The expressions for the resonant and non-resonant contributions to the CARS signal in a time-resolved CARS experiment are derived on the basis of a diagrammatic perturbative expansion of the polarization. The laser fields are assumed to be off-resonance with respect to any electronic level of the system. The probe pulse is supposed to be derived from one of the two pump pulses (omega-1). Under this assumption the effect of the noise content of omega-1 laser pulses on the signal time-profile (coherence artefact) is correctly reproduced by modelling the noise as a stationary stochastic process. The choice of appropriate polarization geometries is shown to allow for direct measurement of the individual contributions to the CARS signal; the experiments performed on a KClO4 single crystal fully confirm the results of the calculation based on our theoretical treatment.

Calculation Of The Signal Time-Profile In Transient Cars Experiments / Torre, R.; Righini, R.; Foggi, R.; Angeloni, L.. - In: APPLIED PHYSICS. B, PHOTOPHYSICS AND LASER CHEMISTRY. - ISSN 0721-7269. - STAMPA. - 52:(1991), pp. 132-137. [10.1007/BF00357667]

Calculation Of The Signal Time-Profile In Transient Cars Experiments

TORRE, RENATO;RIGHINI, ROBERTO;ANGELONI, LEONARDO
1991

Abstract

The expressions for the resonant and non-resonant contributions to the CARS signal in a time-resolved CARS experiment are derived on the basis of a diagrammatic perturbative expansion of the polarization. The laser fields are assumed to be off-resonance with respect to any electronic level of the system. The probe pulse is supposed to be derived from one of the two pump pulses (omega-1). Under this assumption the effect of the noise content of omega-1 laser pulses on the signal time-profile (coherence artefact) is correctly reproduced by modelling the noise as a stationary stochastic process. The choice of appropriate polarization geometries is shown to allow for direct measurement of the individual contributions to the CARS signal; the experiments performed on a KClO4 single crystal fully confirm the results of the calculation based on our theoretical treatment.
52
132
137
Torre, R.; Righini, R.; Foggi, R.; Angeloni, L.
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/2158/354736
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