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  Two-dimensional photon echoes reveal non-Markovian energy transfer in an excitonic dimer

Duan, H.-G., Frey, M., Thorwart, M., & Nalbach, P. (2016). Two-dimensional photon echoes reveal non-Markovian energy transfer in an excitonic dimer. Physical Review E, 94(5): 052146. doi:10.1103/PhysRevE.94.052146.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0001-923A-9 Version Permalink: http://hdl.handle.net/21.11116/0000-0004-919E-6
Genre: Journal Article

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PhysRevE.94.052146.pdf (Publisher version), 2MB
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2016
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© American Physical Society

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https://dx.doi.org/10.1103/PhysRevE.94.052146 (Publisher version)
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 Creators:
Duan, H.-G.1, 2, 3, Author              
Frey, M.2, 4, Author
Thorwart, M.2, 3, Author
Nalbach, P.5, Author
Affiliations:
1Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
2I. Institut für Theoretische Physik, Universität Hamburg, ou_persistent22              
3The Hamburg Centre for Ultrafast Imaging, ou_persistent22              
4Physikalisches Institut, Universität Freiburg, ou_persistent22              
5Westfälische Hochschule, ou_persistent22              

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 Abstract: We show that strong non-Markovian effects can be revealed by the steady-state two-dimensional (2D) photon echo spectra at asymptotic waiting times. For this, we use a simple dimer toy model that is strongly coupled to a harmonic bath with parameters typical for photoactive biomolecules. We calculate the 2D photon echo spectra employing both the numerically exact hierarchy equation of motion and the quasiadiabatic path integral approach and compare these results with approximate results from a time-nonlocal quantum master equation approach. While the latter correctly reproduces the exact population dynamics at long times, it fails at the same time to correctly describe the 2D photon echo spectra at long waiting times. The differences show that non-Markovian effects are much more important for the steady-state 2D photon echoes than for the equilibrium populations. Thus, accurate theoretical descriptions of the energy transfer dynamics in biomolecular complexes have to be based on numerically exact simulations of the environmental fluctuations when nonlinear response functions are analyzed.

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Language(s): eng - English
 Dates: 2016-08-082016-11-282016-11-28
 Publication Status: Published in print
 Pages: -
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 Rev. Method: Peer
 Identifiers: DOI: 10.1103/PhysRevE.94.052146
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Project name : We acknowledge financial support by the Joachim-Herz- Stiftung, Hamburg, within the PIER Fellowship program and by the excellence cluster “The Hamburg Centre for Ultrafast Imaging—Structure, Dynamics and Control of Matter at the Atomic Scale” of the Deutsche Forschungsgemeinschaft. P.N. acknowledges financial support by the Deutsche Forschungs- gemeinschaft (DFG) Project No. NA394/2-1.
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Title: Physical Review E
  Other : Phys. Rev. E
Source Genre: Journal
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Publ. Info: Melville, NY : American Physical Society
Pages: - Volume / Issue: 94 (5) Sequence Number: 052146 Start / End Page: - Identifier: ISSN: 1539-3755
CoNE: /journals/resource/954925225012