# US 10,483,046 B2 · Organometallic halide perovskite single crystals having low defect density and methods of preparation thereof > Agents: this data is available as JSON from the patentgrep API and MCP server — see https://patentgrep.com/llms.txt - Number: US 10,483,046 B2 - Document ID: US10483046B2 - Status: Granted - Kind: B2 - Application number: 15/503,544 - Filed: 2015-08-12 - Published: 2017-08-17 - Granted: 2019-11-19 - Earliest claimed: 2014-08-14 - Assignees: King Abdullah University of Science and Technology - Applicants: King Abdullah University of Science and Technology - Inventors: Osman M. Bakr; Dong Shi - Web page: https://patentgrep.com/patent/US10483046B2 ## CPC - C30B 7/14: the crystallising materials being formed by chemical reactions in the solution - C30B 29/12: Halides - C30B 29/54: Organic compounds - H01G 9/2009: {Solid electrolytes} - H10K 71/15: characterised by the solvent used - H10K 85/30: Coordination compounds - H10K 85/50: Organic perovskites; Hybrid organic-inorganic perovskites [HOIP], e.g. CH3NH3PbI3 - H10K 30/50: Photovoltaic [PV] devices - Y02E 10/542: Dye sensitized solar cells - Y02E 10/549: Organic PV cells - Y02P 70/50: Manufacturing or production processes characterised by the final manufactured product - C30B: SINGLE-CRYSTAL GROWTH (by using ultra-high pressure, e.g. for the formation of diamonds, B01J3/06); UNIDIRECTIONAL SOLIDIFICATION OF EUTECTIC MATERIAL OR UNIDIRECTIONAL DEMIXING OF EUTECTOID MATERIAL; REFINING BY ZONE-MELTING OF MATERIAL (zone-refining of metals or alloys C22B); PRODUCTION OF A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE (casting of metals, casting of other substances by the same processes or devices B22D; working of plastics B29; modifying the physical structure of metals or alloys C21D, C22F); SINGLE CRYSTALS OR HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE; AFTER-TREATMENT OF SINGLE CRYSTALS OR A HOMOGENEOUS POLYCRYSTALLINE MATERIAL WITH DEFINED STRUCTURE (for producing semiconductor devices or parts thereof H10); APPARATUS THEREFOR - H01G: CAPACITORS; CAPACITORS, RECTIFIERS, DETECTORS, SWITCHING DEVICES, LIGHT-SENSITIVE OR TEMPERATURE-SENSITIVE DEVICES OF THE ELECTROLYTIC TYPE (selection of specified materials as dielectric H01B3/00; capacitors having potential barriers H10D1/62, H10K10/10) - H10K: ORGANIC ELECTRIC SOLID-STATE DEVICES - Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION - Y02P: CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS ## Abstract Embodiments of the present disclosure provide for single crystal organometallic halide perovskites, methods of making, methods of use, devices incorporating single crystal organometallic halide perovskites, and the like. ## Claims ### Claim 1 A method of making a single crystal, comprising: providing a first reservoir including a first liquid, wherein the first liquid includes a first precursor and an organic cation precursor dissolved in a first liquid solvent; providing a second reservoir including a second liquid, wherein the second liquid is a non-solvent; wherein the first reservoir and second reservoir are separated by a boundary so that the first liquid and the second liquid do not contact one another, wherein the first reservoir and the second reservoir are in a closed system; allowing for vapor diffusion of the second liquid into the first liquid so that the solubility of the first precursor and organic cation precursor gradually decreases; and precipitating out an organometallic halide perovskite single crystal in the first reservoir. ### Claim 2 (depends on 1) The method of claim 1, wherein the organometallic halide perovskite single crystal has the following formula: AMX3, wherein A is an organic cation, M is selected from the group consisting of: Pb, Sn, Cu, Ni, Co, Fe, Mn, Pd, Cd, Ge, and Eu, and X is a halide. ### Claim 3 (depends on 1) The method of claim 1, wherein the first liquid solvent is selected from the group consisting of: N,N-dimethylformamide (DMF), dimethylsulfoxide (DMSO), gamma-butylrolactone (GBR), and a combination thereof. ### Claim 4 (depends on 3) The method of claim 3, wherein the first precursor is a halide salt of M, wherein M is selected from the group consisting of: Pb, Sn, Cu, Ni, Co, Fe, Mn, Pd, Cd, Ge, and Eu. ### Claim 5 (depends on 4) The method of claim 4, wherein the first precursor is selected from PbBr2 or SnBr2. ### Claim 6 (depends on 1) The method of claim 1, wherein the organic cation precursor is a halide salt of A, wherein A is an organic cation. ### Claim 7 (depends on 6) The method of claim 6, wherein the organic cation precursor is selected from the group consisting of: methylammonium bromide, methylammonium iodide, methylammonium chloride, formamidinium chloride, formamidinium bromide, ormamidinium iodide, and combination thereof. ### Claim 8 (depends on 1) The method of claim 1, wherein the non-solvent has a lower boiling point than the first liquid solvent, and the first precursor and the organic cation precursor are not soluble in the non-solvent. ### Claim 9 (depends on 1) The method of claim 1, wherein the non-solvent is selected from the group consisting of: dichloromethane, chloroform, acetonitrile, toluene, and a combination thereof. ### Claim 10 (depends on 1) The method of claim 1, wherein the organometallic halide perovskite single crystal is selected from the group consisting of: methylammonium lead chloride (MAPbCl3), methylammonium lead iodide (MAPbI3), methylammonium lead bromide (MAPbBr3), formamidinium lead chloride (FAPbCl3), formamidinum lead bromide (FAPbBr3), formamidinum lead iodide (FAPbI3), methylammonium tin chloride (MASnCl3), methylammonium tin bromide (MASnBr3), methylammonium tin iodide (MASnI3), formamidinium tin chloride (FASnCl3), formamidinium tin bromide (FASnBr3), and formamidinium tin iodide (FASnI3). ### Claim 11 (depends on 1) The method of claim 1, wherein the vapor diffusion proceeds at about room temperature and pressure. ### Claim 12 (depends on 1) The method of claim 1, further comprising adjusting a temperature and/or pressure of closed system to control the rate of formation of the organometallic halide perovskite single crystal. ### Claim 13 (depends on 1) The method of claim 1, wherein the organometallic halide perovskite single crystal is formed over a time period ranging from about an hour to one or more days. ### Claim 14 (depends on 1) The method of claim 1, wherein the first reservoir and the second reservoir are a single structure or separate structures.