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.

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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