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

Authors
Citation
T. Pullerits, Exciton states and relaxation in molecular aggregates: Numerical study of photosynthetic light harvesting, J CHIN CHEM, 47(4A), 2000, pp. 773-784
Citations number
56
Categorie Soggetti
Chemistry
Journal title
JOURNAL OF THE CHINESE CHEMICAL SOCIETY
ISSN journal
00094536 → ACNP
Volume
47
Issue
4A
Year of publication
2000
Pages
773 - 784
Database
ISI
SICI code
0009-4536(200008)47:4A<773:ESARIM>2.0.ZU;2-L
Abstract
In this article we briefly review the molecular exciton theory and apply it to photosynthetic light harvesting systems. We derive expressions for exci ton relaxation rates using perturbation theory in Hilbert space representat ion and show how the Forster equation can be obtained from a general relaxa tion rate expression in case of well localized excitons. A detailed analysi s of the exciton level structure and wavefunctions of the ring structure is presented for diagonal and nondiagonal disorder. We conclude that the latt er plays only a minor role in light-harvesting systems. We emphasize the re laxation 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.