Vibronic modulation of lineshapes in two-dimensional electronic spectra

Modulation of lineshapes induced by coupling to vibrational modes observed in two-dimensional electronic spectroscopy. 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 stron...

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Bibliographic Details
Published in:Chemical physics letters 2008-06, Vol.459 (1), p.94-99
Main Authors: Nemeth, Alexandra, Milota, Franz, Mančal, Tomáš, Lukeš, Vladimír, Kauffmann, Harald F., Sperling, Jaroslaw
Format: Article
Language:English
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Summary:Modulation of lineshapes induced by coupling to vibrational modes observed in two-dimensional electronic spectroscopy. 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.
ISSN:0009-2614
1873-4448
DOI:10.1016/j.cplett.2008.05.057