High-quality bulk hybrid perovskite single crystals within minutes by inverse temperature crystallization

Abstract

Single crystals of methylammonium lead trihalide perovskites (MAPbX < inf > 3 < /inf > ; MA=CH < inf > 3 < /inf > NH < inf > 3 < /inf > < sup > + < /sup > , X=Br < sup > - < /sup > or I < sup > - < /sup > ) 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 MAPbX < inf > 3 < /inf > single crystals, an order of magnitude faster than previous reports. The process is based on our observation of the substantial decrease of MAPbX < inf > 3 < /inf > 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 MAPbX < inf > 3 < /inf > 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.