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Title: Local polar fluctuations in lead halide perovskite crystals

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 (CH 3NH 3PbBr 3) and all-inorganic (CsPbBr 3) 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. Furthermore, 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 CsPbBr 3.

Authors:
 [1];  [1];  [2];  [3];  [1];  [4];  [2];  [5];  [3];  [6];  [1];  [2];  [7];  [1]
  1. Columbia Univ., New York, NY (United States)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States)
  3. Weizmann Institute of Science, Rehovoth (Israel)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
  5. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
  6. Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States)
  7. Columbia Univ., New York, NY (United States); Univ. Federal de Minas Gerais, Belo Horizonte (Brazil)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOE National Nuclear Security Administration (NNSA)
OSTI Identifier:
1352545
Alternate Identifier(s):
OSTI ID: 1349148
Grant/Contract Number:  
SC0001085; IOF-622653; N00014-14-1-0761; N00014-12-1-1033; FG02-07ER46431; J3608-N20; NA0002522; AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 118; Journal Issue: 13; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 36 MATERIALS SCIENCE; local polar fluctuations; hybrid perovskites; low frequency Raman scattering; molecular dynamics; radiation detection; Central peak

Citation Formats

Yaffe, Omer, Guo, Yinsheng, Tan, Liang Z., Egger, David A., Hull, Trevor, Stoumpos, Constantinos C., Zheng, Fan, Heinz, Tony F., Kronik, Leeor, Kanatzidis, Mercouri G., Owen, Jonathan S., Rappe, Andrew M., Pimenta, Marcos A., and Brus, Louis E.. Local polar fluctuations in lead halide perovskite crystals. United States: N. p., 2017. Web. doi:10.1103/PhysRevLett.118.136001.
Yaffe, Omer, Guo, Yinsheng, Tan, Liang Z., Egger, David A., Hull, Trevor, Stoumpos, Constantinos C., Zheng, Fan, Heinz, Tony F., Kronik, Leeor, Kanatzidis, Mercouri G., Owen, Jonathan S., Rappe, Andrew M., Pimenta, Marcos A., & Brus, Louis E.. Local polar fluctuations in lead halide perovskite crystals. United States. doi:10.1103/PhysRevLett.118.136001.
Yaffe, Omer, Guo, Yinsheng, Tan, Liang Z., Egger, David A., Hull, Trevor, Stoumpos, Constantinos C., Zheng, Fan, Heinz, Tony F., Kronik, Leeor, Kanatzidis, Mercouri G., Owen, Jonathan S., Rappe, Andrew M., Pimenta, Marcos A., and Brus, Louis E.. Tue . "Local polar fluctuations in lead halide perovskite crystals". United States. doi:10.1103/PhysRevLett.118.136001. https://www.osti.gov/servlets/purl/1352545.
@article{osti_1352545,
title = {Local polar fluctuations in lead halide perovskite crystals},
author = {Yaffe, Omer and Guo, Yinsheng and Tan, Liang Z. and Egger, David A. and Hull, Trevor and Stoumpos, Constantinos C. and Zheng, Fan and Heinz, Tony F. and Kronik, Leeor and Kanatzidis, Mercouri G. and Owen, Jonathan S. and Rappe, Andrew M. and Pimenta, Marcos A. and Brus, Louis E.},
abstractNote = {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. Furthermore, 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.},
doi = {10.1103/PhysRevLett.118.136001},
journal = {Physical Review Letters},
number = 13,
volume = 118,
place = {United States},
year = {Tue Mar 28 00:00:00 EDT 2017},
month = {Tue Mar 28 00:00:00 EDT 2017}
}

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