Unified treatment of quantum coherent and incoherent hopping dynamics in electronic energy transfer: Reduced hierarchy equation approach
Abstract
A new quantum dynamic equation for excitation energy transfer is developed which can describe quantum coherent wavelike motion and incoherent hopping in a unified manner. The developed equation reduces to the conventional Redfield theory and Förster theory in their respective limits of validity. In the regime of coherent wavelike motion, the equation predicts several times longer lifetime of electronic coherence between chromophores than does the conventional Redfield equation. Furthermore, we show quantum coherent motion can be observed even when reorganization energy is large in comparison to intersite electronic coupling (the Förster incoherent regime). In the region of small reorganization energy, slow fluctuation sustains longer-lived coherent oscillation, whereas the Markov approximation in the Redfield framework causes infinitely fast fluctuation and then collapses the quantum coherence. In the region of large reorganization energy, sluggish dissipation of reorganization energy increases the time electronic excitation stays above an energy barrier separating chromophores and thus prolongs delocalization over the chromophores.
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The optimization-based measure of non-Markovianity founded on the trace distance under CP trace-preserving maps is hard to compute in practice due to the nonconvex structure of the set of Markovian maps.
“However, this quantity is hard to compute in practice due to the nonconvex structure of the set of Markovian maps E M [5].”
From Entanglement and Non-Markovianity of Quantum Evolutions (2010) · cites this paper as [5]
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- Authors
- Ishizaki, A., & Fleming, G. R.
- Affiliations
- Lawrence Berkeley National Laboratory (US)
- Venue
- The Journal of Chemical Physics
- Publisher
- AIP Publishing
- Published
- 2009-06-18
- Volume
- 130
- Issue
- 23
- Pages
- 234111-234111
- ISSN
- 0021-9606 (ISSN-L)
- 1089-7690
- OpenAlex
- W2072350015
- Cited by
- 734
- References
- 53
- Citations by year
- 2026: 28 · 2025: 36 · 2024: 39 · 2023: 28 · 2022: 40 · 2021: 31 · 2020: 34 · 2019: 41 · 2018: 37 · 2017: 52 · 2016: 48 · 2015: 46 · 2014: 50 · 2013: 51 · 2012: 69
- FWCI
- 32.10
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- The Journal of Chemical Physics (publishedVersion)
- PubMed (publishedVersion)
- 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
- excitation energy transfer, quantum coherence, incoherent hopping, Redfield theory, Förster theory, reorganization energy, Markov approximation, energy dissipation
- MeSH terms
- Computer Simulation, Electrons, Energy Transfer, Models, Chemical, Quantum Theory
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