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

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.
Authors:
;  [1]
  1. Faculty of Physics, Department of Theoretical Physics, Vilnius University, Saulėtekio 9, LT-10222 Vilnius (Lithuania)
Publication Date:
OSTI Identifier:
22255136
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 6; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 97 MATHEMATICAL METHODS AND COMPUTING; ENERGY TRANSFER; EQUATIONS; EXCITATION; MOLECULAR DYNAMICS METHOD; PROTEINS; SIMULATION; SPECTRAL DENSITY; STOCHASTIC PROCESSES