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Soviet Journal of Quantum Electronics

Coherent interaction effects in probe pulse experiments

B. Wilhelmi, Joachım Herrmann

Published Sep 30, 1980• 9 citations
Publisher

Abstract

An investigation is made of resonance absorption of picosecond pulses when time-delayed approximately collinear or exactly counterpropagating pump and probe pulses are superposed in a sample. The coherent and incoherent components of the influence of the probe beam on the absorption are calculated as a function of the delay time. In addition, the influence of phase modulation of the pump wave and emission of waves of different diffraction orders is studied.

DOI
10.1070/qe1980v010n09abeh010652

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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.

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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, when this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model, which allows us to quantify the oscillating features of the resulting transient-absorption spectra in terms of the atomic populations and phases generated by the intense 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.

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Physical Review A•Feb 1, 1994•2 citations
An investigation is made of resonance absorption of picosecond pulses when time-delayed approximately collinear or exactly counterpropagating pump and probe pulses are superposed in a sample. The coherent and incoherent components of the influence of the probe beam on the absorption are calculated as a function of the delay time. In addition, the influence of phase modulation of the pump wave and emission of waves of different diffraction orders is studied.
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.
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.
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.
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, when this is preceded or followed by a strong pump pulse. Numerical results are interpreted in terms of an analytical model, which allows us to quantify the oscillating features of the resulting transient-absorption spectra in terms of the atomic populations and phases generated by the intense 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.
As a succession of two pulses propagates through a medium which exhibits a resonance (single or multiphoton), the resonant parts of the susceptibility will depend on the relative phase of the two pulses, provided the delay between the pulses is shorter than the phase relaxation time of the interaction. As a result of this "coherent interaction", the reradiation of the sample (the fluorescence, the absorption and the generation of harmonics) will be a periodic function of the phase difference and delay between the two pulses of the sequence 1. The study of these coherent effects is important, because one expect to find conditions under which the maximum harmonic conversion to much shorter wavelengths can be greatly enhanced 2. The presence of the multiphoton resonance enhances the nonlinear susceptibility responsible for the harmonic generation, but reduces also the maximum achievable conversion efficiency because of resonant losses (depletion of the fundamental by multiphoton absorption). The latter effect can be eliminated by a judicious choice of the pulse sequencing and phasing. In addition to demonstrating, for the first time, coherent interaction enhancement in harmonic generation, the data of third harmonic versus relative phase of the pulse sequences enable us to measure the phase angle of the third order susceptibility (hence the contribution of the continuum relative to that of the resonance).