Understanding excited-states of light-harvesting chromophores with ab initio many-body perturbation theory

ORAL

Abstract

Biomimetic light-harvesting systems provide a rich platform for distilling the photophysics underlying natural photosynthetic energy transfer processes. Deducing the mechanisms underpinning these dynamics requires an accurate characterization of the excited states of a chromophore molecule coupled to a dynamic and heterogeneous environment that can lead to complex non-radiative decay pathways. Here, we use time-dependent density functional theory (TDDFT) and ab initio many-body perturbation theory with the GW plus Bethe-Salpeter equation (GW-BSE) approach to predict the excited states and intermolecular coupling of chromophores. We have previously shown GW-BSE is capable of improving on TDDFT for simpler systems that feature differential electron correlation between ground and excited states. Additionally, we identify factors that give rise to the time scales observed in transient absorption experiments and those that yield the desired photodynamics and resulting energy transfer properties.

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Presenters

  • Samia Hamed

    Univ of California - Berkeley

Authors

  • Samia Hamed

    Univ of California - Berkeley

  • Milan Delor

    Univ of California - Berkeley

  • Fabien Bruneval

    Service de Recherches de Métallurgie Physique, CEA, DEN, Université Paris-Saclay

  • Naomi Ginsberg

    Univ of California - Berkeley

  • Jeffrey Neaton

    Molecular Foundry, Lawrence Berkeley National Laboratory; Department of Physics, University of California, Berkeley; Kavli Energy Nanosciences Institute at Berkeley, Physics, University of California, Berkeley; Lawrence Berkeley National Laboratory, Department of Physics, University of California, Univ of California - Berkeley, Lawrence Berkeley Natl Lab, Materials Science Division, Lawrence Berkeley National Laboratory, Molecular Foundry, Lawrence Berkeley National Lab, Physics, University of California, Berkeley, Department of Physics UCB; Molecular Foundry LBNL; Kavli ENSI, Lawrence Berkeley National Laboratory, Department of Physics, Univ of California - Berkeley, Lawrence Berkeley National Lab and University of California - Berkeley