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Exciton coupling induces vibronic hyperchromism in light-harvesting complexes.

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Title: Exciton coupling induces vibronic hyperchromism in light-harvesting complexes.
Authors: Schulze, Jan1, Torbj�rnsson, Magne2, K�hn, Oliver1 oliver.kuehn@uni-rostock.de, Pullerits, T�nu2 tonu.pullerits@chemphys.lu.se
Source: New Journal of Physics. Apr2014, Vol. 16 Issue 4, p045010-045022. 13p.
Subjects: Hyperchromic effect, Multi-configurational self-consistent field method, Fluorescence spectroscopy, Exciton theory, Spectral energy distribution, Vibronic coupling
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. [ABSTRACT FROM AUTHOR]
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Database: Engineering Source
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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. [ABSTRACT FROM AUTHOR]
ISSN:13672630
DOI:10.1088/1367-2630/16/4/045010