Photo-induced Charge Separation in Nanoscale Donor-Bridge-Acceptor Systems: Theory and Experiment

ORAL

Abstract

Understanding and control of light-harvesting processes at the molecular-scale remains a fundamental challenge in solar energy conversion. Donor-bridge-acceptor molecules (DBAM), with atomically-defined interfaces made by a covalently bound bridge between donor and acceptor moieties, allow probing of excited states relevant to optical absorption and charge separation. In close collaboration with experiment, we use first-principles many-body perturbation theory, within the GW approximation and the Bethe-Salpeter equation approach, to compute excited states for six DBAMs. We compare with experiments, and quantitative agreement is obtained. Implications of our results for nanoscale light-harvesting are thoroughly discussed. Support: DOE via the Molecular Foundry and Helios SERC, and NSF via NCN. Computational support provided by NERSC.

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Authors

  • Peter Doak

    • Molecular Foundry, LBNL; Department of Chemistry, UC-Berkeley

  • Pierre Darancet

    • Molecular Foundry, LBNL

  • Kasper Moth-Poulsen

    • Department of Chemical and Biological Engineering, Chalmers U. of Technology

  • Jesse Jenkins

    • Department of Chemistry, UC-Berkeley

  • Rachel Segalman

    • UC Berkeley
    • Department of Chemical Engineering, UC-Berkeley
    • University of California, Berkeley
    • Department of Chemical Engineering, University of California , Berkeley
    • University of California Berkeley
    • University of California - Berkeley

  • Don Tilley

    • Department of Chemistry, UC-Berkeley

  • Jeffrey B. Neaton

    • Molecular Foundry, LBNL
    • Molecular Foundry, Lawrence Berkeley National Laboratory