Photocarrier-induced persistent structural polarization in soft-lattice lead halide perovskites

Qian, Qi; Wan, Zhong; Takenaka, Hiroyuki; Keum, Jong K.; Smart, Tyler J.; Wang, Laiyuan; Wang, Peiqi; Zhou, Jingyuan; Ren, Huaying; Xu, Dong; Huang, Yu; Ping, Yuan; Duan, Xiangfeng

doi:10.1038/s41565-022-01306-x

Photocarrier-induced persistent structural polarization in soft-lattice lead halide perovskites

Journal Article · Thu Jan 26 00:00:00 EST 2023 · Nature Nanotechnology

DOI:https://doi.org/10.1038/s41565-022-01306-x· OSTI ID:1991698

^[1]; ^[1]; Takenaka, Hiroyuki ^[2]; ^[3]; Smart, Tyler J. ^[4]; ^[1]; Wang, Peiqi ^[1]; Zhou, Jingyuan ^[1]; ^[1]; Xu, Dong ^[1]; ^[1]; ^[2]; ^[1]

Univ. of California, Los Angeles, CA (United States)
Univ. of California, Santa Cruz, CA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of California, Santa Cruz, CA (United States); Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

The success of the lead halide perovskites in diverse optoelectronics has motivated considerable interest in their fundamental photocarrier dynamics. Here, in this work, we report the discovery of photocarrier-induced persistent structural polarization and local ferroelectricity in lead halide perovskites. Photoconductance studies of thin-film single-crystal CsPbBr₃ at 10 K reveal long-lasting persistent photoconductance with an ultralong photocarrier lifetime beyond 10⁶ s. X-ray diffraction studies reveal that photocarrier-induced structural polarization is present up to a critical freezing temperature. Photocapacitance studies at cryogenic temperatures further demonstrate a systematic local phase transition from linear dielectric to paraelectric and relaxor ferroelectric under increasing illumination. Our theoretical investigations highlight the critical role of photocarrier–phonon coupling and large polaron formation in driving the local relaxor ferroelectric phase transition. Our findings show that this photocarrier-induced persistent structural polarization enables the formation of ferroelectric nanodomains at low temperature, which suppress carrier recombination and offer the possibility of exploring intriguing carrier–phonon interplay and the rich polaron photophysics.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725; AC52-07NA27344

OSTI ID:: 1991698

Journal Information:: Nature Nanotechnology, Journal Name: Nature Nanotechnology Journal Issue: 4 Vol. 18; ISSN 1748-3387

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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