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Off-resonance dispersion in molecular double resonance experiments

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Abstract

This paper analyses effects related to the real part of the gaseous electric susceptibility in microwave-microwave and infrared-microwave double resonance experiments on two transitions with a common level. The most interesting features are obtained when the gaseous refractive index is probed far off resonance, i.e. in the tail of the dispersion characteristic and when the pump frequency is scanned around the resonance: a resonant change of the refractive index for the probe field is observed, the shape of which is that of the saturated pump line. A calculation using a model of strong collisions gives results in good agreement with the experimental ones. Applications of these phenomena to the determination of frequencies and transition matrix elements of infrared lines are discussed in the general case of lack of overlapping of the laser gain profile and of the infrared line. It is proposed to use these dispersion effects to detect Doppler-free infrared two-photon molecular absorption.

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Macke, B. Off-resonance dispersion in molecular double resonance experiments. Appl. Phys. 13, 271–280 (1977). https://doi.org/10.1007/BF00882892

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