Local Polar Fluctuations in Lead Halide Perovskite Crystals

Omer Yaffe, Yinsheng Guo, Liang Z. Tan, David A. Egger, Trevor Hull, Constantinos C. Stoumpos, Fan Zheng, Tony F. Heinz, Leeor Kronik, Mercouri G. Kanatzidis, Jonathan S. Owen, Andrew M. Rappe, Marcos A. Pimenta, and Louis E. Brus
Phys. Rev. Lett. 118, 136001 – Published 28 March 2017
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Abstract

Hybrid lead-halide perovskites have emerged as an excellent class of photovoltaic materials. Recent reports suggest that the organic molecular cation is responsible for local polar fluctuations that inhibit carrier recombination. We combine low-frequency Raman scattering with first-principles molecular dynamics (MD) to study the fundamental nature of these local polar fluctuations. Our observations of a strong central peak in the cubic phase of both hybrid (CH3NH3PbBr3) and all-inorganic (CsPbBr3) lead-halide perovskites show that anharmonic, local polar fluctuations are intrinsic to the general lead-halide perovskite structure, and not unique to the dipolar organic cation. MD simulations indicate that head-to-head Cs motion coupled to Br face expansion, occurring on a few hundred femtosecond time scale, drives the local polar fluctuations in CsPbBr3.

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  • Received 10 October 2016

DOI:https://doi.org/10.1103/PhysRevLett.118.136001

© 2017 American Physical Society

Physics Subject Headings (PhySH)

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Omer Yaffe1, Yinsheng Guo1, Liang Z. Tan2, David A. Egger3, Trevor Hull1, Constantinos C. Stoumpos4, Fan Zheng2, Tony F. Heinz5,6, Leeor Kronik3, Mercouri G. Kanatzidis4,7, Jonathan S. Owen1, Andrew M. Rappe2, Marcos A. Pimenta1,8, and Louis E. Brus1,*

  • 1Department of Chemistry, Columbia University, New York, New York 10027, USA
  • 2Department of Chemistry, University of Pennsylvania, Philadelphia, Pennsylvania 19104, USA
  • 3Department of Materials and Interfaces, Weizmann Institute of Science, Rehovoth 76100, Israel
  • 4Materials Science Division, Argonne National Laboratory, Argonne, Illinois 60439, USA
  • 5Department of Applied Physics, Stanford University, Stanford, California 94305, USA
  • 6SLAC National Accelerator Laboratory, Menlo Park, California 94025, United States
  • 7Department of Chemistry, Northwestern University, Evanston, Illinois 60208, USA
  • 8Departamento de Fisica, Universidade Federal de Minas Gerais, 30123-970 Belo Horizonte, Brazil

  • *leb26@columbia.edu

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Issue

Vol. 118, Iss. 13 — 31 March 2017

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