Electronic energy transfer through non-adiabatic vibrational-electronic resonance. II. 1D spectra for a dimer

The Journal of Chemical Physics
Vivek Tiwari, David M Jonas

Abstract

Vibrational-electronic resonance in photosynthetic pigment-protein complexes invalidates Förster's adiabatic framework for interpreting spectra and energy transfer, thus complicating determination of how the surrounding protein affects pigment properties. This paper considers the combined effects of vibrational-electronic resonance and inhomogeneous variations in the electronic excitation energies of pigments at different sites on absorption, emission, circular dichroism, and hole-burning spectra for a non-degenerate homodimer. The non-degenerate homodimer has identical pigments in different sites that generate differences in electronic energies, with parameters loosely based on bacteriochlorophyll a pigments in the Fenna-Matthews-Olson antenna protein. To explain the intensity borrowing, the excited state vibrational-electronic eigenvectors are discussed in terms of the vibrational basis localized on the individual pigments, as well as the correlated/anti-correlated vibrational basis delocalized over both pigments. Compared to those in the isolated pigment, vibrational satellites for the correlated vibration have the same frequency and precisely a factor of 2 intensity reduction through vibrational delocalization in both absor...Continue Reading

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Citations

Jun 10, 2019·The Journal of Chemical Physics·Peter A Rose, Jacob J Krich
Dec 16, 2020·The Journal of Chemical Physics·Amitav SahuVivek Tiwari
Jul 10, 2021·The Journal of Chemical Physics·James D GaynorMunira Khalil
Nov 16, 2019·The Journal of Physical Chemistry Letters·Jonathan D SchultzMichael R Wasielewski
Feb 13, 2020·The Journal of Physical Chemistry. a·Aliya MukazhanovaSahar Sharifzadeh

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