The Impact of Lattice and Charge Fluctuations on Carrier Dynamics in Halide Perovskites

ORAL

Abstract

While halide perovskites (HaPs) have shown great technological promise for use as materials in energy devices, several of their unique optoelectronic properties remain incompletely understood. We develop a microscopic theory that is aimed at describing pertinent physical effects related to the carrier transport and optical properties of HaPs. It captures the nuclear displacements to all orders and goes beyond assuming linear electron-phonon coupling in calculating the dynamics of carriers and band gap characteristics. We combine the theory with first-principles calculations and apply it to the paradigm HaP compound MAPbI3. Our results explain intriguing experimental findings related to the charge-carrier mobility and optical properties, including their temperature dependencies. The findings of our work demonstrate that orbital overlap fluctuations in the lead-halide structure play a leading role in determining the optoelectronic features of HaPs.

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Presenters

  • David Egger

    Institute of Theoretical Physics, University of Regensburg, University of Regensburg

Authors

  • Matthew Z. Mayers

    Department of Chemistry, Columbia University

  • Liang Tan

    Department of Chemistry, University of Pennsylvania, Lawrence Berkeley National Laboratory, Molecular Foundry, Lawrence Berkeley National Laboratory, Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley

  • David Egger

    Institute of Theoretical Physics, University of Regensburg, University of Regensburg

  • Andrew Rappe

    University of Pennsylvania, Department of Chemistry, University of Pennsylvania, Chemistry, University of Pennsylvania

  • David Reichman

    Department of Chemistry, Columbia University, Columbia University