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Springer series in chemical physics

Coherence Effects in Pump-Probe Measurements with Collinear, Copropagating Beams

Stephen L. Palfrey, Tony F. Heinz, Kenneth B. Eisenthal

Published Jan 1, 1984• 0 citations
Publisher
DOI
10.1007/978-3-642-82378-7_60

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IEEE Journal of Quantum Electronics•Apr 1, 1983•47 citations
We demonstrate the existence of coherent coupling effects in pump-probe measurements with collinear, copropagating beams, despite the absence of any induced spatial gratings in this geometry. The coherent interaction, which is found to be similar but not identical to that for crossed beams, must be taken into account in analyzing relaxation processes occurring on the time scale of the laser pulse. These coherent effects cannot generally be eliminated by detecting the total change in energy in both the pump and probe beams.
When pump-probe measurements are performed using pulses originating from the same laser, it is necessary to consider the coherent interaction between the two pulses in determining any material relaxation rates on the time scale of the laser pulse.1-5 For pump and probe beams crossing at an angle, the source of the coherent artifact can be understood in the following manner.1 When the two beams are simultaneously present in the sample, they interfere to produce a spatial modulation of the dielectric constant. Light from the pump beam then scatters from this induced grating into the probe direction. This model has led to the suggestion that for the collinear, copropagating beams, where the spatial grating disappears, the coherent artifact should vanish.3 While the spatial modulation is eliminated by choosing this geometry, we demonstrate here that the coherent artifact, which results directly from the nonlinear polarizability of the material, still remains. We have, however, been able to develop a general method for isolating the incoherent response, thus permitting the material relaxation to be extracted without any knowledge of the coherence properties of the pulse.
The effect of parametric coupling between pump and probe beams in time-resolved optical Kerr effect is theoretically discussed for various experimental configurations. It is shown that with a cicularly polarized pump beam, the polarization changes induced on a nearly collinear probe beam are due to this coherence effect only. In other configurations, this parametric coupling can appear as an additional contribution to the observed signal, especially when pump and probe are derived from the same laser beam. It is pointed out that this coupling can occur not only when the pump and probe beams are at the same wavelength, but also when the difference or the sum of their frequencies can excite a Raman or a two-photon resonance in the medium.