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Optics and Spectroscopy

The Effect of Collisions on the Resonance Fluorescence Spectrum of Three-Level Atoms with a V-Configuration of Levels

А. И. Пархоменко, Anatolii M. Shalagin

Published Dec 1, 2021• 1 citation
Publisher

Abstract

The effect of collisions on the resonance fluorescence spectrum of three-level atoms with a V-configuration of levels when excited by two monochromatic resonance fields has been theoretically investigated. The analysis has been carried out for the systems with a small Doppler broadening compared to the collision frequency (high buffer gas pressures) and for the general case of an arbitrary change (from complete failure to complete preservation) of the phase memory at any of the three transitions in the V-system. It has been shown that in the three-level V-type atoms excited by two monochromatic fields, the resonant fluorescence spectrum (the number of spectral lines and their widths) at one of the transitions strongly depends on the presence of resonant radiation at the adjacent transition. Under certain conditions, the line widths will be completely determined by the relaxation characteristics of the adjacent transition and, in particular, can be repeatedly narrowed with an increase in the radiation intensity at the adjacent transition. It has been shown that despite the homogeneous nature of the broadening of the absorption lines, the resonance fluorescence spectrum has a pronounced anisotropy with respect to the mutual orientation of the wave vectors of spontaneous and exciting radiation. It has been established that the line widths in the resonance fluorescence spectrum are proportional to the diffusion coefficient of the atoms interacting with radiation under certain conditions. This fact can serve as the basis for a spectroscopic method for measuring the transport frequencies of the collisions of the radiation-absorbing particles with the buffer ones. It has been shown that the effects of phase memory in the collisions lead to a strong qualitative and quantitative modification of the resonance fluorescence spectrum.

