Ab initio study of the polarization dependence of the optoelectronic properties of hybrid halide perovskites

ORAL

Abstract

With efficiencies as high as 20\%, hybrid organic-inorganic halide perovskites have garnered much of the photovoltaic community's attention. In light of recent experimental results [1], we investigate the coupling mechanism between polarization and optoelectronic properties of methylammonium (MA) lead iodide, (CH$_3$NH$_3$)PbI$_3$, and related halide perovskites. In particular, we study the conditions that promote a combined effect of strong spin-orbit coupling and inversion symmetry breaking and that lead to a sizable Rashba/Dresselhaus effect. Using density functional theory calculations, we elucidate the emergence of Rashba/Dresselhaus splitting associated with local distortions and long-range coherent alignment of MA moieties in the material. We examine the extent to which the magnitude of the splitting, as well as other important electronic and optical properties [1], can be altered by increasing the macroscopic polarization. This opens avenues for manipulation of optoelectronic properties by an external electric field and/or chemical substitution of the MA molecule. \newline [1] S.Y. Leblebici, L. Leppert, et al, Facet-dependent photovoltaic efficiency variations in single perovskite grains, submitted (2015).

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Authors

  • Linn Leppert

    • Molecular Foundry, Lawrence Berkeley National Lab; Department of Physics, University of California Berkeley

  • Sebastian Reyes-Lillo

    • Molecular Foundry, Lawrence Berkeley National Lab; Department of Physics, University of California Berkeley
    • Physics Department, UC Berkeley; Molecular Foundry, Lawrence Berkeley National Lab

  • Jeffrey Neaton

    • University of California, Berkeley; Lawrence Berkeley National Laboratory
    • Lawrence Berkeley Natl Lab/UC Berkeley
    • Physics Department, UC Berkeley, The Molecular Foundry, LBNL \& Kavli Energy NanoSciences Institute at Berkeley, Berkeley, CA
    • Molecular Foundry, Lawrence Berkeley National Lab; Department of Physics, University of California Berkeley; Kavli Energy NanoSciences Insitute
    • Molecular Foundry, LBNL; Dept. of Physics, UC Berkeley; Kavli ENSI
    • UC Berkeley; Molecular Foundry, LBNL; Kavli Energy Nanosciences Institute at Berkeley
    • Dept. of Physics, UC Berkeley \& Lawrence Berkeley National Lab (USA)
    • Molecular Foundry, LBNL, Dept. of Physics, UC-Berkeley and Kavli ESNI at Berkeley
    • Molecular Foundry, Lawrence Berkeley National Laboratory
    • Physics Department, UC Berkeley; Molecular Foundry, Lawrence Berkeley National Lab; Kavli Energy NanoSciences Institute at Berkeley