Excitation transfer pathways in excitonic aggregates revealed by the stochastic Schrödinger equation

J Chem Phys. 2014 Feb 14;140(6):065103. doi: 10.1063/1.4863968.

Abstract

We derive the stochastic Schrödinger equation for the system wave vector and use it to describe the excitation energy transfer dynamics in molecular aggregates. We suggest a quantum-measurement based method of estimating the excitation transfer time. Adequacy of the proposed approach is demonstrated by performing calculations on a model system. The theory is then applied to study the excitation transfer dynamics in a photosynthetic pigment-protein Fenna-Matthews-Olson (FMO) aggregate using both the Debye spectral density and the spectral density obtained from earlier molecular dynamics simulations containing strong vibrational high-frequency modes. The obtained results show that the excitation transfer times in the FMO system are affected by the presence of the vibrational modes; however, the transfer pathways remain the same.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Bacterial Proteins / chemistry*
  • Chlorobi / chemistry*
  • Energy Transfer
  • Light-Harvesting Protein Complexes / chemistry*
  • Models, Molecular
  • Quantum Theory
  • Stochastic Processes

Substances

  • Bacterial Proteins
  • FMO bacteriochlorophyll protein, Bacteria
  • Light-Harvesting Protein Complexes