Effects of molecular packing in organic crystals on singlet fission with ab initio many body perturbation theory

ORAL

Abstract

Multi-exciton generation processes, in which multiple charge carriers are generated from a single photon, are mechanisms of significant interest for achieving efficiencies beyond the Shockley-Queisser limit of conventional p-n junction solar cells. One well-studied multiexciton process is singlet fission, whereby a singlet decays into two spin-correlated triplet excitons. Here, we use a newly developed computational approach to calculate singlet-fission coupling terms and rates with an ab initio Green’s function formalism based on many-body perturbation theory (MBPT) within the GW approximation and the Bethe-Salpeter equation approach. We compare results for crystalline pentacene and TIPS-pentacene and explore the effect of molecular packing on the singlet fission mechanism.

*This work is supported by the Department of Energy.

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Authors

  • Jonah Haber

    • Dept. of Physics, University of California Berkeley, CA, USA

  • Sivan Refaely-Abramson

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

  • Felipe H. da Jornada

    • 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

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