How Lattice and Charge Fluctuations Control Carrier Dynamics in Halide Perovskites

Matthew Z. Mayers, Liang Z. Tan, David A. Egger, Andrew M. Rappe, David R. Reichman

Research output: Contribution to journalArticlepeer-review

100 Scopus citations

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 MAPbI 3 system, our theory explains seemingly disparate experimental findings associated with both the charge-carrier mobility and optical absorption properties, including their temperature dependencies. Our findings demonstrate that orbital-overlap fluctuations in the lead-halide structure plays a significant role in determining the optoelectronic features of halide perovskites.

Original languageEnglish
Pages (from-to)8041-8046
Number of pages6
JournalNano Letters
Volume18
Issue number12
DOIs
StatePublished - 12 Dec 2018
Externally publishedYes

Keywords

  • Halide perovskites
  • carrier dynamics
  • carrier mobility
  • electron-phonon coupling
  • structural dynamics
  • theoretical model

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