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Title: Unified treatment of coherent and incoherent electronic energy transfer dynamics using classical electrodynamics

Journal Article · · J. Chem. Phys.
DOI:https://doi.org/10.1063/1.3488136· OSTI ID:1066071
 [1];  [1]
  1. MIT (Massachusetts Inst. of Technology), Cambridge, MA (United States). Dept. of Chemistry

Recent experiments on resonance energy transfer (RET) in photosynthetic systems have found evidence of quantum coherence between the donor and the acceptor. Under these conditions, Foerster’s theory of RET is no longer applicable and no theory of coherent RET advanced to date rivals the intuitive simplicity of Foerster’s theory. Here, we develop a framework for understanding RET that is based on classical electrodynamics but still captures the essence of the quantum coherence between the molecules. Our theory requires only a knowledge of the complex polarizabilities of the two molecules participating in the transfer as well as the distance between them. We compare our results to quantum mechanical calculations and show that the results agree quantitatively.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
DOE Contract Number:
SC0001088
OSTI ID:
1066071
Journal Information:
J. Chem. Phys., Vol. 133, Issue 14; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; ISSN 0021-9606: JCPSA6
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English