Exciton dissociation at donor-acceptor polymer heterojunctions: Quantum nonadiabatic dynamics and effective-mode analysis

Hiroyuki Tamura, Eric R. Bittner, Irene Burghardt

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    56 Citations (Scopus)

    Abstract

    The quantum-dynamical mechanism of photoinduced subpicosecond exciton dissociation and the concomitant formation of a charge-separated state at a semiconducting polymer heterojunction is elucidated. The analysis is based upon a two-state vibronic coupling Hamiltonian including an explicit 24-mode representation of a phonon bath comprising high-frequency (CC stretch) and low-frequency (torsional) modes. The initial relaxation behavior is characterized by coherent oscillations, along with the decay through an extended nonadiabatic coupling region. This region is located in the vicinity of a conical intersection hypersurface. A central ingredient of the analysis is a novel effective mode representation, which highlights the role of the low-frequency modes in the nonadiabatic dynamics. Quantum dynamical simulations were carried out using the multiconfiguration time-dependent Hartree method.

    Original languageEnglish
    Article number021103
    JournalJournal of Chemical Physics
    Volume126
    Issue number2
    DOIs
    Publication statusPublished - 2007

    ASJC Scopus subject areas

    • Physics and Astronomy(all)
    • Physical and Theoretical Chemistry

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