Published August 17, 2014 | Version v1
Journal article

Dynamic coherence in excitonic molecular complexes under various excitation conditions

Description

Highlights: • Dynamic coherence does not improve energy transfer efficiency in natural conditions. • Photo-induced quantum jumps are discussed in classical context. • Natural time scale of a light excitation event is identified. • Coherence in FMO complex averages out under excitation by neighboring antenna. • This result is valid even in absence of dissipation. - Abstract: We investigate the relevance of dynamic quantum coherence in the energy transfer efficiency of molecular aggregates. We derive the time evolution of the density matrix for an open quantum system excited by light or by a neighboring antenna. Unlike in the classical case, the quantum description does not allow for a formal decomposition of the dynamics into sudden jumps in an observable quantity – an expectation value. Rather, there is a natural finite time-scale associated with the excitation process. We propose a simple experiment to test the influence of this time scale on the yield of photosynthesis. We demonstrate, using typical parameters of the Fenna–Matthews–Olson (FMO) complex and a typical energy transfer rate from the chlorosome baseplate, that dynamic coherences are averaged out in the complex even when the FMO model is completely free of all dissipation and dephasing

Availability note (English)

Available from http://dx.doi.org/10.1016/j.chemphys.2014.05.008

Additional details

Identifiers

DOI
10.1016/j.chemphys.2014.05.008;
arXiv
arXiv:1306.1693v2;
PII
S0301-0104(14)00138-4;

Publishing Information

Journal Title
Chemical Physics
Journal Volume
439
Journal Page Range
p. 100-110
ISSN
0301-0104
CODEN
CMPHC2

INIS

Country of Publication
Netherlands
Country of Input or Organization
International Atomic Energy Agency (IAEA)
INIS RN
46124963
Subject category
S74: ATOMIC AND MOLECULAR PHYSICS;
Descriptors DEI
DECOMPOSITION; DENSITY MATRIX; ENERGY TRANSFER; EXCITATION; EXPECTATION VALUE; PHOTOSYNTHESIS; QUANTUM SYSTEMS; VISIBLE RADIATION
Descriptors DEC
CHEMICAL REACTIONS; ELECTROMAGNETIC RADIATION; ENERGY-LEVEL TRANSITIONS; MATRICES; PHOTOCHEMICAL REACTIONS; RADIATIONS; SYNTHESIS

Optional Information

Copyright
Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.