Theory of femtosecond coherent double-pump single-molecule spectroscopy: Application to light harvesting complexes

Lipeng Chen, Maxim F. Gelin, Wolfgang Domcke, Yang Zhao

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25 Scopus citations

Abstract

We develop a first principles theoretical description of femtosecond double-pump single-molecule signals of molecular aggregates. We incorporate all singly excited electronic states and vibrational modes with significant exciton-phonon coupling into a system Hamiltonian and treat the ensuing system dynamics within the Davydov D1 Ansatz. The remaining intra- and inter-molecular vibrational modes are treated as a heat bath and their effect is accounted for through lineshape functions. We apply our theory to simulate single-molecule signals of the light harvesting complex II. The calculated signals exhibit pronounced oscillations of mixed electron-vibrational (vibronic) origin. Their periods decrease with decreasing exciton-phonon coupling.

Original languageEnglish
Article number164106
JournalJournal of Chemical Physics
Volume142
Issue number16
DOIs
StatePublished - 28 Apr 2015

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