Dynamically Disordered Lattice in a Layered Pb-I-SCN Perovskite Thin Film Probed by Two-Dimensional Infrared Spectroscopy

Journal of the American Chemical Society
Jun NishidaMichael D Fayer

Abstract

The dynamically flexible lattices in lead halide perovskites may play important roles in extending carrier recombination lifetime in 3D perovskite solar-cell absorbers and in exciton self-trapping in 2D perovskite white-light phosphors. Two-dimensional infrared (2D IR) spectroscopy was applied to study a recently reported Pb-I-SCN layered perovskite. The Pb-I-SCN perovskite was spin-coated on a SiO2 surface as a thin film, with a thickness of ∼100 nm, where the S12CN- anions were isotopically diluted with the ratio of S12CN:S13CN = 5:95 to avoid vibrational coupling and excitation transfer between adjacent SCN- anions. The 12CN stretch mode of the minor S12CN- component was the principal vibrational probe that reported on the structural evolution through 2D IR spectroscopy. Spectral diffusion was observed with a time constant of 4.1 ± 0.3 ps. Spectral diffusion arises from small structural changes that result in sampling of frequencies within the distribution of frequencies comprising the inhomogeneously broadened infrared absorption band. These transitions among discrete local structures are distinct from oscillatory phonon motions of the lattice. To accurately evaluate the structural dynamics through measurement of spectral d...Continue Reading

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Citations

Mar 15, 2020·Proceedings of the National Academy of Sciences of the United States of America·Eric A MullerMarkus B Raschke
Sep 11, 2020·Journal of the American Chemical Society·Joseph E ThomazMichael D Fayer
May 1, 2020·Journal of the American Chemical Society·Boning WuMichael D Fayer
Feb 27, 2019·The Journal of Physical Chemistry Letters·Daniel B StrausCherie R Kagan
Jan 29, 2019·Chemical Reviews·Matthew D SmithHemamala I Karunadasa
Nov 25, 2020·Inorganic Chemistry·Takafumi YamamotoJames R Neilson
Apr 4, 2020·The Journal of Physical Chemistry Letters·Kyle T MunsonJohn B Asbury
Aug 21, 2020·ACS Applied Materials & Interfaces·Yangyang DangXutang Tao
Sep 18, 2021·The Journal of Physical Chemistry Letters·Saptarsi MondalMinhaeng Cho

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