Exciton coupling induces vibronic hyperchromism in light-harvesting complexes

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Abstract

The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model that includes ground-state vibrations is investigated using the multi-configuration time-dependent Hartree method with a parameter set typical to photosynthetic light-harvesting complexes. The absorption spectra are discussed based on the Coulomb coupling, the detuning of the site energies, and the number of vibrational modes. Fluorescence spectra calculations show that the spectral densities obtained from the low-temperature fluorescence line-narrowing measurements of light-harvesting systems need to be corrected for the effects of excitons. For the J-aggregate configuration, as in most light-harvesting complexes, the true spectral density has a larger amplitude than that obtained from the measurement.

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Research areas and keywords

Subject classification (UKÄ) – MANDATORY

  • Atom and Molecular Physics and Optics

Keywords

  • coherence, electronic 2D spectroscopy, excitons, vibronic coupling, Huang-Rhys factor, fluorescence line narrowing
Original languageEnglish
Article number045010
JournalNew Journal of Physics
Volume16
Publication statusPublished - 2014
Publication categoryResearch
Peer-reviewedYes

Bibliographic note

The information about affiliations in this record was updated in December 2015. The record was previously connected to the following departments: Chemical Physics (S) (011001060)