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International Conference on Ultrafast Phenomena

Two-Color Three Pulse Photon Echo Peak Shift Spectroscopy

Ritesh Agarwal, Bradley S. Prall, Abbas H. Rizvi, Mino Yang, Graham R. Fleming

Published Jan 1, 2002• 0 citations
Publisher

Abstract

Two-color three pulse photon echo spectroscopy has been used to probe correlation in two different regions of the electronic spectrum of a chromophore in the condensed phase.
DOI
10.1364/up.2002.wd29

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Two-color three pulse photon echo peak shift spectroscopy

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Two-color three pulse photon echo peak shift spectroscopy (2C3PEPS) has been used to probe correlation in electronic transitions in two different regions of the electronic spectrum of a chromophore in the condensed phase. The 2C3PEPS can be done in an “uphill” or a “downhill” sense, where the first two interactions are of lower (higher) frequency than the final interaction with the radiation field. In both cases no correlation between the two spectral regions is observed at very short times. Different parts of the spectrum gain correlation owing to ultrafast solvent motion and the accompanying Stokes shift. We propose a model for the spectral shift that incorporates a conditional probability distribution for transition frequencies in the two spectral regions. The model qualitatively reproduces all the features of complete numerical simulations. Our results show that memory is partially conserved during the spectral diffusion process from the pump to the probe region. The downhill difference peak shift is very sensitive to the time scale of the inertial component of solvation and seems very promising for an accurate determination of this time scale.
A two-color photon echo peak shift measurement to probe the electronic coupling strength in molecular complexes is proposed. Exciton transfer between the electronic eigenstates is neglected and the baths associated with each monomer are assumed to be independent of each other. Within this simplified model, we derive a useful relation which can be used to estimate the electronic coupling strength via a combination of a normal one-color and the present two-color peak shift measurements. A simulation based on the cumulant expansion technique illustrates the validity of our suggestion.