse temperature crystallization, antisolvent vapor diffusion crystallization, and spatial confinement. The growth of metal halide single crystals involves multiple processes, including nucleation, mass transfer, and reaction. Effectively controlling the crystallization behavior of metal halide single crystals remains challenging. From a microscopic perspective, the micellar behavior of metal halides directly influences the crystallization behavior of their single crystals. Specifically, larger micelles make it easier for the nuclei to reach a critical nucleation size, resulting in preferential nucleation. However, the subsequent mass transfer process is slow due to the large size of the micelles. Conversely, smaller perovskite micelles make it difficult for the nuclei to reach a critical nucleation size. Homogeneous nucleation results in large-scale random nucleation, but the subsequent diffusion rate is faster during growth. Although the crystal growth rate is improved, the excessive amount of nuclei formed results in a crystal size significantly different from that required for practical applications.

[0004] To address this issue, researchers have used methods such as changing solvent types and engineering additives to intentionally reduce or increase micelle size, thereby individually manipulating the nucleation or mass transfer behavior of metal halide single crystals. However, simultaneously controlling the nucleation and mass transfer processes to obtain high-quality, large-sized metal halide single crystals remains a challenge.

[0005] Dynamic molecules refer to a class of molecules that can undergo structural and performance changes after receiving external stimuli such as light irradiation or temperature changes. Regulating the size of perovskite micelles by dynamic molecular switch response may be a reliable way to fundamentally solve problems such as the large number of perovskite single crystal nucleations and slow growth rate. Summary of the Invention

[0006] The present invention is based on the above-mentioned problems and aims to provide a method for growing metal halide single crystals regulated by dynamic molecules. The method is based on the structural and performance changes of dynamic molecules under external stimuli such as light irradiation or temperature changes, thereby regulating the micelle size of perovskite, ultimately achieving the goal of minimizing the nucleation density and accelerating the single crystal growth rate, and is used to prepare high-quality, large-area metal halide single crystal blocks or single crystal films.

[0007] In order to achieve the above-mentioned purpose, the technical solutions to be protected by the present invention are as follows:

[0008] In a first aspect, the present invention provides a method for growing metal halide single crystals under dynamic molecular control, comprising the following steps:

[0009] (1) Completely dissolving a metal halide precursor with a certain stoichiometric ratio and an appropriate amount of dynamic molecules in a solvent to prepare a precursor solution of a metal halide single crystal;

[0010] (2) Transferring the metal halide precursor solution into a single crystal growth vessel;

[0011] (3) Heating the single crystal growth container to change the concentration of the metal halide precursor and induce the nucleation of the metal halide single crystal;

[0012] (4) Introducing external stimuli such as light irradiation or temperature changes to change the structure and properties of dynamic molecules, affecting the growth process of metal halide single crystals;

[0013] (5) After a period of growth, the metal halide single crystal is separated from the precursor solution, and finally a metal halide bulk single crystal or single crystal thin film is obtained.

[0014] The preferred technical solutions for each step are as follows:

[0015] In step (1), the composition of the metal halide perovskite precursor is: 1 n A x B y X z , where A 1 is at least one of butylamine, hexylamine, phenylethylamine, benzylamine, 1-4-butylene diamine, 4-aminomethylpiperidine, 3-aminomethylpiperidine, N,N-2-dimethylethylenediamine, hexamethylenebisdimethylamine, 3-bromopropylammonium, and N-methylcyclohexylamine; A is at least one of rubidium ion, cesium ion, methylamine ion, formamidine ion, and dimethylamine ion; B is at least one of lead, tin, germanium, bismuth, antimony, iron, manganese, cobalt, copper, and silver ion; X is at least one of iodine, bromine, and chloride ion; the value of n is 0-2; the value of x is 0-7; the value of y is 1-6; and the value of z is 3-19.

[0016] In specific implementation, A 1 , A, B, X or compounds of A, B, X are mixed and dissolved in a solvent in equal molar amounts to form a metal halide perovskite precursor.

[0017] More preferably, the concentration of each compound in the metal halide perovskite precursor is 1-2 mol / L.

[0018] Preferably, the dynamic molecule is selected from at least one of dibenzoyl peroxide, azobenzene, spiropyran, diarylethene, fulgide and derivatives thereof; the derivatives refer to modified derivatives by adding alkanes and heteroatom groups, polymer grafting, etc.

[0019] More preferably, the amount of dynamic molecules added is 0.01-50 g / L.

