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Exciton states and relaxation in molecular aggregates : Numerical study of photosynthetic light harvesting

Pullerits, Tõnu LU (2000) In Journal of the Chinese Chemical Society 47(4A). p.773-784
Abstract

In this article we briefly review the molecular exciton theory and apply it to photosynthetic light harvesting systems. We derive expressions for exciton relaxation rates using perturbation theory in Hibert space representation and show how the Förster equation can be obtained from a general relaxation rate expression in case of well localized excitons. A detailed analysis of the exciton level structure and wavefunctions of the ring structure is presented for diagonal and nondiagonal disorder. We conclude that the latter plays only a minor role in light-harvesting systems. We emphasize the relaxation rate dependency on square of the energy gap, which makes the high frequency modes particularly important for the exciton relaxation. We... (More)

In this article we briefly review the molecular exciton theory and apply it to photosynthetic light harvesting systems. We derive expressions for exciton relaxation rates using perturbation theory in Hibert space representation and show how the Förster equation can be obtained from a general relaxation rate expression in case of well localized excitons. A detailed analysis of the exciton level structure and wavefunctions of the ring structure is presented for diagonal and nondiagonal disorder. We conclude that the latter plays only a minor role in light-harvesting systems. We emphasize the relaxation rate dependency on square of the energy gap, which makes the high frequency modes particularly important for the exciton relaxation. We found a reasonably good agreement between the measured and calculated relaxation rates in photosynthetic purple bacteria.

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Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
Coherence, Excitons, LH2, Photosynthesis
in
Journal of the Chinese Chemical Society
volume
47
issue
4A
pages
12 pages
publisher
Chinese Chemical Society
external identifiers
  • scopus:0001659493
ISSN
0009-4536
DOI
10.1002/jccs.200000106
language
English
LU publication?
yes
id
35874534-955e-4594-a997-b5280b752335
date added to LUP
2025-10-28 17:09:44
date last changed
2025-10-31 10:04:51
@article{35874534-955e-4594-a997-b5280b752335,
  abstract     = {{<p>In this article we briefly review the molecular exciton theory and apply it to photosynthetic light harvesting systems. We derive expressions for exciton relaxation rates using perturbation theory in Hibert space representation and show how the Förster equation can be obtained from a general relaxation rate expression in case of well localized excitons. A detailed analysis of the exciton level structure and wavefunctions of the ring structure is presented for diagonal and nondiagonal disorder. We conclude that the latter plays only a minor role in light-harvesting systems. We emphasize the relaxation rate dependency on square of the energy gap, which makes the high frequency modes particularly important for the exciton relaxation. We found a reasonably good agreement between the measured and calculated relaxation rates in photosynthetic purple bacteria.</p>}},
  author       = {{Pullerits, Tõnu}},
  issn         = {{0009-4536}},
  keywords     = {{Coherence; Excitons; LH2; Photosynthesis}},
  language     = {{eng}},
  number       = {{4A}},
  pages        = {{773--784}},
  publisher    = {{Chinese Chemical Society}},
  series       = {{Journal of the Chinese Chemical Society}},
  title        = {{Exciton states and relaxation in molecular aggregates : Numerical study of photosynthetic light harvesting}},
  url          = {{http://dx.doi.org/10.1002/jccs.200000106}},
  doi          = {{10.1002/jccs.200000106}},
  volume       = {{47}},
  year         = {{2000}},
}