Quantum dynamics of ultrafast charge transfer at an oligothiophene- fullerene heterojunction

Hiroyuki Tamura, Rocco Martinazzo, Matthias Ruckenbauer, Irene Burghardt

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    66 Citations (Scopus)

    Abstract

    Following up on our recent study of ultrafast charge separation at oligothiophene-fullerene interfaces [H. Tamura, I. Burghardt, and M. Tsukada, J. Phys. Chem. C 115, 10205 (2011)10.1021/jp203174e], we present here a detailed quantum dynamical perspective on the charge transfer process. To this end, electron-phonon coupling is included non-perturbatively, by an explicit quantum dynamical treatment using the multi-configuration time-dependent Hartree (MCTDH) method. Based upon a distribution of electron-phonon couplings determined from electronic structure studies, a spectral density is constructed and employed to parametrize a linear vibronic coupling Hamiltonian. The diabatic coupling is found to depend noticeably on the inter-fragment distance, whose effect on the dynamics is here investigated. MCTDH calculations of the nonadiabatic transfer dynamics are carried out for the two most relevant electronic states and 60 phonon modes. The electron transfer process is found to be ultrafast and mediated by electronic coherence, resulting in characteristic oscillatory features during a period of about 100 fs.

    Original languageEnglish
    Article number22A540
    JournalJournal of Chemical Physics
    Volume137
    Issue number22
    DOIs
    Publication statusPublished - 2012 Dec 14

    ASJC Scopus subject areas

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

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