Vibrational wave packet induced oscillations in two-dimensional electronic spectra. I. Experiments

Details Vibrational wave packet induced oscillations in two-dimensional electronic spectra. I. Experiments Vibrational wave packet induced oscillations in two-dimensional electronic spectra. I. Experiments

2010-03-22

arxiv.org/abs/1003.4174v1

J. Chem. Phys. 132 (2010) 184514

Physics

Chemical Physics

13 pages, 8 figures

Scientific paper

10.1063/1.3404404

This is the first in a series of two papers investigating the effect of electron-phonon coupling in two-dimensional Fourier transformed electronic spectroscopy. We present a series of one- and two-dimensional nonlinear spectroscopic techniques for studying a dye molecule in solution. Ultrafast laser pulse excitation of an electronic transition coupled to vibrational modes induces a propagating vibrational wave packet that manifests itself in oscillating signal intensities and line-shapes. For the two-dimensional electronic spectra we can attribute the observed modulations to periodic enhancement and decrement of the relative amplitudes of rephasing and non-rephasing contributions to the total response. Different metrics of the two-dimensional signals are shown to relate to the frequency-frequency correlation function which provides the connection between experimentally accessible observations and the underlying microscopic molecular dynamics. A detailed theory of the time-dependent two-dimensional spectral line-shapes is presented in the accompanying paper [T. Mancal et al., arXiv:1003.xxxx].

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