Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 9, Issue 14, Pages 3998-4005Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.8b01512
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Funding
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division within the Physical Chemistry of Inorganic Nanostructures Program [DE-AC02-05-CH11231, KC3103]
- Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy [DE-AC02-05CH11231]
- David and Lucile Packard Fellowship for Science and Engineering
- STROBE, A National Science Foundation Science and Technology Center [DMR 1548924]
- Lam Research Graduate Fellowship
- NSF Graduate Research Fellowship [DGE 1106400]
- Alfred P. Sloan Research Fellowship
- Camille Dreyfus Teacher-Scholar Award
- UC Berkeley College of Chemistry
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Photoinduced phase separation in mixed halide perovskites emerges from their electro-mechanical properties and high ionic conductivities, resulting in photoinduced I--rich charge carrier traps that diminish photovoltaic performance. Whether photoinduced phase separation stems from the polycrystalline microstructure or is an intrinsic material property has been an open question. We investigate the nanoscale photoinduced behavior of single-crystal mixed Br-/I- methylammonium (MA(+)) lead halide perovskite (MAPb(BrxI1-x)(3)) nanoplates, eliminating effects from extended structural defects. Even in these nanoplates, we find that phase separation occurs, resulting in I--rich clusters that are nucleated stochastically and stabilized by polarons. Upon lowering the electron-phonon coupling strength by partially exchanging MA(+) for Cs+, a phase-separated steady state is not reached, nevertheless transient I- clustering still occurs. Our results, supported by multiscale modeling, demonstrate that photoinduced phase separation is an intrinsic property of mixed halide perovskites, the extent and dynamics of which depends on the electron-phonon coupling strength.
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