[0020] Preferably, the solvent is selected from at least one of acetonitrile, γ-butyrolactone, γ-valerolactone, ethylene glycol monomethyl ether, N,N-dimethylformamide, dimethyl sulfoxide, and N-methylpyrrolidone, or a mixed solvent of the above solvents in any proportion.

[0021] More preferably, the complete dissolution refers to heating at room temperature to 100° C. with continuous shaking, ultrasound or magnetic stirring for 1 to 48 hours until the solution is clear and no residue is observed by naked eye, and then filtering with a filter element with a pore size of 0.01 to 1.5 microns.

[0022] In step (2), the single crystal growth container is a container for preparing bulk single crystals or single crystal thin films. For bulk single crystals, the growth container can be at least one of a glass bottle, a beaker, a crystallization dish, a weighing bottle, and a polytetrafluoroethylene bottle; for single crystal thin films, the growth container can be a confined space formed by a combination of any two of a silicon wafer, a conductive glass sheet, a mica sheet, and a polyethylene terephthalate plate, wherein the confined space can be adjusted by inserting a spacer or applying pressure, and the spacer is at least one of aluminum foil, tape, and a silicone gasket.

[0023] Further preferably, the single crystal growth container can be surface treated to reduce adverse effects on perovskite single crystal nucleation and growth. The surface treatment can be hydrophilic or hydrophobic, and the surface treatment agent can be selected from at least one of poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], perfluorododecyltrichlorosilane, [2-(9H-carbazol-9-yl)ethyl]phosphonic acid, and [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid.

[0024] In step (3), the heating of the single crystal growth container is selected from at least one of an oil bath, a water bath, a hot plate, an oven, and laser heating; the heating temperature is any suitable temperature between 30 and 200°C; and the heating rate is 0.1 to 40°C / h.

[0025] The induced nucleation of metal halide single crystals refers to the significant increase in microscopic micelles after the addition of dynamic molecules compared to the perovskite precursor solution without additions; after heating for 1 to 100 hours, a small number of crystal nuclei are preferentially precipitated.

[0026] In step (4), the external stimulus is selected from ultraviolet light irradiation and temperature change; the dynamic molecular structure and performance changes are characterized by the refinement of the size of the perovskite micelles. Specifically, the dynamic molecular structure changes involve isomerization, decomposition, etc.; the performance changes involve dielectric constant, dipole moment, Lewis pH, etc.; the refined perovskite micelles have a faster diffusion rate during the growth process, and efficient mass transfer exhibits an accelerated single crystal growth rate, while also avoiding crystal defects caused by insufficient mass transfer.

[0027] In step (5), the growth time of the single crystal is 0.5 to 400 hours. When obtaining the single crystal, for bulk single crystals, the single crystal is removed with a spoon; for single crystal thin films, the confined space formed by the substrate is separated with a blade; after the bulk single crystal and the single crystal thin film are separated from the solution environment, the residual solution needs to be wiped dry with dust-free paper; the single crystal block and thin film need to be slowly cooled from the growth temperature to room temperature to avoid large thermal stress causing cracking of the single crystal.

[0028] Experimental results show that after ultraviolet light stimulation of the dynamic molecules, their absorbance changes significantly, indicating changes in their structure and properties. During single crystal preparation, the addition of the dynamic molecules increases the number of metal halide micelles compared to before, indicating preferential nucleation. After the introduction of ultraviolet light or temperature stimulation, the metal halide micelles gradually dissociate to a level lower than before the addition of the dynamic molecules. Smaller micelles help reduce the amount of nucleation and mass transfer in the single crystal, resulting in an accelerated crystal growth rate. Optical images of the single crystals show that the metal halide bulk crystals regulated by the dynamic molecules are between 10 and 15 mm in size, exhibit excellent crystallinity, and have a mirror-like reflective surface.

[0029] In a second aspect, the present invention provides a metal halide single crystal material prepared by the above method, wherein the single crystal material is selected from a bulk single crystal or a single crystal thin film.

[0030] In a third aspect, the present invention provides semiconductor devices containing the above-mentioned metal halide single crystal materials, such as solar cells, light-emitting diodes, radiation detection devices, etc.

[0031] In a fourth aspect, the present invention provides an optoelectronic product comprising the semiconductor device described above.

