Transfer of vibrational coherence through incoherent energy transfer process in Forster limit

Summary, in English

We study transfer of coherent nuclear oscillations between an excitation energy donor and an acceptor in a simple dimeric electronic system coupled to an unstructured thermodynamic bath and some pronounced vibrational intramolecular mode. Our focus is on the nonlinear optical response of such a system, i.e., we study both excited state energy transfer and the compensation of the so-called ground-state bleach signal. The response function formalism enables us to investigate a heterodimer with monomers coupled strongly to the bath and by a weak resonance coupling to each other (Forster rate limit). Our work is motivated by recent observation of various vibrational signatures in two-dimensional coherent spectra of energy-transferring systems including large structures with a fast energy diffusion. We find that the vibrational coherence can be transferred from donor to acceptor molecules provided the transfer rate is sufficiently fast. The ground-state bleach signal of the acceptor molecules does not show any oscillatory signatures, and oscillations in ground-state bleaching signal of the donor prevail with the amplitude, which is not decreasing with the relaxation rate.

• Author: Tomas Mancal; Jakub Dostal; Jakub Psencik; Donatas Zigmantas
• Department/s: Chemical Physics
• Publishing year: 2014
• Language: English
• Pages: 135-143
• Publication/Series: Canadian Journal of Chemistry
• Volume: 92
• Issue: 2
• Links: http://dx.doi.org/10.1139/cjc-2013-0351
• Document type: Journal article
• Publisher: National Research Council of Canada
• Topic: Atom and Molecular Physics and Optics
• Keywords: 2D coherent spectroscopy; vibrational coherence; coherence transfer; energy transfer
• Status: Published
• ISBN/ISSN/Other: ISSN: 0008-4042