Charge transport in complex halide perovskites from first principles calculations

ORAL

Abstract

Halide perovskites are attractive materials for solar energy conversion applications due to their strong light-matter interactions, structural tunability, and the relative ease with which they can be synthesized and processed. In metal halide perovskites, an important aspect in the energy conversion process is the underlying nature of the charge transport. Recent high-pressure measurements up to 50 GPa on a mixed-valent metal halide perovskite reveal a 12 order of magnitude increase in conductivity relative to ambient pressure and suggest that the charge transport is polaronic in nature. However a detailed picture of the underlying microscopic mechanism is still missing. Using first principles DFT calculations, we calculate the electronic structure and elucidate charge transport mechanisms, specifically focusing on the rich interplay between Jahn-Teller distortions, charge disproportionation, and polaronic hopping as a function of externally applied pressure. Our findings provide insight into the precise nature of the charge transport further guiding the design of next-generation halide perovskite-based photovoltaic devices.

*This work is supported by the Department of Energy; computational resources provided by NERSC.

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Presenters

  • Armin Eghdami

    • Department of Physics, University of California, Berkeley

Authors

  • Armin Eghdami

    • Department of Physics, University of California, Berkeley

  • Jonah B Haber

    • University of California, Berkeley
    • University of California, Berkeley; Lawrence Berkeley National Laboratory
    • Department of Physics, University of California, Berkeley
    • Department of Physics, University of California, Berkeley, CA 94720; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720.

  • Nathan R Wolf

    • Department of Chemistry, Stanford University, Stanford
    • Stanford University

  • Hemamala I Karunadasa

    • Department of Chemistry, Stanford University, Stanford; Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, Menlo Park
    • Stanford Univ
    • Stanford University

  • Jeffrey B Neaton

    • Lawrence Berkeley National Laboratory
    • University of California, Berkeley; Lawrence Berkeley National Laboratory; Kavli Energy NanoSciences Institute at Berkeley
    • Department of Physics, University of California, Berkeley; Materials Sciences Division, Lawrence Berkeley National Laboratory; Kavli Energy NanoScience Institute at Berkeley
    • Department of Physics, University of California, Berkeley, CA 94720; Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720; Kavli Energy Nano