Singlet-Fission from First-Principles Many-Body Perturbation Theory

ORAL

Abstract

We present an ab initio approach to investigate the interaction between single excitons and non-interacting biexcitons from first-principles using many-body perturbation theory within the GW approximation and the Bethe-Salpeter Equation approach. We apply our model to explore singlet-fission in acene molecular crystals. For these systems, we calculate the electronic coupling between singlet excitations and non-interacting but spin-correlated triplet pairs, explore the resulting singlet-fission rate, and associate the exciton-exciton coupling mechanism in terms of the crystal structure and given the nature and symmetry of the involved solid-state excitons.

*This work is supported by the Department of Energy.

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Authors

  • Sivan Refaely-Abramson

    • University of California
    • Molecular Foundry, Lawrence Berkeley National Lab; Dept. of Physics, University of California Berkeley, CA, USA

  • Felipe H. da Jornada

    • UC Berkeley and Lawrence Berkeley National Lab
    • University of California at Berkeley and Lawrence Berkeley National Lab
    • Dept. of Physics, University of California Berkeley; Materials Sciences Division, Lawrence Berkeley National Lab, CA, USA

  • Steven G. Louie

    • Dept. of Physics, University of California Berkeley; Materials Sciences Division, Lawrence Berkeley National Lab, CA, USA

  • Jeffrey B. Neaton

    • Department of Physics, UC Berkeley; Molecular Foundry, LBNL
    • Department of Physics, UC Berkeley & Molecular Foundry, LBNL
    • Department of Physics, UC Berkeley; Molecular Foundry, LBNL; Kavli Energy NanoScience Institute
    • Department of Physics, University of California, Berkeley
    • Lawrence Berkeley National Laboratory
    • Molecular Foundry, LBNL; Dept. of Physics, UC Berkeley; Kavli ENSI
    • LBNL
    • Univ of California - Berkeley, Lawrence Berkeley National Lab
    • Physics, UC Berkeley, and Molecular Foundry, LBNL
    • University of California
    • Molecular Foundry, Lawrence Berkeley National Lab; Dept. of Physics, University of California Berkeley; Kavli NanoScience Institute, Berkeley, CA, USA
    • Department of Physics, UC Berkeley; Molecular Foundry, LBNL; Kavli Energy NanoSciences Institute at Berkeley
    • Physics Department, UC Berkeley; Molecular Foundry, Lawrence Berkeley National Lab; Kavli Energy NanoSciences Institute at Berkeley