[0032] The beneficial protection and effects of the present invention are as follows:

[0033] The present invention provides a method for controllably preparing metal halide single crystals, which effectively avoids the pain points of uncontrollable nucleation and slow growth. Specifically, the introduction of dynamic molecules causes the metal halide micelles to become larger, and nucleation behavior occurs preferentially. After the introduction of external stimuli such as light irradiation or temperature changes, the structure and properties of the dynamic molecules change, and the metal halide micelles are refined, so that the metal halide nuclei obtain sufficient material supply, thereby accelerating the growth rate of the single crystal. This method has shown significant optimization effects in multiple perovskite single crystal systems. In addition, high-throughput mass transfer can also avoid defects such as vacancies in metal halide single crystals, showing enhanced photoelectric properties. In summary, the introduction of dynamic molecules can obtain fewer nuclei and faster crystal growth rates, and ultimately obtain high-quality, large-area metal halide single crystal blocks and thin films, overcoming the defect that conventional metal halide single crystal regulation can only solve the problems of nucleation or growth during the crystallization process alone. BRIEF DESCRIPTION OF THE DRAWINGS

[0034] Figure 1 The absorbance of the dynamic molecule in ethylene glycol monomethyl ether solvent is shown before and after UV illumination. The figure shows a significant change in the absorbance of the dynamic molecule before and after UV illumination, indicating changes in its structure and properties, which will affect the microscopic micelle state of the metal halide single crystal precursor.

[0035] Figure 2 Figure 1 shows the nucleation statistics for methylamine lead iodine metal halide single crystals. As can be seen from the figure, within a 100×100 mm area, the nucleation rate for both bulk single crystals and thin single crystal films in the blank sample is much greater than that in the sample after dynamic molecule addition. This is determined by the size of the metal halide micelles.

[0036] Figure 3 This is a dynamic light scattering image of a methylamine lead iodine metal halide single crystal solution. As can be seen, the metal halide micelles in the blank sample are concentrated at 0.96 nanometers. After the addition of the dynamic molecules, the metal halide micelles increase to 1.5 nanometers, which preferentially nucleates. When the temperature reaches the thermal decomposition temperature of the dynamic molecules, the metal halide micelles gradually dissociate to 0.72 nanometers. Smaller micelles facilitate mass transfer in the single crystal, resulting in accelerated crystal growth.

[0037] Figure 4 This is a dynamic light scattering image of a methylamine lead bromide metal halide single crystal solution. As can be seen, the metal halide micelles in the blank sample are concentrated at 1.1 nanometers. After the addition of dynamic molecules, the metal halide micelles increase to 2.0 nanometers, which preferentially nucleates. After the introduction of temperature fluctuations, the metal halide micelles gradually dissociate to 0.83 nanometers. Smaller micelles facilitate mass transfer in the single crystal, resulting in accelerated crystal growth.

[0038] Figure 5These are optical images of a bulk single crystal of methylamine lead iodine metal halide before and after the addition of dynamic molecules. As can be seen, the metal halide bulk single crystal after dynamic molecule manipulation is nearly 10 mm in size, exhibiting excellent crystallinity and a mirror-like surface. The blank sample is less than 5 mm in size, exhibits unclear edges and corners, and has a very poor surface quality.

[0039] Figure 6 These are optical images of a bulk single crystal of methylamine lead bromine metal halide before and after the addition of dynamic molecules. As can be seen, the metal halide bulk single crystal after dynamic molecule manipulation is nearly 15 mm in size, exhibiting excellent crystallinity and a mirror-like surface. The blank sample is approximately 5 mm in size, exhibiting poor light transmittance and unclear edges and corners. DETAILED DESCRIPTION

[0040] The following examples and experimental examples further illustrate the present invention and should not be construed as limiting the present invention. The examples do not include detailed descriptions of conventional methods, which are well known to those skilled in the art and are described in numerous publications.

[0041] Unless otherwise defined, all professional and scientific terms used herein have the same meanings as those familiar to those skilled in the art. In addition, any methods and materials similar or equivalent to those described herein can be applied to the present invention, and the preferred implementation methods and materials described in the specific embodiments are for illustrative purposes only.

[0042] The experimental methods in the following examples, where specific conditions are not specified, are generally carried out under conventional conditions or the conditions recommended by the manufacturers. Unless otherwise specified, the reagents used in the examples of the present invention can be obtained from sales companies.

