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

Myeongkee Park, Amanda J. Neukirch, Sebastian E. Reyes-Lillo, Minliang Lai, Scott R. Ellis, Daniel Dietze, Jeffrey B. Neaton, Peidong Yang, Sergei Tretiak and Richard A. Mathies ()
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Myeongkee Park: University of California
Amanda J. Neukirch: Los Alamos National Laboratory
Sebastian E. Reyes-Lillo: Universidad Andres Bello
Minliang Lai: University of California
Scott R. Ellis: University of California
Daniel Dietze: Osram Opto Semiconductors GmbH
Jeffrey B. Neaton: University of California
Peidong Yang: University of California
Sergei Tretiak: Los Alamos National Laboratory
Richard A. Mathies: University of California

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: Abstract 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 PbI64− 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.

Date: 2018
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DOI: 10.1038/s41467-018-04946-7

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