Abstract
Single crystals of methylammonium lead trihalide perovskites (MAPbX3; MA=CH3NH3+, X=Br− or I−) have shown remarkably low trap density and charge transport properties; however, growth of such high-quality semiconductors is a time-consuming process. Here we present a rapid crystal growth process to obtain MAPbX3 single crystals, an order of magnitude faster than previous reports. The process is based on our observation of the substantial decrease of MAPbX3 solubility, in certain solvents, at elevated temperatures. The crystals can be both size- and shape-controlled by manipulating the different crystallization parameters. Despite the rapidity of the method, the grown crystals exhibit transport properties and trap densities comparable to the highest quality MAPbX3 reported to date. The phenomenon of inverse or retrograde solubility and its correlated inverse temperature crystallization strategy present a major step forward for advancing the field on perovskite crystallization.
Highlights
Single crystals of methylammonium lead trihalide perovskites (MAPbX3; MA 1⁄4 CH3NH3þ, X 1⁄4 Br À or I À ) have shown remarkably low trap density and charge transport properties; growth of such high-quality semiconductors is a time-consuming process
Single crystals of MAPbBr3 and MAPbI3 were shown to possess long carrier diffusion lengths and a remarkably low trap-state densities, which is comparable to the best photovoltaicquality silicon[17]
These properties provide a view of the ultimate potential of hybrid perovskites, and make single crystals of MAPbX3 a highly desirable semiconductor for optoelectronic applications that are much broader than their polycrystalline thin film counterpart
Summary
Single crystals of methylammonium lead trihalide perovskites (MAPbX3; MA 1⁄4 CH3NH3þ , X 1⁄4 Br À or I À ) have shown remarkably low trap density and charge transport properties; growth of such high-quality semiconductors is a time-consuming process. Single crystals of MAPbBr3 and MAPbI3 were shown to possess long carrier diffusion lengths and a remarkably low trap-state densities, which is comparable to the best photovoltaicquality silicon[17] These properties provide a view of the ultimate potential of hybrid perovskites, and make single crystals of MAPbX3 a highly desirable semiconductor for optoelectronic applications that are much broader than their polycrystalline thin film counterpart. We show that MAPbX3 perovskites exhibit inverse temperature solubility behaviour in certain solvents This novel phenomenon in hybrid perovskites enabled us to design an innovative crystallization method for these materials, referred to here as inverse temperature crystallization (ITC), to rapidly grow high-quality size- and shape-controlled single crystals of both. The versatility of our approach provides the continuous enlargement of crystals, through replacement of the depleted growth solution, and the use of templates for controlling their shapes
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