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Journal of the Optical Society of America B

Coherent interactions in pump–probe absorption measurements: the effect of phase gratings

Stephen L. Palfrey, Tony F. Heinz

Published Apr 1, 1985• 106 citations
Publisher

Abstract

We show that in order to describe completely the coherent coupling between the pump and probe pulses in a pump– probe measurement of transient absorption, the influence of induced phase gratings must be included. The importance of phase gratings is demonstrated experimentally for the case of a bleachable dye and analyzed in terms of transient four-wave mixing. These results are relevant to the interpretation of pump–probe measurements on all time scales performed with pulses from a single laser, particularly when the pulse duration is comparable with the material response time.

DOI
10.1364/josab.2.000674

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We show that in order to describe completely the coherent coupling between the pump and probe pulses in a pump– probe measurement of transient absorption, the influence of induced phase gratings must be included. The importance of phase gratings is demonstrated experimentally for the case of a bleachable dye and analyzed in terms of transient four-wave mixing. These results are relevant to the interpretation of pump–probe measurements on all time scales performed with pulses from a single laser, particularly when the pulse duration is comparable with the material response time.
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.
Abstract The quantum dynamics of a system of Rb atoms, modeled by a V -type three-level system interacting with intense probe and pump pulses, are studied. The time-delay-dependent transient-absorption spectrum of an intense probe pulse is thus predicted, simulating pump-probe experiments in which this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model based on interaction operators , which quantify the transformation undergone by the system under the action of an intense pulse. The oscillating features of the resulting transient-absorption spectra, due to the coupling of several excited states, are thus interpreted in terms of the atomic population and phase changes imposed by the pump and probe pulses. Strong-field-induced phases and their influence on the resulting transient-absorption spectra are thereby investigated for different values of pump and probe intensities and frequencies, focusing on the atomic properties which are encoded in the absorption line shapes for positive and negative time delays.
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.
Four-wave phase conjugation in bleachable dye solutions modeled by two-, three-, and four-level schemes with Stokes-shifted absorption and emission bands is analyzed theoretically. The contribution of different types of dynamic gratings (resonance and thermal) to the formation of the conjugate wave, the influence of pump wave absorption, and the conditions for multistable reflectivity are considered. The conditions of the high reflectivity (R>1) caused by phase dynamic gratings have been determined.>
We present a detailed quantitative theory of transient multiwave mixing effects in a nonlinear medium produced by two incident coherent laser beams. Our theory accounts for all the relevant parameters such as laser pulse widths, medium response times, nonlinearities, interaction length, intensities, beam ratio, phase-modulation effects, losses, side diffractions, and explicitly shows how the dynamics and the multiwave mixing processes are interrelated with these parameters. The crucial role played by the diffracted beams and the time-dependent phase shifts among the beams and the interplay among the various intensity and index gratings are explicitly evaluated. In particular, the gain experienced by a weak incident probe beam via these mixing effects from the incident strong pump beam is investigated as a function of the aforementioned parameters.