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On the Mechanism of Light Harvesting in Photosynthetic Purple Bacteria: B800 to B850 Energy Transfer
Abstract
The rate of energy transfer from B800 to B850 in the peripheral light harvesting complex LH2 is modeled in detail. A method for determining ensemble average energy transfer rates in complex, coupled multichromophoric systems is reported and is employed to investigate the interplay of electron−phonon coupling (fast fluctuations of the protein) and site energy disorder (slow fluctuations) on the spectral overlap between donor and acceptor, and therefore the energy transfer rate. A series of model calculations for Rb. sphaeroides is reported. The disorder is found to have a marked influence on the calculated rate of energy transfer and is responsible for a faster energy transfer time than would occur in its absence and furthermore accounts for the weak temperature dependence observed in experiment. The excitonic nature of the acceptor (albeit dynamically localized) also has impact in terms of how B850 functions as an energy acceptor. These conclusions are further elucidated by calculations of Rps. acidophila B800−B850 and a series of reconstituted complexes containing a systematically blue-shifted B800 absorption band. The role of dielectric effects is considered. It is reported that interaction of the B800 and B850 transition densities with the carotenoids has an effect on the B800−B850 electronic couplings.
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Citations
Cited by
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Self-citationCoherent Two-Dimensional Optical Spectroscopy
Cho, M. (2008) · Chemical Reviews · doi:10.1021/cr078377b · Cited by 835
Using coherence to enhance function in chemical and biophysical systems
Scholes, G. D., Fleming, G. R., Chen, L. X., Aspuru-Guzik, A., Buchleitner, A., Coker, D. F., Engel, G. S., van Grondelle, R., Ishizaki, A., Jonas, D. M., et al. (2017) · Nature · doi:10.1038/nature21425 · Cited by 668
Self-citationQuantum entanglement in photosynthetic light-harvesting complexes
Sarovar, M., Ishizaki, A., Fleming, G. R., & Whaley, K. B. (2010) · Nature Physics · doi:10.1038/nphys1652 · Cited by 644
Self-citationBeyond Förster Resonance Energy Transfer in Biological and Nanoscale Systems
Beljonne, D., Curutchet, C., Scholes, G. D., & Silbey, R. J. (2009) · The Journal of Physical Chemistry B · doi:10.1021/jp900708f · Cited by 451
Self-citationCoherence in Energy Transfer and Photosynthesis
Chenu, A., & Scholes, G. D. (2015) · Annual Review of Physical Chemistry · doi:10.1146/annurev-physchem-040214-121713 · Cited by 420
Self-citationQuantum Coherent Energy Transfer over Varying Pathways in Single Light-Harvesting Complexes
Hildner, R., Brinks, D., Nieder, J. B., Cogdell, R. J., & van Hulst, N. F. (2013) · Science · doi:10.1126/science.1235820 · Cited by 351
(2009) · Modern Optical Spectroscopy · doi:10.1007/978-3-540-37542-5_7 · Cited by 296
Physical origins and models of energy transfer in photosynthetic light-harvesting
Novoderezhkin, V. I., & van Grondelle, R. (2010) · Physical Chemistry Chemical Physics · doi:10.1039/c003025b · Cited by 217
The feasibility of coherent energy transfer in microtubules.
Craddock, T. J. A., Friesen, D., Mane, J., Hameroff, S., & Tuszynski, J. A. (2014) · Journal of The Royal Society Interface · doi:10.1098/rsif.2014.0677 · Cited by 111
Multiscale model of light harvesting by photosystem II in plants
Amarnath, K., Bennett, D. I. G., Schneider, A. R., & Fleming, G. R. (2016) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1524999113 · Cited by 88
Self-citationElectronic energy migration in microtubules
Kalra, A. P., Benny, A., Travis, S. M., Zizzi, E. A., Morales-Sanchez, A., Oblinsky, D. G., Craddock, T. J. A., Hameroff, S. R., MacIver, M. B., Tuszyński, J. A., et al. (2023) · ACS Central Science · doi:10.1021/acscentsci.2c01114 · Cited by 80
Self-citationEnergy-scales convergence for optimal and robust quantum transport in photosynthetic complexes
Mohseni, M., Shabani, A., Lloyd, S., & Rabitz, H. (2014) · The Journal of Chemical Physics · doi:10.1063/1.4856795 · Cited by 55
Bennett, D. I. G., Fleming, G. R., & Amarnath, K. (2018) · Proceedings of the National Academy of Sciences · doi:10.1073/pnas.1806597115 · Cited by 47
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Metadata
- Authors
- Scholes, G. D., & Fleming, G. R.
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 2000-02-03
- Volume
- 104
- Issue
- 8
- Pages
- 1854-1868
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2002435812
- Cited by
- 463
- References
- 0
- FWCI
- 16.12
- Type
- journal article
- Language
- en
- Open access
- closed
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