Electronic excitation dynamics in multichromophoric systems described via a polaron-representation master equation
Open accessAbstract
We derive a many-site version of the non-Markovian time-convolutionless polaron master equation [Jang et al., J. Chem Phys. 129, 101104 (2008)]10.1063/1.2977974 to describe electronic excitation dynamics in multichromophoric systems. By treating electronic and vibrational degrees of freedom in a combined frame (polaron frame), this theory is capable of interpolating between weak and strong exciton-phonon coupling and is able to account for initial non-equilibrium bath states and spatially correlated environments. Besides outlining a general expression for the expected value of any electronic system observable in the original frame, we also discuss implications of the Markovian and Secular approximations highlighting that they need not hold in the untransformed frame despite being strictly satisfied in the polaron frame. The key features of the theory are illustrated using as an example a four-site subsystem of the Fenna-Mathews-Olson light-harvesting complex. For a spectral density including a localised mode, we show that oscillations of site populations may only be observed when non-equilibrium bath effects are taken into account. Furthermore, we illustrate how this formalism allows us to identify the electronic and vibrational components of the oscillatory dynamics.
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Full understanding of the chemical compass requires studying the entire system composed of electron spins and nuclear spins.
“To gain a full understanding of the chemical compass and the role of coherence one must study the entire system composed of electron spins and nuclear spins [138].”
From Vibrations, quanta and biology (2013) · cites this paper as [138]
The coherence of the initial state (electronic singlet state and unpolarized nuclear spins) in the basis of eigenstates of the full system in the absence of a magnetic field has predictive power for the sensitivity of the chemical compass.
“It turns out that it is the coherence of the initial state (electronic singlet state and unpolarized nuclear spins) in the basis made up of the eigenstates of the full system in the absence of a magnetic field that has predictive power of the sensitivity of the chemical compass.”
From Vibrations, quanta and biology (2013) · cites this paper as [138]
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- Authors
- Kolli, A., Nazir, A., & Olaya-Castro, A.
- Affiliations
- University College London (GB)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2011-10-20
- Volume
- 135
- Issue
- 15
- Pages
- 154112-154112
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W2120948133
- Cited by
- 124
- References
- 58
- Citations by year
- 2026: 1 · 2025: 5 · 2024: 7 · 2023: 5 · 2022: 7 · 2021: 6 · 2020: 4 · 2019: 8 · 2018: 4 · 2017: 10 · 2016: 10 · 2015: 13 · 2014: 16 · 2013: 13 · 2012: 14
- FWCI
- 7.45
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- The Journal of Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- Research Explorer (The University of Manchester) (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- Spiral (Imperial College London) (submittedVersion)
- arXiv (Cornell University)
- Funders
- Engineering and Physical Sciences Research Council (EP/G005222/1)
- 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
- time-convolutionless master equation, non-Markovian dynamics, multichromophoric systems, exciton-phonon coupling, Markov approximation, secular approximation, light-harvesting complexes, power spectrum
- MeSH terms
- Algorithms, Electrons, Energy Transfer, Models, Chemical, Quantum Theory, Photosynthetic Reaction Center Complex Proteins
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