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Optics and Spectroscopy

Multiphoton resonance fluorescence in a strong low-frequency field

В. П. Крайнов, A. V. Kruglikov

Published Jul 1, 1977• 0 citations
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Journal of the Optical Society of America B•Aug 1, 1998•14 citations
We study the fluorescence spectrum of a strongly driven two-level system (TLS) with modulated transition frequency, which is a bichromatically driven TLS and has multiple resonance frequencies. We are aiming to provide a reliable description of the fluorescence in a regime that is difficult to tackle with perturbation theory and the rotating-wave approximation (RWA), and illustrate the spectral features of the fluorescence under off- and multiphoton-resonance conditions. To go beyond the RWA, we use a semianalytical counter-rotating-hybridized rotating-wave method that combines a unitary transformation and Floquet theory to calculate the two-mode Floquet states and quasienergies for the bichromatically driven TLS. We then solve the master equation accounting for the spontaneous decay in the bases of the two-mode Floquet states, and derive a physically transparent fluorescence spectrum. In comparison with the numerically exact spectrum from the generalized Floquet-Liouville approach, the present spectrum is found to be applicable in a wide range of the parameters where the RWA and the secular approximation may break down. We find that the counter-rotating (CR) terms of the transverse field omitted in the RWA have non-negligible contributions to the spectrum under certain conditions. Particularly, at the multiphoton resonance the width of which is comparable with the Bloch-Siegert shift, the RWA and non-RWA spectra markedly differ from each other because of the CR-induced shift. We also analyze the symmetry of the spectrum in terms of the transition matrix elements between the two-mode Floquet states. We show that the strict symmetry of the spectrum cannot be expected without the RWA but the almost symmetric spectrum can be obtained at the single-photon resonance that takes the Bloch-Siegert shift into account if the driving is moderately strong and at the multiphoton resonance with a sufficiently weak transverse field.
We consider the interaction of a fully amplitude-modulated, narrow-band laser with a strongly inhomogeneously broadened two-level medium and show that harmonics of the fluorescence of susceptibility, unlike the time-averaged fluorescence, retain the characteristic multiphoton resonance structure that is found in the absence of inhomogeneous broadening. This behavior correlates with the existence of double branches of the corresponding Bloch-Siegert resonance curves. For strong fields, the depth of modulation and the phase shift of the lowest fluorescence harmonic may deviate significantly from the results for weak, broadband excitation.
We study the behavior of a two-level atom that is driven by a bichromatic field consisting of a strong resonant component and a weaker tunable component. In addition to the splitting of the energy levels (the multiphoton AC Stark effect), we find that the weaker component also shifts the subharmonic resonances, an effect we attribute to a dynamic Stark shift. When the weaker component is tuned to a shifted resonance, no fluorescence occurs at either the frequency of the strong component or the three-photon mixing frequency. Results are obtained with numerical techniques and explained in terms of the dressed-atom model of the system.