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

MPG-Autoren

Duan,  Hong-Guang
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
I. Institut für Theoretische Physik, Universität Hamburg, Jungiusstraße 9, 20355 Hamburg, Germany;
The Hamburg Center for Ultrafast Imaging, Luruper Chaussee 149, 22761 Hamburg, Germany;

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Prokhorenko,  Valentyn
Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science, Notkestraße 85, 22607 Hamburg, Germany;

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New J. Phys. 17 072002.pdf
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Zitation

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.


Zitierlink: http://hdl.handle.net/11858/00-001M-0000-0028-4D63-6
Zusammenfassung
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.