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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28 January 2016
Research Article|
January 27 2016
Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations
Jake Iles-Smith;
Jake Iles-Smith
a)
1Controlled Quantum Dynamics Theory,
Imperial College London
, London SW7 2PG, United Kingdom
2Photon Science Institute and School of Physics and Astronomy,
The University of Manchester
, Oxford Road, Manchester M13 9PL, United Kingdom
3Department of Photonics Engineering,
DTU Fotonik
, Ørsteds Plads, 2800 Kongens Lyngby, Denmark
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Arend G. Dijkstra;
Arend G. Dijkstra
4
Max Planck Institute for the Structure and Dynamics of Matter
, Luruper Chaussee 149, 22761 Hamburg, Germany
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Neill Lambert;
Neill Lambert
5
CEMS, RIKEN
, Saitama 351-0198, Japan
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Ahsan Nazir
Ahsan Nazir
b)
2Photon Science Institute and School of Physics and Astronomy,
The University of Manchester
, Oxford Road, Manchester M13 9PL, United Kingdom
Search for other works by this author on:
Jake Iles-Smith
1,2,3,a)
Arend G. Dijkstra
4
Neill Lambert
5
Ahsan Nazir
2,b)
1Controlled Quantum Dynamics Theory,
Imperial College London
, London SW7 2PG, United Kingdom
2Photon Science Institute and School of Physics and Astronomy,
The University of Manchester
, Oxford Road, Manchester M13 9PL, United Kingdom
3Department of Photonics Engineering,
DTU Fotonik
, Ørsteds Plads, 2800 Kongens Lyngby, Denmark
4
Max Planck Institute for the Structure and Dynamics of Matter
, Luruper Chaussee 149, 22761 Hamburg, Germany
5
CEMS, RIKEN
, Saitama 351-0198, Japan
a)
Electronic mail: [email protected]
b)
Electronic mail: [email protected]
J. Chem. Phys. 144, 044110 (2016)
Article history
Received:
November 18 2015
Accepted:
January 07 2016
Citation
Jake Iles-Smith, Arend G. Dijkstra, Neill Lambert, Ahsan Nazir; Energy transfer in structured and unstructured environments: Master equations beyond the Born-Markov approximations. J. Chem. Phys. 28 January 2016; 144 (4): 044110. https://doi.org/10.1063/1.4940218
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