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

Zigmantas, Donatas LU ; Read, E. L.; Mancal, T.; Brixner, T.; Gardiner, A. T.; Cogdell, R. J. and Fleming, G. R. (2006) In Proceedings of the National Academy of Sciences 103(34). p.12672-12677
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... (More)
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 Forster/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. (Less)
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author
publishing date
type
Contribution to journal
publication status
published
subject
keywords
photosynthetic complexes, multichromophoric systems, ultrafast spectroscopy, photosynthetic purple bacteria, excitation-energy transfer, echo peak shift, femtosecond spectroscopy, room-temperature, transfer dynamics, lh2, antenna system, couplings, acidophila, excitons
in
Proceedings of the National Academy of Sciences
volume
103
issue
34
pages
12672 - 12677
publisher
National Acad Sciences
external identifiers
  • scopus:33748032078
ISSN
1091-6490
DOI
10.1073/pnas.0602961103
language
English
LU publication?
no
id
77503070-528d-462e-bf7d-51f5c18f5ba3 (old id 1433120)
date added to LUP
2009-07-02 14:48:32
date last changed
2018-12-02 04:25:04
@article{77503070-528d-462e-bf7d-51f5c18f5ba3,
  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 Forster/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.},
  author       = {Zigmantas, Donatas and Read, E. L. and Mancal, T. and Brixner, T. and Gardiner, A. T. and Cogdell, R. J. and Fleming, G. R.},
  issn         = {1091-6490},
  keyword      = {photosynthetic complexes,multichromophoric systems,ultrafast spectroscopy,photosynthetic purple bacteria,excitation-energy transfer,echo peak shift,femtosecond spectroscopy,room-temperature,transfer dynamics,lh2,antenna system,couplings,acidophila,excitons},
  language     = {eng},
  number       = {34},
  pages        = {12672--12677},
  publisher    = {National Acad Sciences},
  series       = {Proceedings of the National Academy of Sciences},
  title        = {Two-dimensional electronic spectroscopy of the B800-B820 light-harvesting complex},
  url          = {http://dx.doi.org/10.1073/pnas.0602961103},
  volume       = {103},
  year         = {2006},
}