Two-dimensional electronic spectroscopy of the B800-B820 light-harvesting complex

Zigmantas, D., Read, E. L., Mancal, T., Brixner, T., Gardiner, A. T., Cogdell, R. J. and Fleming, G. R. (2006) Two-dimensional electronic spectroscopy of the B800-B820 light-harvesting complex. Proceedings of the National Academy of Sciences of the United States of America, 103, pp. 12672-12677. (doi:10.1073/pnas.0602961103)

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Abstract

Emerging nonlinear optical spectroscopies enable deeper insight into the intricate world of interactions and dynamics of complex molecular systems. 2D electronic spectroscopy appears to be especially well suited for studying multichromophoric complexes such as light-harvesting complexes of photosynthetic organisms as it allows direct observation of couplings between the pigments and charts dynamics of energy flow on a 2D frequency map. Here, we demonstrate that a single 2D experiment combined with self-consistent theoretical modeling can determine spectroscopic parameters dictating excitation energy dynamics in the bacterial B800–B820 light-harvesting complex, which contains 27 bacteriochlorophyll molecules. Ultrafast sub-50-fs dynamics dominated by coherent intraband processes and population transfer dynamics on a picosecond time scale were measured and modeled with one consistent set of parameters. Theoretical 2D spectra were calculated by using a Frenkel exciton model and modified Förster/Redfield theory for the calculation of dynamics. They match the main features of experimental spectra at all population times well, implying that the energy level structure and transition dipole strengths are modeled correctly in addition to the energy transfer dynamics of the system.

Item Type:Articles
Status:Published
Refereed:Yes
Glasgow Author(s) Enlighten ID:Cogdell, Professor Richard and Gardiner, Dr Alastair
Authors: Zigmantas, D., Read, E. L., Mancal, T., Brixner, T., Gardiner, A. T., Cogdell, R. J., and Fleming, G. R.
College/School:College of Medical Veterinary and Life Sciences > Institute of Molecular Cell and Systems Biology
Journal Name:Proceedings of the National Academy of Sciences of the United States of America
ISSN:0027-8424
ISSN (Online):1091-6490

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
303032The structure and function of purple bacterial antenna complexesRichard CogdellBiotechnology and Biological Sciences Research Council (BBSRC)BB/D000610/1Institute of Molecular Cell and Systems Biology