Modelling of oscillations in two-dimensional echo-spectra of the Fenna–Matthews–Olson complex

Hein, Birgit; Kreisbeck, Christoph; Kramer, Tobias; Rodríguez, Mirta

doi:10.1088/1367-2630/14/2/023018

Cited by 120Spectroscopy and Quantum Chemical StudiesStrong Light-Matter InteractionsPhotochemistry and Electron Transfer Studies

Modelling of oscillations in two-dimensional echo-spectra of the Fenna–Matthews–Olson complex

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Hein, Birgit, Kreisbeck, Christoph, Kramer, Tobias, Rodríguez, Mirta·2012·New Journal of Physics

DOI 10.1088/1367-2630/14/2/023018

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Abstract

Recent experimental observations of time-dependent beatings in the two-dimensional echo-spectra of light-harvesting complexes at ambient temperatures have opened up the question of whether coherence and wave-like behaviour play a significant role in photosynthesis. We carry out a numerical study of the absorption and echo-spectra of the Fenna–Matthews–Olson (FMO) complex in Chlorobium tepidum and analyse the requirements in the theoretical model needed to reproduce beatings in the calculated spectra. The energy transfer in the FMO pigment–protein complex is theoretically described by an exciton Hamiltonian coupled to a phonon bath which accounts for the pigments' electronic and vibrational excitations, respectively. We use the hierarchical equations of motions method to treat the strong couplings in a non-perturbative way. We show that the oscillations in the two-dimensional echo-spectra persist in the presence of thermal noise and static disorder.

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ARTICLE pubs.acs.org/JPCB Modified Scaled Hierarchical Equation of Motion Approach for the Study of Quantum Coherence in Photosynthetic Complexes
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Modified Scaled Hierarchical Equation of Motion Approach for the Study of Quantum Coherence in Photosynthetic Complexes
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Authors: Hein, B., Kreisbeck, C., Kramer, T., & Rodríguez, M.
Affiliations: University of Regensburg (DE)
Harvard University (US)
Instituto de Estructura de la Materia (ES)
Venue: New Journal of Physics
Publisher: IOP Publishing
Published: 2012-02-07
Volume: 14
Issue: 2
Pages: 023018
ISSN: 1367-2630 (ISSN-L)
DOI: 10.1088/1367-2630/14/2/023018
OpenAlex: W2018715350
Cited by: 120
References: 53
Citations by year: 2026: 1 · 2025: 5 · 2024: 7 · 2023: 6 · 2022: 2 · 2021: 7 · 2020: 10 · 2019: 5 · 2018: 12 · 2017: 9 · 2016: 12 · 2015: 11 · 2014: 15 · 2013: 10 · 2012: 8
FWCI: 7.28
Type: journal article
Language: en
Open access: gold
doi.org
Licence: cc-by
Locations: New Journal of Physics (publishedVersion, cc-by)
arXiv (Cornell University) (submittedVersion)
DIGITAL.CSIC (Spanish National Research Council (CSIC)) (submittedVersion)
arXiv (Cornell University)
Funders: Deutscher Akademischer Austauschdienst
Deutsche Forschungsgemeinschaft
Ministerio de Ciencia e Innovación
Topics: Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Strong Light-Matter Interactions
Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Keywords: Fenna-Matthews-Olson complex, spectral oscillations, light-harvesting complexes, photosynthetic energy transfer, exciton-phonon coupling, hierarchical equations of motion, thermal noise, static disorder, Chlorobium tepidum

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Modelling of oscillations in two-dimensional echo-spectra of the Fenna–Matthews–Olson complex

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