Journal
CHEMICAL PHYSICS LETTERS
Volume 459, Issue 1-6, Pages 94-99Publisher
ELSEVIER SCIENCE BV
DOI: 10.1016/j.cplett.2008.05.057
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We report and analyze oscillatory behavior of lineshapes in two-dimensional photon-echo relaxation spectra of a perylene-based dye molecule, whose four-wave-mixing signals are strongly modulated by coupling to low-frequency vibrational modes. Vibrational wavepacket motion is found to induce a pronounced beating of the anti-diagonal absorptive peak width, accompanied by orientational changes in the dispersive signal part. The effects are reproduced well by simulations based on a Brownian oscillator model, and can be assigned to periodic alternations in the relative amplitudes of rephasing and non-rephasing contributions to the spectrum. (C) 2008 Elsevier B.V. All rights reserved.
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