Abstract
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.
Original language | English |
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Pages (from-to) | 135-143 |
Journal | Canadian Journal of Chemistry |
Volume | 92 |
Issue number | 2 |
DOIs | |
Publication status | Published - 2014 |
Bibliographical note
The information about affiliations in this record was updated in December 2015.The record was previously connected to the following departments: Chemical Physics (S) (011001060)
Subject classification (UKÄ)
- Atom and Molecular Physics and Optics
Free keywords
- 2D coherent spectroscopy
- vibrational coherence
- coherence transfer
- energy transfer