Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites

Bischak, Connor G.; Wong, Andrew B.; Lin, Elbert; Limmer, David T.; Yang, Peidong; Ginsberg, Naomi S.

doi:10.1021/acs.jpclett.8b01512

Tunable Polaron Distortions Control the Extent of Halide Demixing in Lead Halide Perovskites

Journal Article · Fri Jul 06 04:00:00 EDT 2018 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.8b01512· OSTI ID:1601185

^[1]; ^[1]; Lin, Elbert ^[1]; Limmer, David T. ^[2]; ^[2]; ^[2]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States). Kavli Energy NanoScience Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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(Br_xI_{1- 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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1601185

Alternate ID(s):: OSTI ID: 1543670

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 14 Vol. 9; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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