The nature of the low energy band of the Fenna-Matthews-Olson complex: Vibronic signatures
Open accessAbstract
Based entirely upon actual experimental observations on electron-phonon coupling, we develop a theoretical framework to show that the lowest energy band of the Fenna-Matthews-Olson complex exhibits observable features due to the quantum nature of the vibrational manifolds present in its chromophores. The study of linear spectra provides us with the basis to understand the dynamical features arising from the vibronic structure in nonlinear spectra in a progressive fashion, starting from a microscopic model to finally performing an inhomogeneous average. We show that the discreteness of the vibronic structure can be witnessed by probing the diagonal peaks of the nonlinear spectra by means of a relative phase shift in the waiting time resolved signal. Moreover, we demonstrate that the photon-echo and non-rephasing paths are sensitive to different harmonics in the vibrational manifold when static disorder is taken into account. Supported by analytical and numerical calculations, we show that non-diagonal resonances in the 2D spectra in the waiting time, further capture the discreteness of vibrations through a modulation of the amplitude without any effect in the signal intrinsic frequency. This fact generates a signal that is highly sensitive to correlations in the static disorder of the excitonic energy albeit protected against dephasing due to inhomogeneities of the vibrational ensemble.
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There is compelling theoretical and/or experimental evidence that quantum phenomena are essential for understanding magneto-reception of birds.
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- Authors
- Caycedo-Soler, F., Chin, A. W., Almeida, J., Huelga, S. F., & Plenio, M. B.
- Affiliations
- Institute of Theoretical Physics , Albert-Einstein-Allee 11 D-89069 Ulm, Germany
- Universität Ulm (DE)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2012-04-18
- Volume
- 136
- Issue
- 15
- Pages
- 155102-155102
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W1974492467
- Cited by
- 46
- References
- 43
- Citations by year
- 2021: 2 · 2020: 1 · 2019: 2 · 2018: 1 · 2017: 2 · 2016: 5 · 2015: 10 · 2014: 4 · 2013: 10 · 2012: 9
- FWCI
- 5.46
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- The Journal of Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- arXiv (Cornell University)
- Topics
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Spectroscopy and Quantum Chemical Studies
- Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
- Physical Sciences › Physics and Astronomy › Atomic and Molecular Physics, and Optics › Strong Light-Matter Interactions
- Keywords
- Fenna-Matthews-Olson complex, vibronic structure, electron-phonon coupling, vibrational manifold, nonlinear spectroscopy, photon echo, static disorder, dephasing, photosynthetic light harvesting
- MeSH terms
- Thermodynamics, Vibration, Nonlinear Dynamics
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