Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite

Park, Myeongkee; Neukirch, Amanda J.; Reyes-Lillo, Sebastian E.; Lai, Minliang; Ellis, Scott R.; Dietze, Daniel; Neaton, Jeffrey B.; Yang, Peidong; Tretiak, Sergei; Mathies, Richard A.

doi:10.1038/s41467-018-04946-7

Excited-state vibrational dynamics toward the polaron in methylammonium lead iodide perovskite

Journal Article · Thu Jun 28 00:00:00 EDT 2018 · Nature Communications

DOI:https://doi.org/10.1038/s41467-018-04946-7· OSTI ID:1459840

Park, Myeongkee ^[1]; Neukirch, Amanda J. ^[2]; Reyes-Lillo, Sebastian E. ^[3]; Lai, Minliang ^[4]; Ellis, Scott R. ^[4]; ^[5]; Neaton, Jeffrey B. ^[6]; Yang, Peidong ^[7]; ^[2]; ^[4]

Univ. of California, Berkeley, CA (United States). Dept. of Chemistry; Dong-A Univ., Busan (Korea, Republic of). Dept. of Chemistry
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Andrés Bello National Univ., Santiago (Chile). Dept. of Physical Sciences; Univ. of California, Berkeley, CA (United States). Dept. of Physics; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
Osram Opto Semiconductors GmbH, Regensburg (Germany)
Univ. of California, Berkeley, CA (United States). Dept. of Physics. Kavli Energy NanoSciences Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
Univ. of California, Berkeley, CA (United States). Dept. of Chemistry. Dept. of Materials Science and Engineering. Kavli Energy NanoSciences Inst.; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division

Hybrid organic–inorganic perovskites have attractive optoelectronic properties including exceptional solar cell performance. The improved properties of perovskites have been attributed to polaronic effects involving stabilization of localized charge character by structural deformations and polarizations. Here we examine the Pb–I structural dynamics leading to polaron formation in methylammonium lead iodide perovskite by transient absorption, time-domain Raman spectroscopy, and density functional theory. Methylammonium lead iodide perovskite exhibits excited-state coherent nuclear wave packets oscillating at ~20, ~43, and ~75 cm^-1 which involve skeletal bending, in-plane bending, and c-axis stretching of the I–Pb–I bonds, respectively. The amplitudes of these wave packet motions report on the magnitude of the excited-state structural changes, in particular, the formation of a bent and elongated octahedral PbI₆^4- geometry. We have predicted the excited-state geometry and structural changes between the neutral and polaron states using a normal-mode projection method, which supports and rationalizes the experimental results. This study reveals the polaron formation via nuclear dynamics that may be important for efficient charge separation.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: LANL Laboratory Directed Research and Development (LDRD) Program; LBNL Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC52-06NA25396

OSTI ID:: 1459840

Alternate ID(s):: OSTI ID: 1506380

Report Number(s):: LA-UR--17-31256

Journal Information:: Nature Communications, Journal Name: Nature Communications Vol. 9; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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