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Cited by 130Spectroscopy and Quantum Chemical StudiesPhotosynthetic Processes and MechanismsPhotochemistry and Electron Transfer Studies

Coherent Nuclear and Electronic Dynamics in Primary Charge Separation in Photosynthetic Reaction Centers: A Redfield Theory Approach

Novoderezhkin, Vladimir I., Yakovlev, Andrey G., van Grondelle, Rienk, Shuvalov, Vladimir A.·2004·The Journal of Physical Chemistry B
DOI 10.1021/jp0373346
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Abstract

Primary charge separation dynamics is modeled in the pheophytin-modified Rhodobacter sphaeroides R-26 reaction center (RC). To explain the observed spectral evolution, it is assumed that the process is coupled to coherent nuclear motion. A density matrix equation with the Redfield relaxation superoperator is used for simulation of the electron-vibrational dynamics and its spectral signatures. The model includes two diabatic states, i.e., an excited state P* of the primary donor (i.e., special pair, P), and a charge-transfer state (P + B -, which is the primary photoproduct in the pheophytin-modified RC). The strong coupling of these states with two collective nuclear modes is supposed. The mixing of diabatic states (with different displacements along each of the two nuclear coordinates) results in a complicated potential surface that determines the dynamics of the excited-state wave packet. The coupled nuclear and charge-transfer dynamics is calculated in the basis of vibronic eigenstates obtained by numerical diagonalization of the electron-vibrational Hamiltonian. The third-order nonlinear response associated with excited-state dynamics is calculated, including the P* → P stimulated emission (SE) and the P + B - → P + (B - )* excited-state absorption (ESA). The model allowed us to obtain a quantitative fit of the experimental kinetics of the SE near 900−950 nm and the ESA in the 1020-nm region of the pheophytin-modified Rhodobacter sphaeroides R-26 RC (Yakovlev, A. G.; Shkuropatov, A. Ya.; Shuvalov, V. A. FEBS Lett. 2000, 466, 209). By use of the parameters adjusted from the fit, we have obtained a direct visualization of the electron-vibrational wave packet evolution, including the surface-crossing dynamics superimposed with oscillatory motion along two reaction coordinates in the P* and P + B - states. It is concluded that nonequilibrated vibrational modes involved in electron-transfer play an important role in photoproduct formation in bacterial RC. We found that the specific configuration of two vibrational coordinates (obtained from the modeling) determines high efficiency of charge separation both for coherent and noncoherent excitation.

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Crossref · 10.1021/jp0373346

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  • With the advent of femtosecond transient absorption spectroscopy in the early 1990s, long-lived vibrational coherences, lasting on the order of a picosecond, were detected for bacterial and plant light-harvesting complexes.

    “With the advent of femtosecond transient absorption spectroscopy in the early 1990s, long-lived vibrational coherences, lasting on the order of a picosecond, were detected for bacterial and plant light-harvesting complexes [35 -40].”

    From The future of quantum biology (2018) · cites this paper as [40]

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Authors
Novoderezhkin, V. I., Yakovlev, A. G., van Grondelle, R., & Shuvalov, V. A.
Affiliations
  • Lomonosov Moscow State University (RU)
  • A. N. Belozersky Institute of Physico-Chemical Biology, Moscow State University, Leninskie Gory, 119992, Moscow, Russia, and Department of Biophysics and Physics of Complex Systems, Faculty of Sciences, Vrije Universiteit, De Boelelaan 1081, 1081 HV Amsterdam, The Netherlands
ORCID
Novoderezhkin, Vladimir I.
Venue
The Journal of Physical Chemistry B
Publisher
American Chemical Society (ACS)
Published
2004-05-05
Volume
108
Issue
22
Pages
7445-7457
ISSN
  • 1520-5207 (ISSN-L)
  • 1520-6106
DOI
10.1021/jp0373346
OpenAlex
W2123017736
Cited by
130
References
39
Citations by year
2026: 5 · 2025: 6 · 2024: 4 · 2023: 1 · 2022: 3 · 2021: 5 · 2020: 8 · 2019: 9 · 2018: 3 · 2017: 9 · 2016: 5 · 2015: 11 · 2014: 9 · 2013: 16 · 2012: 8
FWCI
2.25
Type
journal article
Language
en
Open access
closed
Locations
  • The Journal of Physical Chemistry B (publishedVersion)
  • VU Research Portal (publishedVersion)
  • Digital Academic REpository of VU University Amsterdam (Vrije Universiteit Amsterdam) (submittedVersion)
  • Data Archiving and Networked Services (DANS) (submittedVersion)
Topics
  • Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
  • Life Sciences › Biochemistry, Genetics and Molecular Biology › Molecular Biology › Photosynthetic Processes and Mechanisms
  • Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Keywords
primary charge separation, photosynthetic reaction center, vibronic coupling, diabatic states, charge-transfer states, stimulated emission, excited-state absorption, nonlinear optical properties, surface crossing, photoproduct formation

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