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Optics Communications

Probe of the dressed molecule energy levels by infrared radiofrequency double resonance

Armel Jacques, P. Glorieux

Published Jan 1, 1982• 9 citations
Publisher
DOI
10.1016/0030-4018(82)90260-7

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Infrared (ir) radio-frequency (rf) double-resonance spectroscopy was carried out on the vibrational-overtone band of methyl iodide molecules (CH3I). An optical Fabry-Perot cavity was employed as an absorption cell to record saturated ir spectral lines even by a small-power extended-cavity diode laser with a high sensitivity and a wide tunability in the presence of a rf field. These features allowed investigation of molecules strongly coupled with monochromatic and bichromatic rf fields, or dressed molecules, at various rf power levels and detuning frequencies for a variety of ir and rf transitions. At appropriate energy-level schemes, quantum-interference effects were observed. All resultant spectra showed good agreement with dressed-state theoretical calculations, indicating that the present spectrometer is valid for precise investigation of dressed molecules.
The molecular response in laser intracavity experiments where molecules interact simultaneously with a radio frequency field and an infrared one is analyzed theoretically. In the quantized field approach the molecule–radio frequency interaction is treated exactly. For the laser intensity the density matrix equations are solved either in a third-order perturbation treatment or through a matrix continued fraction analysis. The resonance line shapes in different two-level and three-level configurations are analyzed numerically.