Calculation of the signal time-profile in transient CARS experiments

Year: 1991

Authors: Torre R., Righini R., Foggi P., Angeloni L.

Autors Affiliation: European Laboratory for Non Linear Spectroscopy (LENS), Universitą di Firenze, Florence, I-50125, Italy; Dipartimento di Fisica, Universitą di Firenze, Florence, I-50125, Italy; Dipartimento di Chimica, Universitą di Firenze, Florence, I-50121, Italy

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 (?1). Under this assumption the effect of the noise content of ?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.

Journal/Review: APPLIED PHYSICS B-PHOTOPHYSICS AND LASER CHEMISTRY

Volume: 52 (2)      Pages from: 132  to: 137

KeyWords: Laser Beams – Polarization; Light – Nonlinear Optical Effects; Potassium Compounds – Spectroscopic Analysis, Coherent Anti-Stokes Raman Spectroscopy; Nonlinear Polarization, Spectroscopy, Raman
DOI: 10.1007/BF00357667

Citations: 3
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