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Journal of Physics B Atomic and Molecular Physics

The effect of collisions on resonance fluorescence and Rayleigh scattering at high intensities

Jan Fiutak, Jan Van Kranendonk

Published Aug 14, 1980• 33 citations
Publisher

Abstract

The theory of the collisional and radiative relaxation of an atom perturbed by foreign-gas atoms in the presence of an intense monochromatic laser beam is developed. The spatial degeneracy of the levels and the reorientation effects of the collisions are included. The impact approximation is not made, but the Doppler effect is neglected. The spectrum of the fluorescent and scattered light is obtained from an eigenvalue problem in Liouville space using the dressed-atom approach and rotationally irreducible tensors. Minimal symmetry-adapted bases in Liouville space are constructed for linear, circular and elliptical incident polarisation. The method is illustrated for S 0 -P 1 transitions.

DOI
10.1088/0022-3700/13/15/006

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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.

Optics and Spectroscopy•Dec 1, 2021•1 citation
The theory of the collisional and radiative relaxation of an atom perturbed by foreign-gas atoms in the presence of an intense monochromatic laser beam is developed. The spatial degeneracy of the levels and the reorientation effects of the collisions are included. The impact approximation is not made, but the Doppler effect is neglected. The spectrum of the fluorescent and scattered light is obtained from an eigenvalue problem in Liouville space using the dressed-atom approach and rotationally irreducible tensors. Minimal symmetry-adapted bases in Liouville space are constructed for linear, circular and elliptical incident polarisation. The method is illustrated for S 0 -P 1 transitions.
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.
Resonance fluorescence due to intense laser fields from a Zeeman degenerate atom being perturbed by collisional interactions is calculated in the impact regime by using the quantum-fluctuation-regression theorem. Various interesting effects are found. For example, the scattered intensity spectrum for a J=0J=0J=0 to J=1J=1J=1 transition for polarization parallel to the laser polarization is essentially an asymmetric triplet, whereas for a perpendicular polarization due to collisions the spectrum is essentially a doublet (whose frequencies do not correspond with any of those of the triplet). Further, the width of the fluorescent component (whose frequency is close to the unperturbed frequency) actually decreases with increasing laser power.
The author derives an expression for the spectrum of the radiation scattered by an atom that suffers binary collisions in the weak-field limit. The frequency of the incident radiation is in near-resonance with a multiplet transition. The authors accounts for strong atom-perturber correlations that are induced when the incident or the detected frequency is in the far wing of an absorption line. For an isolated transition between two degenerate atomic levels the model picture of quasistatic absorption followed by adiabatic reorientation of the excited state predicts a redistributed fluorescence line with a polarisation that is determined by geometrical factors.
The time-dependent theory of Courtens and Sz\"oke is generalized using the approach of Burnett et al. to derive time-dependent spectral intensities of resonance fluorescence from atoms driven by a pulsed laser in the presence of collisions. These results are valid both for laser detunings inside and outside the usual impact region of the spectrum, including Zeeman degeneracy effects. We apply this theory to a simple but important example (J=0J=0J=0 to J=1J=1J=1) to obtain quantitative predictions for the observable scattered-light spectrum which can be directly compared with recent experiments.
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.