Optical Signatures of Quantum Delocalization over Extended Domains in Photosynthetic Membranes

J Phys Chem A. 2015 Aug 27;119(34):9043-50. doi: 10.1021/acs.jpca.5b04804. Epub 2015 Aug 14.

Abstract

The prospect of coherent dynamics and excitonic delocalization across several light-harvesting structures in photosynthetic membranes is of considerable interest, but challenging to explore experimentally. Here we demonstrate theoretically that the excitonic delocalization across extended domains involving several light-harvesting complexes can lead to unambiguous signatures in the optical response, specifically, linear absorption spectra. We characterize, under experimentally established conditions of molecular assembly and protein-induced inhomogeneities, the optical absorption in these arrays from polarized and unpolarized excitation, and demonstrate that it can be used as a diagnostic tool to determine the resonance coupling between iso-energetic light-harvesting structures. The knowledge of these couplings would then provide further insight into the dynamical properties of transfer, such as facilitating the accurate determination of Förster rates.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Cell Membrane / chemistry
  • Cell Membrane / metabolism*
  • Models, Molecular
  • Molecular Conformation
  • Optical Phenomena*
  • Photosynthesis*
  • Quantum Theory*