Solid-state optical absorption from optimally tuned time-dependent range-separated hybrid density functional theory

ORAL

Abstract

We present a framework for obtaining solid-state charge and optical excitations and spectra from optimally tuned range-separated hybrid density functional theory, which allows for the accurate prediction of exciton binding energies. We demonstrate our approach through calculations of one- and two-particle excitations in pentacene, a molecular semiconducting crystal, where we find excellent agreement with experiments and prior computations. We show that with one adjustable parameter, our method accurately predicts band structures and optical spectra of Si and LiF, prototypical covalent and ionic solids. For a range of extended bulk systems, this method may provide a computationally inexpensive alternative to many-body perturbation theory, opening the door to studies of materials of increasing size and complexity [Phys. Rev. B 92, 081204(R), 2015].

*This work was supported by DOE

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Authors

  • Sivan Refaely-Abramson

    • Molecular Foundry, LBNL and Dept. of Physics, UC-Berkeley

  • Manish Jain

    • Dept. of Physics, IISc, Bangalore, India

  • Sahar Sharifzadeh

    • Department of Electrical and Computer Engineering, Boston University
    • Dept. of Electrical and Computer Engineering and Physics Division of MSE, Boston University
    • Boston University

  • 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

  • Leeor Kronik

    • Dept. of Materials and Interfaces, Weizmann Institute