DOI
10.1134/s0030400x21090186

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The effect of collisions on the resonance fluorescence spectrum of three-level atoms with a V-configuration of levels when excited by two monochromatic resonance fields has been theoretically investigated. The analysis has been carried out for the systems with a small Doppler broadening compared to the collision frequency (high buffer gas pressures) and for the general case of an arbitrary change (from complete failure to complete preservation) of the phase memory at any of the three transitions in the V-system. It has been shown that in the three-level V-type atoms excited by two monochromatic fields, the resonant fluorescence spectrum (the number of spectral lines and their widths) at one of the transitions strongly depends on the presence of resonant radiation at the adjacent transition. Under certain conditions, the line widths will be completely determined by the relaxation characteristics of the adjacent transition and, in particular, can be repeatedly narrowed with an increase in the radiation intensity at the adjacent transition. It has been shown that despite the homogeneous nature of the broadening of the absorption lines, the resonance fluorescence spectrum has a pronounced anisotropy with respect to the mutual orientation of the wave vectors of spontaneous and exciting radiation. It has been established that the line widths in the resonance fluorescence spectrum are proportional to the diffusion coefficient of the atoms interacting with radiation under certain conditions. This fact can serve as the basis for a spectroscopic method for measuring the transport frequencies of the collisions of the radiation-absorbing particles with the buffer ones. It has been shown that the effects of phase memory in the collisions lead to a strong qualitative and quantitative modification of the resonance fluorescence spectrum.
The effect of collisions on the resonance fluorescence spectrum of two-level atoms excited by monochromatic resonance radiation is studied. Analysis is performed for systems where the Doppler broadening is small compared to the collision frequency (high buffer gas pressures) and for the general case where collisions arbitrarily change the phase of the radiation-induced dipole moment (from completely interrupted to completely unaffected phase of the dipole moment). Both at a relatively low and at a high excitation radiation intensity, the resonance fluorescence spectrum is shown to depend on whether the two-level system is closed or open. This is especially true for the narrow unshifted Rayleigh scattering line. It is shown that, although the absorption line is homogeneously broadened, the resonance fluorescence spectrum exhibits a clearly pronounced anisotropy. In a direction close to the direction of propagation of the excitation radiation, the Rayleigh scattering line is maximally narrowed. Under certain conditions (that can easily be created in experiments), the width of this line is proportional to the diffusion coefficient of atoms interacting with the radiation.
The influence of phase memory effects on the spectrum of resonance Raman scattering by three-level atoms with the Λ configuration of levels experiencing collisions with buffer gas atoms in a strong monochromatic radiation field is studied theoretically. Systems with a small Doppler broadening compared to the collision frequency (large buffer gas pressures) are analysed in the general case of an arbitrary change (from complete change to complete preservation) in the phase memory at any of three transitions in the Λ system. It is shown that in the absence of the collision relaxation of the low-frequency coherence at the transitions between two lower levels of the Λ system, the radiation scattering spectrum has a spectrally narrow component at the Raman frequency, which, despite the homogeneous broadening of the absorption line, exhibits a strongly pronounced anisotropy. In the direction, close to the propagation direction of exciting radiation, this line maximally narrows down. It is significant that upon optical pumping to the level unaffected by a strong field the resonance Raman spectrum noticeably differs from the spectrum in the case of the probe field. A simple expression is proposed for calculating the degree of the phase memory preservation in collisions from the relative amplitude of the Raman resonance.
The spectrum of weak probe field absorption (amplification) by two-level atoms experiencing collisions with buffer gas atoms in a strong resonance laser field is studied theoretically. Analysis is carried out for systems with a weak Doppler broadening under relatively mild constraints on the strong field intensity for the general case of an arbitrary change in the phase of the radiation-induced dipole moment in elastic collisions of gas particles. It is shown that, in spite of uniform broadening of the absorption line, the probe field spectrum exhibits a clearly manifested anisotropy to mutual orientation of the wavevectors of strong and probe radiation. It is found that the width of resonances in the probe field spectrum under definite conditions (that can easily be created in experiments) is proportional to the diffusion coefficient for atoms interacting with radiation. This fact can form the basis of the spectroscopic method for measuring the transport frequencies of collisions between particles absorbing radiation and buffer particles. It is shown that phase memory effects in collisions strongly modify the probe field spectrum both qualitatively and quantitatively. Simple operative formulas proposed for the probe field spectrum are convenient for experimental data processing.
The absorption (amplification) spectrum of a weak probe field by two-level atoms located in a strong resonant laser field and colliding with buffer-gas atoms is analyzed theoretically. The analysis is performed for low collision frequencies compared to the Doppler absorption linewidth (low gas pressure) and with allowance made for an arbitrary change in the phase of the radiation-induced dipole moment at elastic collisions between gas particles. The phase memory effects have been found to lead to a strong qualitative and quantitative transformation of the probe-field spectrum even at rare collisions, when the well-known Dicke manifestation mechanism of the phase memory effects (the removal of Doppler broadening due to the restriction of the spatial particle motion by collisions) is inoperative. The strong influence of the phase memory effects on the spectral resonances at low gas pressures stems from the fact that the phase-conserving collisions change the velocity dependence of the partial refractive index n ( v ) (the refractive index for particles moving with velocity v ).
The resonance fluorescence spectra of a degenerate three-level atom of the V -type in the field of an intense monochromatic wave with an arbitrary polarization composition are investigated. Analytical expressions are derived for the resonance fluorescence spectra, and the angular distribution of spontaneous fluorescence of atoms is analyzed for the D -line emitted by vapors of alkali atoms. It is shown that the number of lines in the spectrum may decrease in the case of the linear polarization of spontaneous radiation. The radiation relaxation operator is obtained for the D -line of alkali metals in the case when an atom is near the metal surface. Interference effects for such systems are analyzed.
A two-state atom in a perturber gas is irradiated by intense light with an arbitrary spectral profile. The authors derive a general expression for the fluorescence spectrum in terms of the conventional low-intensity absorption profile and the spectral density of the incident light. This result, which contains previous results as special limiting cases, describes the transition from the three-line fluorescence spectrum excited by intense monochromatic light and the power-broadened Lorentzian spectrum produced by broad-band excitation.