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Title: How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites

Abstract

Here we develop a microscopic approach aimed at the description of a suite of physical effects related to carrier transport in, and the optical properties of, halide perovskites. Our theory is based on the description of the nuclear dynamics to all orders and goes beyond the common assumption of linear electron-phonon coupling in describing the carrier dynamics and band gap characteristics. When combined with first-principles calculations and applied to the prototypical MAPbI3 system, our theory explains seemingly disparate experimental findings associated with both the charge-carrier mobility and optical absorption properties, including their temperature dependencies. Furthermore, our findings demonstrate that orbital-overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [2];  [1]
  1. Columbia Univ., New York, NY (United States)
  2. Univ. of Pennsylvania, Philadelphia, PA (United States)
  3. Univ. of Regensburg, Regensburg (Germany)
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1563984
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 12; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Mayers, Matthew Z., Tan, Liang Z., Egger, David A., Rappe, Andrew M., and Reichman, David R. How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.8b04276.
Mayers, Matthew Z., Tan, Liang Z., Egger, David A., Rappe, Andrew M., & Reichman, David R. How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites. United States. https://doi.org/10.1021/acs.nanolett.8b04276
Mayers, Matthew Z., Tan, Liang Z., Egger, David A., Rappe, Andrew M., and Reichman, David R. Fri . "How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites". United States. https://doi.org/10.1021/acs.nanolett.8b04276. https://www.osti.gov/servlets/purl/1563984.
@article{osti_1563984,
title = {How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites},
author = {Mayers, Matthew Z. and Tan, Liang Z. and Egger, David A. and Rappe, Andrew M. and Reichman, David R.},
abstractNote = {Here we develop a microscopic approach aimed at the description of a suite of physical effects related to carrier transport in, and the optical properties of, halide perovskites. Our theory is based on the description of the nuclear dynamics to all orders and goes beyond the common assumption of linear electron-phonon coupling in describing the carrier dynamics and band gap characteristics. When combined with first-principles calculations and applied to the prototypical MAPbI3 system, our theory explains seemingly disparate experimental findings associated with both the charge-carrier mobility and optical absorption properties, including their temperature dependencies. Furthermore, our findings demonstrate that orbital-overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.},
doi = {10.1021/acs.nanolett.8b04276},
journal = {Nano Letters},
number = 12,
volume = 18,
place = {United States},
year = {2018},
month = {11}
}

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