[0043] 1. Preparation of Metal Halide Single Crystals

[0044] Example 1

[0045] 15 mmol of methylamine iodine and 15 mmol of lead iodide were dissolved in 10 mL of ethylene glycol monomethyl ether solvent. 100 mg of dibenzoyl peroxide was added as a dynamic molecule and ultrasonically stirred at room temperature for 6 hours. The metal halide solution was transferred to a crystallizing dish and heated in an oil bath. The nucleation step was performed from room temperature to 57°C at a heating rate of 10°C per hour. After a small number of nuclei were precipitated, heating was continued at 3°C ​​per hour to 70°C. The single crystal growth temperature range was close to the decomposition temperature of dibenzoyl peroxide, which would generate benzoyloxy radicals and refine the micelle size. After 24 hours of growth, the metal halide bulk single crystal was removed with a spatula, the residual solution on the crystal surface was wiped dry with dust-free paper, and the crystal was slowly cooled to room temperature.

[0046] Example 2

[0047] Dissolve 12 mmol of methylamine bromide and 12 mmol of lead bromide in 10 mL of N,N-dimethylformamide solvent, add 75 mg of diarylethene as a dynamic molecule, and shake at room temperature for 8 hours. Transfer the metal halide solution to a glass bottle and heat it in a water bath from room temperature to 41°C at a heating rate of 6°C per hour. After a small amount of crystal nuclei are precipitated, use ultraviolet light to irradiate the crystallization vessel to refine the perovskite micelles. Continue heating at 4°C per hour to 60°C. After growing for 36 hours, use a spatula to remove the metal halide bulk single crystal, wipe the residual solution on the crystal surface with dust-free paper, and slowly cool to room temperature.

[0048] Example 3

[0049] Dissolve 12 mmol of iodine formamidinium and 12 mmol of tin iodide in 10 mL of γ-butyrolactone solvent, add 75 mg of fulgide as a dynamic molecule, and stir magnetically at room temperature for 12 hours. Transfer the metal halide solution to a beaker and heat it on a hot plate from room temperature to 55°C at a heating rate of 5°C per hour. After a small amount of crystal nuclei are precipitated, use ultraviolet light to irradiate the crystallization vessel to refine the perovskite micelles. Continue heating at 3°C ​​per hour to 75°C. After growing for 48 hours, use a medicine spoon to remove the metal halide bulk single crystal, wipe the residual solution on the crystal surface with dust-free paper, and slowly cool to room temperature.

[0050] Example 4

[0051] 1.5 mmol of methylamine iodide and 1.5 mmol of lead iodide were dissolved in 1 mL of γ-butyrolactone, and 5 mg of spiropyran was added as a dynamic molecule. The mixture was magnetically stirred at 60°C for 8 hours. The metal halide solution was transferred to a confined space formed by two pieces of white glass treated with poly[bis(4-phenyl)(2,4,6-trimethylphenyl)amine], with a 100-micron silica gel gasket as the spacer. Heating was performed using a hot plate from 60 to 75°C at a heating rate of 10°C per hour. After a small amount of crystal nuclei were precipitated, the crystallization vessel was irradiated with ultraviolet light to refine the metal halide micelles. The mixture was heated at 2°C per hour to 120°C. After 36 hours of growth, the substrate was separated using a blade, the residual solution on the crystal surface was wiped dry with dust-free paper, and the crystal was slowly cooled to room temperature.

[0052] Example 5

[0053] 1.2 mmol of methylamine bromide and 1.2 mmol of lead bromide were dissolved in 1 mL of N,N-dimethylformamide solvent. 5 mg of azobenzene was added as a dynamic molecule and magnetically stirred at room temperature for 12 hours. The metal halide solution was transferred to a confined space formed by two sheets of conductive glass treated with [2-(3,6-dimethoxy-9H-carbazol-9-yl)ethyl]phosphonic acid, separated by a 70-micron aluminum foil. Heating was performed using a hot plate from room temperature to 40°C at a rate of 5°C per hour. After a small number of crystal nuclei were precipitated, the crystallization vessel was irradiated with ultraviolet light to refine the metal halide micelles. Heating was continued at 3°C ​​per hour to 60°C. After 24 hours of growth, the substrates were separated using a blade, the residual solution on the crystal surface was wiped clean with lint-free paper, and the crystal was slowly cooled to room temperature.

