Issue 6, 2007

Appearance of intramolecular high-frequency vibrations in two-dimensional, time-integrated three-pulse photon echo data

Abstract

An alternative experimental outline to measure homodyne detected three-pulse photon-echo data is presented. The novel experimental approach allowing for online monitoring and correction of experimental timing and stability is discussed in detail using the paradigm system of Nile blue in alcohol solution. It is shown that excellent signal-to-noise ratios together with high reproducibility of the data can be routinely achieved. We report in detail on the appearance of high-frequency intramolecular vibrations in the two-dimensional three-pulse photon-echo data and suggest that besides the conventionally discussed three-pulse photon-echo peak-shift the width of the integrated echo signal as a function of population time contains identical and easily accessible information on high-frequency intramolecular vibrations. A comparison of experimental data with theoretical modeling is performed showing that the observed echo-width oscillations are in line with predictions of the Brownian oscillator model.

Graphical abstract: Appearance of intramolecular high-frequency vibrations in two-dimensional, time-integrated three-pulse photon echo data

Article information

Article type
Paper
Submitted
02 Oct 2006
Accepted
21 Nov 2006
First published
06 Dec 2006

Phys. Chem. Chem. Phys., 2007,9, 701-710

Appearance of intramolecular high-frequency vibrations in two-dimensional, time-integrated three-pulse photon echo data

B. Dietzek, N. Christensson, P. Kjellberg, T. Pascher, T. Pullerits and A. Yartsev, Phys. Chem. Chem. Phys., 2007, 9, 701 DOI: 10.1039/B614332F

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