Calculating polaron mobility in halide perovskites

Jarvist Moore Frost

Research output: Contribution to journalArticle

36 Citations (Scopus)

Abstract

Lead halide perovskite semiconductors are soft, polar materials. The strong driving force for polaron formation (the dielectric electron-phonon coupling) is balanced by the light band effective masses, leading to a strongly-interacting large polaron. A first-principles prediction of mobility would help understand the fundamental mobility limits. Theories of mobility need to consider the polaron (rather than free-carrier) state due to the strong interactions. In this material we expect that at room temperature polar-optical phonon mode scattering will dominate and so limit mobility. We calculate the temperature-dependent polaron mobility of hybrid halide perovskites by variationally solving the Feynman polaron model with the finite-temperature free energies of Ōsaka. This model considers a simplified effective-mass band structure interacting with a continuum dielectric of characteristic response frequency. We parametrize the model fully from electronic-structure calculations. In methylammonium lead iodide at 300K we predict electron and hole mobilities of 133 and 94cm2V-1s-1, respectively. These are in acceptable agreement with single-crystal measurements, suggesting that the intrinsic limit of the polaron charge carrier state has been reached. Repercussions for hot-electron photoexcited states are discussed. As well as mobility, the model also exposes the dynamic structure of the polaron. This can be used to interpret impedance measurements of the charge-carrier state. We provide the phonon-drag mass renormalization and scattering time constants. These could be used as parameters for larger-scale device models and band-structure dependent mobility simulations.

Original languageEnglish
Article number195202
JournalPhysical Review B
Volume96
Issue number19
DOIs
Publication statusPublished - 7 Nov 2017

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perovskites
halides
Charge carriers
Band structure
Scattering
Hole mobility
Hot electrons
Electron mobility
Model structures
charge carriers
Perovskite
Temperature
Electron energy levels
Free energy
Frequency response
Electronic structure
Drag
Lead
Single crystals

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics

Cite this

Calculating polaron mobility in halide perovskites. / Frost, Jarvist Moore.

In: Physical Review B, Vol. 96, No. 19, 195202, 07.11.2017.

Research output: Contribution to journalArticle

Frost, Jarvist Moore. / Calculating polaron mobility in halide perovskites. In: Physical Review B. 2017 ; Vol. 96, No. 19.
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