Coherent versus incoherent energy transfer and trapping in photosynthetic antenna complexes

被引:171
作者
Leegwater, JA
机构
[1] Department of Physics and Astronomy, Vrije Universiteit Amsterdam, 1081 HV-NL Amsterdam
关键词
D O I
10.1021/jp961448i
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
In this paper we present a study of a model in which there is energy transfer as well as a special site where an irreversible reaction takes place. This model has an arbitrary ratio of homogeneous broadening versus site interaction energy. This allows us to study the crossover from hopping dynamics to exciton dynamics. We show that for the survival time the hopping (Forster) approximation gives a surprisingly accurate final result even when the energy transfer is excitonic. Fluorescence depolarization however is a sensitive probe for the nature of the energy transfer. We study the number of coherent molecules by considering a generalization of the inverse participation ratio. For LH1, assuming that it is a ring of 16 dimers, we estimate that the excitation is, on the average, delocalized over two dimers. The excitation is localized by phonons.
引用
收藏
页码:14403 / 14409
页数:7
相关论文
共 18 条
[1]   EXCITATION TRANSFER IN THE CORE LIGHT-HARVESTING COMPLEX (LH-1) OF RHODOBACTER-SPHAEROIDES - AN ULTRAFAST FLUORESCENCE DEPOLARIZATION AND ANNIHILATION STUDY [J].
BRADFORTH, SE ;
JIMENEZ, R ;
VANMOURIK, F ;
VANGRONDELLE, R ;
FLEMING, GR .
JOURNAL OF PHYSICAL CHEMISTRY, 1995, 99 (43) :16179-16191
[2]   A MULTIMER MODEL FOR P680, THE PRIMARY ELECTRON-DONOR OF PHOTOSYSTEM-II [J].
DURRANT, JR ;
KLUG, DR ;
KWA, SLS ;
VANGRONDELLE, R ;
PORTER, G ;
DEKKER, JP .
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 1995, 92 (11) :4798-4802
[3]  
Economou E. N., 1979, GREENS FUNCTIONS QUA
[4]   OPTICAL-PROPERTIES OF DISORDERED MOLECULAR AGGREGATES - A NUMERICAL STUDY [J].
FIDDER, H ;
KNOESTER, J ;
WIERSMA, DA .
JOURNAL OF CHEMICAL PHYSICS, 1991, 95 (11) :7880-7890
[5]  
Forster T., 1965, Modern Quantum Chemistry, Ved, ppp 93
[6]   EXACTLY SOLVABLE MODEL FOR COHERENT AND INCOHERENT EXCITON MOTION [J].
HAKEN, H ;
STROBL, G .
ZEITSCHRIFT FUR PHYSIK, 1973, 262 (02) :135-148
[7]  
Kenkre V. M., 1982, EXCITON DYNAMICS MOL, DOI 10.1007/BFb0041435
[8]   CHROMOPHORE INTERACTIONS IN ALLOPHYCOCYANIN [J].
MACCOLL, R ;
CSATORDAY, K ;
BERNS, DS ;
TRAEGER, E .
BIOCHEMISTRY, 1980, 19 (12) :2817-2820
[9]   STRUCTURE OF A BACTERIOCHLOROPHYLL A-PROTEIN FROM THE GREEN PHOTOSYNTHETIC BACTERIUM PROSTHECOCHLORIS-AESTUARII [J].
MATTHEWS, BW ;
FENNA, RE ;
BOLOGNESI, MC ;
SCHMID, MF ;
OLSON, JM .
JOURNAL OF MOLECULAR BIOLOGY, 1979, 131 (02) :259-285
[10]   CRYSTAL-STRUCTURE OF AN INTEGRAL MEMBRANE LIGHT-HARVESTING COMPLEX FROM PHOTOSYNTHETIC BACTERIA [J].
MCDERMOTT, G ;
PRINCE, SM ;
FREER, AA ;
HAWTHORNTHWAITELAWLESS, AM ;
PAPIZ, MZ ;
COGDELL, RJ ;
ISAACS, NW .
NATURE, 1995, 374 (6522) :517-521