Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite

Lan, Yang; Dringoli, Benjamin J.; Valverde-Chávez, David A.; Ponseca, Carlito S.; Sutton, Mark; He, Yihui; Kanatzidis, Mercouri G.; Cooke, David G.

doi:10.1126/sciadv.aaw5558

Title: Ultrafast correlated charge and lattice motion in a hybrid metal halide perovskite

Journal Article · 30 May 2019 · Science Advances

DOI: https://doi.org/10.1126/sciadv.aaw5558 · OSTI ID:1611842

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^[3]; Sutton, Mark ^[2]; He, Yihui ^[4];

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McGill Univ., Montreal, QC (Canada); DOE/OSTI
McGill Univ., Montreal, QC (Canada)
Linköpings Univ. (Sweden)
Northwestern Univ., Evanston, IL (United States)

Hybrid organic-inorganic halide perovskites have shown remarkable optoelectronic properties, exhibiting an impressive tolerance to defects believed to originate from correlated motion of charge carriers and the polar lattice forming large polarons. Few experimental techniques are capable of directly probing these correlations, requiring simultaneous sub–millielectron volt energy and femtosecond temporal resolution after absorption of a photon. Here, we use time-resolved multi-THz spectroscopy, sensitive to the internal excitations of the polaron, to temporally and energetically resolve the coherent coupling of charges to longitudinal optical phonons in single-crystal CH₃NH₃PbI₃(MAPI). We observe room temperature intraband quantum beats arising from the coherent displacement of charge from the coupled phonon cloud. Our measurements provide strong evidence for the existence of polarons in MAPI at room temperature, suggesting that electron/hole-phonon coupling is a defining aspect of the hybrid metal-halide perovskites contributing to the protection from scattering and enhanced carrier lifetimes that define their usefulness in devices.

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Research Organization:: Univ. of California, Santa Barbara, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0012541

OSTI ID:: 1611842

Journal Information:: Science Advances, Journal Name: Science Advances Journal Issue: 5 Vol. 5; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Coherent charge-phonon correlations and exciton dynamics in orthorhombic CH ₃ NH ₃ PbI ₃ measured by ultrafast multi-THz spectroscopy Lan, Yang; Tao, Xixi; Kong, Xianghua The Journal of Chemical Physics, Vol. 151, Issue 21 https://doi.org/10.1063/1.5127992	journal	December 2019
Time- and momentum-resolved phonon population dynamics with ultrafast electron diffuse scattering de Cotret, Laurent P. René; Pöhls, Jan-Hendrik; Stern, Mark J. arXiv https://doi.org/10.48550/arxiv.1908.02795	text	January 2019
Time- and momentum-resolved phonon population dynamics with ultrafast electron diffuse scattering René de Cotret, Laurent P.; Pöhls, Jan-Hendrik; Stern, Mark J. Physical Review B, Vol. 100, Issue 21 https://doi.org/10.1103/physrevb.100.214115	journal	December 2019

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