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RAPID Manuscript_ChemRxiv combined final.pdf (12.41 MB)

Robot-Accelerated Perovskite Investigation and Discovery (RAPID): 1. Inverse Temperature Crystallization

submitted on 22.10.2019, 15:42 and posted on 24.10.2019, 21:04 by Zhi Li, Mansoor Ani Najeeb, Liana Alves, Alyssa Sherman, Peter Cruz Parrilla, Ian M. Pendleton, Matthias Zeller, Joshua Schrier, Alexander J. Norquist, Emory Chan
Metal halide perovskites are a promising class of materials for next-generation photovoltaic and optoelectronic devices. The discovery and full characterization of new perovskite-derived materials are limited by the difficulty of growing high quality crystals needed for single-crystal X-ray diffraction studies. We present the first automated, high-throughput approach for metal halide perovskite single crystal discovery based on inverse temperature crystallization (ITC) as a means to rapidly identify and optimize synthesis conditions for the formation of high quality single crystals. Using this automated approach, a total of 1928 metal halide perovskite synthesis reactions were conducted using six organic ammonium cations (methylammonium, ethylammonium, n-butylammonium, formamidinium, guanidinium, and acetamidinium), increasing the number of metal halide perovskite materials accessible by ITC syntheses by three and resulting in the formation of a new phase, [C2H7N2][PbI3]. This comprehensive dataset allows for a statistical quantification of the total experimental space and of the likelihood of large single crystal formation. Moreover, this dataset enables the construction and evaluation of machine learning models for predicting crystal formation conditions. This work is a proof-of-concept that combining high throughput experimentation and machine learning accelerates and enhances the study of metal halide perovskite crystallization. This approach is designed to be generalizable to different synthetic routes for the acceleration of materials discovery.


Defense Advanced Research Projects Agency (DARPA) Contract No. HR001118C0036

U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Contract No. DE-AC02-05CH11231

U.S. Department of Energy, Office of Science, Office of Workforce Development for Teachers and Scientists (WDTS), Contract No. DE-AC02-05CH11231

Henry Dreyfus Teacher-Scholar Award (TH-14-010)

National Science Foundation, Major Research Instrumentation Program, Grant No. CHE 1625543


Email Address of Submitting Author


Lawrence Berkeley National Laboratory


United States

ORCID For Submitting Author


Declaration of Conflict of Interest

No conflict of interest