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  On the origin of oscillations in two-dimensional spectra of excitonically-coupled molecular systems

Duan, H.-G., Nalbach, P., Prokhorenko, V., Mukamel, S., & Thorwart, M. (2015). On the origin of oscillations in two-dimensional spectra of excitonically-coupled molecular systems. New Journal of Physics, 17(7): 072002. doi:10.1088/1367-2630/17/7/072002.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-4D63-6 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-4D64-4
Genre: Journal Article

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New J. Phys. 17 072002.pdf (Publisher version), 2MB
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New J. Phys. 17 072002.pdf
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2015
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© IOP Publishing Ltd and Deutsche Physikalische Gesellschaft

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 Creators:
Duan, Hong-Guang1, 2, 3, Author
Nalbach, Peter2, 3, Author
Prokhorenko, Valentyn1, 4, Author              
Mukamel, Shaul5, Author
Thorwart, Michael2, 3, 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, Jungiusstraße 9, 20355 Hamburg, Germany, ou_persistent22              
3The Hamburg Center for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg, Germany, ou_persistent22              
4Center for Free-Electron Laser Science, Notkestraße 85, 22607 Hamburg, Germany, ou_persistent22              
5Department of Chemistry, University of California, Irvine, 1102 Natural Sciences 2, Irvine, California 92697-2025, USA, ou_persistent22              

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Free keywords: exciton dynamics; nonlinear spectroscopy; vibronic effects
 Abstract: We investigate an artificial molecular dimer made of two dipole coupled cyanine dye monomers in which a strong coherent coupling between electronic and vibrational degrees of freedom arises. Clear signatures of this coupling are reflected in an oscillatory time evolution of the off-diagonal vibronic cross peaks in the two-dimensional optical photon echo spectrum. We find a strong coherence component damped by fast electronic dephasing (≈50 fs) accompanied by a much weaker component which decays on the longer time scales (ps) associated to vibrational dephasing. We find that vibronic coupling does not cause longer dephasing times of the dominant photo echo component but additional weak but long-lived components emerge.

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Language(s): eng - English
 Dates: 2015-06-302015-02-262015-07-022015-07-31
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1088/1367-2630/17/7/072002
 Degree: -

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Title: New Journal of Physics
  Abbreviation : New J. Phys.
Source Genre: Journal
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Publ. Info: Bristol : IOP Publishing
Pages: - Volume / Issue: 17 (7) Sequence Number: 072002 Start / End Page: - Identifier: ISSN: 1367-2630
CoNE: /journals/resource/954926913666