[0054] Example 6

[0055] 1.2 mmol of iodine formamidinium and 1.2 mmol of tin iodide were dissolved in 1 mL of γ-butyrolactone solvent, 1 mg of diarylethene was added as a dynamic molecule, and magnetic stirring was carried out at room temperature for 12 hours. 100 microliters of the metal halide solution was transferred to the confined space formed by two silicon wafers treated with perfluorododecyltrichlorosilane, and the confined space was further reduced using weights. Heating was performed using a heating table from room temperature to 55°C at a heating rate of 5°C per hour. After a small amount of crystal nuclei were precipitated, ultraviolet light was used to irradiate the crystallization vessel to refine the metal halide micelles. Continue heating at 3°C ​​per hour to 75°C. After growing for 48 hours, the substrate was separated using a blade, the residual solution on the crystal surface was wiped dry with dust-free paper, and the crystal was slowly cooled to room temperature.

[0056] 2. Effect Verification

[0057] The effect in Example 1 is verified as follows:

[0058] Figure 1 The absorbance of the dynamic molecule in ethylene glycol monomethyl ether solvent is shown before and after UV illumination. The figure shows a significant change in the absorbance of the dynamic molecule before and after UV illumination, indicating changes in its structure and properties, which will affect the microscopic micelle state of the metal halide single crystal precursor.

[0059] Figure 2 Figure 1 shows the nucleation statistics for methylamine lead iodine metal halide single crystals. As can be seen from the figure, within a 100×100 mm area, the nucleation rate for both bulk single crystals and thin single crystal films in the blank sample is much greater than that in the sample after dynamic molecule addition. This is determined by the size of the metal halide micelles.

[0060] Figure 3This is a dynamic light scattering image of a methylamine lead iodine metal halide single crystal solution. As can be seen, the metal halide micelles in the blank sample are concentrated at 0.96 nanometers. After the addition of the dynamic molecules, the metal halide micelles increase to 1.5 nanometers, which preferentially nucleates. When the temperature reaches the thermal decomposition temperature of the dynamic molecules, the metal halide micelles gradually dissociate to 0.72 nanometers. Smaller micelles facilitate mass transfer in the single crystal, resulting in accelerated crystal growth.

[0061] Figure 4 This is a dynamic light scattering image of a methylamine lead bromide metal halide single crystal solution. As can be seen, the metal halide micelles in the blank sample are concentrated at 1.1 nanometers. After the addition of dynamic molecules, the metal halide micelles increase to 2.0 nanometers, which preferentially nucleates. After the introduction of temperature fluctuations, the metal halide micelles gradually dissociate to 0.83 nanometers. Smaller micelles facilitate mass transfer in the single crystal, resulting in accelerated crystal growth.

[0062] Figure 5 These are optical images of a bulk single crystal of methylamine lead iodine metal halide before and after the addition of dynamic molecules. As can be seen, the metal halide bulk single crystal after dynamic molecule manipulation is nearly 10 mm in size, exhibiting excellent crystallinity and a mirror-like surface. The blank sample is less than 5 mm in size, exhibits unclear edges and corners, and has a very poor surface quality.

[0063] Figure 6 These are optical images of a bulk single crystal of methylamine lead bromine metal halide before and after the addition of dynamic molecules. As can be seen, the metal halide bulk single crystal after dynamic molecule manipulation is nearly 15 mm in size, exhibiting excellent crystallinity and a mirror-like surface. The blank sample is approximately 5 mm in size, exhibiting poor light transmittance and unclear edges and corners.

[0064] Any undescribed parts of the present invention are the same as or implemented using existing technologies. The applicant declares that the present invention uses the above-mentioned embodiments to illustrate the detailed methods of the present invention, but the present invention is not limited to the above-mentioned detailed methods, that is, it does not mean that the present invention must rely on the above-mentioned detailed methods to be implemented. Those skilled in the art should understand that any improvements to the present invention, equivalent replacement of various raw materials of the product of the present invention, addition of auxiliary ingredients, selection of specific methods, etc., all fall within the scope of protection and disclosure of the present invention.

Claims

1. A method for growing metal halide single crystals under dynamic molecular control, characterized in that: The following steps are involved: (1) Completely dissolving a metal halide precursor with a certain stoichiometric ratio and an appropriate amount of dynamic molecules in a solvent to prepare a precursor solution of a metal halide single crystal; (2) Transferring the metal halide precursor solution into a single crystal growth vessel; (3) Heating the single crystal growth container to change the concentration of the metal halide precursor and induce the nucleation of the metal halide single crystal; (4) Introducing external stimuli such as light irradiation or temperature changes to change the structure and properties of dynamic molecules, affecting the growth process of metal halide single crystals; (5) After a period of growth, the metal halide single crystal is separated from the precursor solution, and finally a metal halide bulk single crystal or single crystal thin film is obtained.

