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  Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations

Iles-Smith, J., Dijkstra, A., Lambert, N., & Nazir, A. (2016). Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations. The Journal of Chemical Physics, 144(4): 044110. doi:10.1063/1.4940218.

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http://dx.doi.org/10.1063/1.4940218 (Publisher version)
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http://arxiv.org/abs/1511.05181 (Preprint)
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 Creators:
Iles-Smith, Jake1, 2, 3, Author
Dijkstra, Arend4, Author              
Lambert, Neill5, Author
Nazir, Ahsan2, Author
Affiliations:
1Controlled Quantum Dynamics Theory, Imperial College London, London SW7 2PG, United Kingdom, ou_persistent22              
2Photon Science Institute and School of Physics and Astronomy, The University of Manchester, Oxford Road, Manchester M13 9PL, United Kingdom, ou_persistent22              
3Department of Photonics Engineering, DTU Fotonik, Ørsteds Plads, 2800 Kongens Lyngby, Denmark, ou_persistent22              
4Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
5CEMS, RIKEN, Saitama 351-0198, Japan, ou_persistent22              

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Free keywords: Energy transfer; Friction; Partial differential equations; Rotational correlation time; Population dynamics
 Abstract: We explore excitonic energy transfer dynamics in a molecular dimer system coupled to both structured and unstructured oscillator environments. By extending the reaction coordinate master equation technique developed by Iles-Smith et al. [Phys. Rev. A 90, 032114 (2014)], we go beyond the commonly used Born-Markov approximations to incorporate system-environment correlations and the resultant non-Markovian dynamical effects. We obtain energy transfer dynamics for both underdamped and overdamped oscillator environments that are in perfect agreement with the numerical hierarchical equations of motion over a wide range of parameters. Furthermore, we show that the Zusman equations, which may be obtained in a semiclassical limit of the reaction coordinate model, are often incapable of describing the correct dynamical behaviour. This demonstrates the necessity of properly accounting for quantum correlations generated between the system and its environment when the Born-Markov approximations no longer hold. Finally, we apply the reaction coordinate formalism to the case of a structured environment comprising of both underdamped (i.e., sharply peaked) and overdamped (broad) components simultaneously. We find that though an enhancement of the dimer energy transfer rate can be obtained when compared to an unstructured environment, its magnitude is rather sensitive to both the dimer-peak resonance conditions and the relative strengths of the underdamped and overdamped contributions.

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Language(s): eng - English
 Dates: 2015-11-182016-01-072016-01-272016-01-28
 Publication Status: Published in print
 Pages: 13
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1063/1.4940218
arXiv: 1511.05181
 Degree: -

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Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
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Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: - Volume / Issue: 144 (4) Sequence Number: 044110 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226