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Transfer of excitation energy in a three-dimensional-doped molecular crystal .5. Self-consistency of the temporal processes involved in energy transfer in photosynthetic units

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Title Transfer of excitation energy in a three-dimensional-doped molecular crystal .5. Self-consistency of the temporal processes involved in energy transfer in photosynthetic units
 
Creator DATTA, SN
TANDON, D
MALLIK, B
 
Subject incoherent exciton motion
coupled coherent
transport
model
chlorophyll
absorption
migration
kinetics
 
Description Numerical experiments were carried out to determine the timewise self-consistency of different physical processes involved in the energy transfer in green plant photosynthetic units. A 6 x 6 x 6 array of chlorophyll-a with cubic lattice constants a = b = c = 20 Angstrom was chosen as a model of the thylakoid disc. Another model aggregate was obtained by substituting chlorophyll-b molecules for some of the chlorophyll-a molecules. In both models, a reaction center occupied a central site in the last xy plane. Two extreme arrangements were considered for the orientation of molecules. In one, the transition moments of all molecules were directed along the y-axis. The other had chlorophyll molecules randomly oriented. The four resulting model systems were used in our investigation on exciton generation, transport, decay by fluorescence, and trapping. All excitons were assumed to be generated by a 20 ms exposure to sunlight at high altitudes. The general trends noticed from these computations are as follows: The number of excitons generated is influenced by lattice disorders. Disorders also increase the time for the establishment of an equilibrium distribution The decay of excitons by fluorescence is always a monotonic function of time. The energy transfer is adversely affected by a lower degree of orientation in the crystal: The trapping time increases with disorder. The number of trappings decreases with the onset of fluorescence of the host molecules and the trap. From these investigations, we also made three specific observations: (1) The efficiency of exciton utilization varies from 12% for a completely random arrangement of transition dipoles to 46% for a perfectly ordered arrangement. This agrees with the experimental efficiency, about 20%. (2) The number of excitons trapped varies from one to six. This tallies with the time scale of electron transfer along the Z-scheme that requires at least two excitons trapped in about 20 ms. Thus, the photon density and the exciton transfer rate are consistent with the rates of electron transfers. (3) The trapping rate also indicates that the thylakoid disc must resemble a considerably ordered system. (C) 1996 , Inc.
 
Publisher JOHN WILEY & SONS INC
 
Date 2011-08-16T16:44:27Z
2011-12-26T12:55:02Z
2011-12-27T05:43:35Z
2011-08-16T16:44:27Z
2011-12-26T12:55:02Z
2011-12-27T05:43:35Z
1996
 
Type Article
 
Identifier INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, 60(5), 1045-1055
0020-7608
http://dx.doi.org/10.1002/(SICI)1097-461X(1996)60:5<1045::AID-QUA11>3.0.CO;2-6
http://dspace.library.iitb.ac.in/xmlui/handle/10054/9558
http://hdl.handle.net/10054/9558
 
Language en