Exciton-phonon interactions in organic crystals from first principles many-body perturbation theory

ORAL

Abstract

Molecular crystals are attractive candidates for solar energy conversion applications due to their strong light-matter interactions, nearly endless structural tunability, and the relative inexpense with which they can be synthesized and processed. Acene crystals, such as tetracene and pentacene, possess both strong electron-hole and significant electron-phonon interactions, and a thorough understanding of the photophysics of these materials requires a careful analysis of the interplay between the ionic and excitonic degrees of freedom. In this talk, we present our linear response framework for computing exciton-phonon matrix elements, using ab initio density functional perturbation theory and many-body perturbation theory within the GW plus Bethe-Salpeter equation approach. We apply this method to compute exciton-phonon scattering rates for spin-singlet and spin-triplet excitons in prototypical acene crystals and compare with experimental linewidths. Finally, we discuss the implications of our calculations for exciton diffusion and multiexciton generation in these extended organic systems.

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

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Presenters

  • Jonah Haber

    • Physics, University of California Berkeley
    • Department of Physics, University of California, Berkeley
    • Physics, University of California, Berkeley

Authors

  • Jonah Haber

    • Physics, University of California Berkeley
    • Department of Physics, University of California, Berkeley
    • Physics, University of California, Berkeley

  • Sivan Refaely-Abramson

    • Department of Materials and Interfaces, Weizmann Institute of Science
    • Lawrence Berkeley National Laboratory
    • Materials and Interfaces, Weizmann Institute of Science, Israel
    • Weizmann Institute of Science, Lawrence Berkeley National Laboratory, University of California - Berkeley

  • Gabriel Antonius

    • Département de Chimie, Biochimie et Physique, Université du Québec à Trois-Rivières
    • Department of Physics, University of California at Berkeley and Materials Sciences Division, Lawrence Berkeley National Laboratory
    • University of California, Berkeley
    • Department of Physics, University of California at Berkeley, California 94720, USA, Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 9

  • Felipe Da Jornada

    • Department of Physics, University of California, Berkeley
    • Department of Physics, University of California at Berkeley and Materials Sciences Division, Lawrence Berkeley National Laboratory
    • Physics, University of California at Berkeley
    • Lawrence Berkeley National Laboratory
    • University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Physics, University of California, Berkeley
    • UC Berkeley and Lawrence Berkeley National Lab
    • Lawrence Berkeley National Lab
    • Lawrence Berkeley National Lab and University of California, Berkeley

  • Steven G. Louie

    • Physics, UC Berkeley
    • University of California, Berkeley
    • Department of Physics, University of California, Berkeley
    • Physics Department, UC Berkeley and Lawrence Berkeley National Lab
    • Department of Physics, University of California at Berkeley and Materials Sciences Division, Lawrence Berkeley National Laboratory
    • Physics, University of California at Berkeley
    • University of California at Berkeley and Lawrence Berkeley National Lab
    • University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Physics, University of California, Berkeley
    • UC Berkeley and Lawrence Berkeley National Lab
    • Physics, University of California - Berkeley
    • Physics and Materials Sciences, University of California at Berkeley and Lawrence Berkeley National Laboratory
    • Lawrence Berkeley National Lab and University of California, Berkeley
    • University of California - Berkeley, Lawrence Berkeley National Laboratory

  • Jeffrey B Neaton

    • Molecular Foundry, Lawrence Berkeley National Lab
    • University of California, Berkeley
    • Lawrence Berkeley National Laboratory
    • Molecular Foundry, Lawrence Berkeley National Laboratory
    • Department of Physics, University of California, Berkeley
    • UC Berkeley/Lawrence Berkeley Natl Lab
    • Lawrence Berkeley National Lab, Berkeley, CA
    • Physics, University of California, Berkeley
    • Molecular Foundry, LBNL; UC Berkeley; Kavli ENSI
    • Lawrence Berkeley National Laboratory, University of California - Berkeley, Kavli Energy NanoSciences Institute at Berkeley