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Multiple Exciton Coherence Sizes in Photosynthetic Antenna Complexes viewed by Pump−Probe Spectroscopy
Abstract
The pump−probe signal from the light-harvesting antenna LH2 of purple bacteria is analyzed using a Green function expression derived by solving the nonlinear exciton-oscillator equations of motion (NEE). A microscopic definition of the exciton mean free path ( L f ) and localization size ( L ρ ) is given in terms of the off-diagonal elements of the exciton Green function and density matrix, respectively. Using phonon-induced (homogeneous) and disorder-induced (inhomogeneous) line widths compatible with superradiane measurements, we find that at 4.2 K the localization size is L ρ = 15 and that the shift ΔΩ between the positive and negative peaks in the differential absorption is determined by a different effective size L f /2 = 5.6 associated with the exciton mean free path. Our model further predicts the recently observed superradiance coherence size determined by L ρ .
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Citations
Cited by
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Mukamel, S. (2000) · Annual Review of Physical Chemistry · doi:10.1146/annurev.physchem.51.1.691 · Cited by 894
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Beljonne, D., Curutchet, C., Scholes, G. D., & Silbey, R. J. (2009) · The Journal of Physical Chemistry B · doi:10.1021/jp900708f · Cited by 451
Ultrafast excitation energy transfer dynamics in photosynthetic pigment–protein complexes
Renger, T., May, V., & Kühn, O. (2001) · Physics Reports · doi:10.1016/s0370-1573(00)00078-8 · Cited by 413
Novoderezhkin, V., Monshouwer, R., & van Grondelle, R. (2000) · The Journal of Physical Chemistry B · doi:10.1021/jp001881z · Cited by 34
Quantum effects in photosynthesis
van Grondelle, R., & Novoderezhkin, V. I. (2011) · Procedia Chemistry · doi:10.1016/j.proche.2011.08.027 · Cited by 22
Metadata
- Authors
- Meier, T., Chernyak, V., & Mukamel, S.
- Venue
- The Journal of Physical Chemistry B
- Publisher
- American Chemical Society (ACS)
- Published
- 1997-09-01
- Volume
- 101
- Issue
- 37
- Pages
- 7332-7342
- ISSN
- 1520-5207 (ISSN-L)
- 1520-6106
- OpenAlex
- W2100337713
- Cited by
- 195
- References
- 0
- FWCI
- 14.04
- Type
- journal article
- Language
- en
- Open access
- closed
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