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The Journal of Chemical Physics

Radio frequency–infrared double-resonance and multiphoton Lamb dips in a dressed molecule

E. Arimondo, Antonio Sasso, M. Allegrini

Published Mar 1, 1986• 1 citation
Publisher

Abstract

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.

DOI
10.1063/1.450362

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In an optical radio-frequency double-resonance experiment on NO2{\mathrm{O}}_{2}O2​ optical saturation resonances are observed. These resonances appear superimposed on the normal magnetic resonance spectrum. With increasing laser light intensity they change the resonance spectrum considerably. We present a model to describe the observed saturation phenomena: The resonances are attributed to the interaction of two optical photons and at least one radio-frequency photon with the molecule. The theory shows that saturation resonances appear in the population and in the coherence of the dressed-molecule levels in agreement with the experimental results.
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A dressed-state study of lasing without population inversion from a three-level atom interacting with a bichromatic laser field in the ladder configuration is being formulated. The system is allowed to be dressed by both laser-field photons (double dressing). The temporal behavior of the system under consideration is being explored numerically. Although the use of dressed-basis density matrix equations introduces major complexity into the equations, this procedure has crucial importance to the understanding of the atomic spectrum and the underlying physics of the processes involved. The system is found to possess a gain without population inversion, as well as a regular gain with inversion for various transitions, both in the transient and steady-state regimes. Enhancement of the refractive index accompanied by vanishingly small absorption was also found. The frequency response of various transitions is explored via numerical Fourier analysis. Some transitions are found to exhibit a dispersion-like line shape, clear evidence of a quantum-coherent interference effect. The spectrum consists of two distinct quintets centered about the coupling and probe-laser frequencies. The spectral features consisting of each quintet are located symmetrically (at resonance conditions only) around the line center at positions shifted from the center by the generalized Rabi and double Rabi frequencies.