2. The method for growing metal halide single crystals under dynamic molecular control according to claim 1, wherein: in, In step (1), the composition of the metal halide perovskite precursor is: 1 n A x B y X z , where A 1 is at least one of butylamine, hexylamine, phenylethylamine, benzylamine, 1-4-butylene diamine, 4-aminomethylpiperidine, 3-aminomethylpiperidine, N,N-2-dimethylethylenediamine, hexamethylenebisdimethylamine, 3-bromopropylammonium, and N-methylcyclohexylamine; A is at least one of rubidium ion, cesium ion, methylamine ion, formamidine ion, and dimethylamine ion; B is at least one of lead, tin, germanium, bismuth, antimony, iron, manganese, cobalt, copper, and silver ion; X is at least one of iodine, bromine, and chloride ion; the value of n is 0-2; the value of x is 0-7; the value of y is 1-6; and the value of z is 3-19.

3. The method for growing metal halide single crystals under dynamic molecular control according to claim 2, wherein: in, A 1 , A, B, X or compounds of A, B, X are mixed and dissolved in a solvent in equal molar amounts to form a metal halide perovskite precursor; The concentration of each compound in the metal halide perovskite precursor is 1~2 mol / L.

4. The method for growing metal halide single crystals under dynamic molecular control according to claim 1, wherein: in, The dynamic molecule is selected from at least one of dibenzoyl peroxide, azobenzene, spiropyran, diarylethene, fulgide and derivatives thereof, and the addition amount is 0.01-50 g / L; The solvent is selected from one or more of acetonitrile, γ-butyrolactone, γ-valerolactone, ethylene glycol monomethyl ether, N,N-dimethylformamide, dimethyl sulfoxide, and N-methylpyrrolidone, mixed in any proportion.

5. The method for growing metal halide single crystals under dynamic molecular control according to claim 1, wherein: in, The metal halide precursor and dynamic molecule are heated at room temperature to 100° C. with continuous shaking, ultrasound or magnetic stirring for 1 to 48 hours until the solution is clear and no residue is observed by naked eye, and then filtered using a filter element with a pore size of 0.01 to 1.5 microns.

6. The method for growing metal halide single crystals under dynamic molecular control according to claim 1, wherein: in, The single crystal growth container in step (2) and step (3) includes a bulk single crystal growth container and a single crystal thin film growth container; the bulk single crystal growth container is selected from at least one of a glass bottle, a beaker, a crystallization dish, a weighing bottle, and a polytetrafluoroethylene bottle; the single crystal thin film growth container is selected from a limited space formed by a combination of any two of a silicon wafer, a conductive glass sheet, a mica sheet, and a polyethylene terephthalate plate, and the size of the space is adjusted by inserting a spacer or applying pressure, and the spacer is selected from at least one of aluminum foil, tape, and a silicone gasket. The single crystal growth container is surface treated in advance to reduce adverse effects on the nucleation and growth of the perovskite single crystal, wherein the surface treatment is a hydrophilic or hydrophobic treatment; In step (3), the method of heating the single crystal growth container is selected from at least one of oil bath, water bath, hot plate, oven, and laser heating; the heating temperature is any suitable temperature between 30°C and 200°C; and the heating rate is 0.1°C to 40°C per hour.

7. The method for growing metal halide single crystals under dynamic molecular control according to claim 1, wherein: in, In step (4), the light irradiation is selected from ultraviolet light irradiation; In step (5), the single crystal growth time is 0.5 to 400 hours, and the temperature is continuously increased by 13 to 50°C from the nucleation temperature at a heating rate of 2 to 4°C during the growth process; When separating single crystals, for bulk single crystals, the single crystal is taken out with a spoon; for single crystal films, the confined space formed by the substrate is separated by a blade; after the bulk single crystal and the single crystal film are separated from the solution environment, the residual solution needs to be wiped dry with dust-free paper; the bulk single crystal and the single crystal film need to be slowly cooled from the growth temperature to room temperature to avoid large thermal stress causing cracking of the single crystal.

8. A metal halide single crystal material, characterized in that: The single crystal material is prepared by the method according to any one of claims 1 to 7.

9. A semiconductor device, characterized in that: Contains the metal halide single crystal material according to claim 8.

10. A photoelectric product, characterized in that: A semiconductor device comprising the semiconductor device according to claim 9.

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