Influence of Complex Exciton-Phonon Coupling on Optical Absorption and Energy Transfer of Quantum Aggregates
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We present a theory that efficiently describes the quantum dynamics of an electronic excitation that is coupled to a continuous, highly structured phonon environment. Based on a stochastic approach to non-Markovian open quantum systems, we develop a dynamical framework that allows us to handle realistic systems where a fully quantum treatment is desired yet the usual approximation schemes fail. The capability of the method is demonstrated by calculating spectra and energy transfer dynamics of mesoscopic molecular aggregates, elucidating the transition from fully coherent to incoherent transfer.
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Traditional perturbative treatments (Lindblad, Redfield, modified Redfield) do not well model structured environments and non-perturbative coupling.
“Both features are not well modeled by the traditional perturbative treatments that lead to master equations of Lindblad [139, 140], Redfield [141] or modified Redfield type [46, 142, 143] (see [60] for a review of master equations).”
From Vibrations, quanta and biology (2013) · cites this paper as [141]
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- Authors
- Roden, J., Eisfeld, A., Wolff, W., & Strunz, W. T.
- Affiliations
- Max Planck Institute for the Physics of Complex Systems (DE)
- Venue
- Physical Review Letters
- Publisher
- American Physical Society (APS)
- Published
- 2009-07-31
- Volume
- 103
- Issue
- 5
- Pages
- 058301-058301
- ISSN
- 0031-9007 (ISSN-L)
- 1079-7114
- OpenAlex
- W2066881078
- Cited by
- 109
- References
- 40
- Citations by year
- 2024: 2 · 2022: 3 · 2021: 1 · 2020: 4 · 2019: 4 · 2018: 5 · 2017: 5 · 2016: 6 · 2015: 9 · 2014: 12 · 2013: 12 · 2012: 17
- FWCI
- 8.53
- Type
- journal article
- Language
- en
- Open access
- green
- arxiv.org
- Locations
- Physical Review Letters (publishedVersion)
- PubMed (publishedVersion)
- arXiv (Cornell University) (submittedVersion)
- Max Planck Institute for Plasma Physics (submittedVersion)
- MPG.PuRe (Max Planck Society) (submittedVersion)
- arXiv (Cornell University)
- 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
- exciton-phonon coupling, optical absorption spectra, energy transfer dynamics, stochastic quantum dynamics
- MeSH terms
- Models, Chemical, Quantum Theory, Thermodynamics, Light-Harvesting Protein Complexes
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