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Journal of Physics B Atomic and Molecular Physics

Collisional broadening of resonance fluorescence with excitation by intense radiation of finite bandwidth

Gerard Nienhuis

Published Jun 14, 1980• 9 citations
Publisher

Abstract

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.

DOI
10.1088/0022-3700/13/11/013

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Journal of Experimental and Theoretical Physics•May 1, 2008•1 citation
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.
The authors derive an expression for the spectrum of fluorescence by a two-state atom in a perturber gas irradiated by nearly resonant monochromatic light of arbitrary intensity. The result is fully expressed in terms of the absorption profile that would be measured in a conventional low-intensity absorption experiment and of the rate of radiative and collisional transitions. The present result generalises previous work and the authors demonstrate that expressions obtained before in special cases are recovered by taking the appropriate limits.
The problem of resonance fluorescence from a two-level atom that is driven near resonance by a laser beam of finite bandwidth is tackled via the Heisenberg equations of motion, by a simple generalization of our previous treatment. It is found that the two-time intensity correlation function is again factorizable into a product of the mean light intensities at the two times, each of which is slightly modified under broad-band excitation from its value under monochromatic excitation. The spectrum of the fluorescence is affected rather more drastically, and, in general, becomes asymmetric under broad-band excitation.
The formal structure of the time dependence of the state of an atom in a perturber bath in an intense classical monochromatic radiation field is studied. The authors allow the cross sections of binary collisions to be affected by the radiation field. The result is used to derive an expression for the collision-broadened saturated fluorescence excitation spectrum and absorption rate in terms of a collisional relaxation operator. This operator can be related to the rate of collisionally aided radiative excitation.
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.