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Physical Review Letters

Dipole-Dipole Broadened Line Shape in a Partially Excited Dense Atomic Gas

Vladimir A. Sautenkov, H. van Kampen, E. R. Eliel, J. P. Woerdman

Published Oct 14, 1996• 81 citations
Publisher

Abstract

We have experimentally investigated the resonance line shape of a partially excited dense atomic rubidium vapor at a density where the binary collision approximation starts to break down. The overall spectral shape is well represented by a simple expression for the dielectric function that includes an excitation-dependent linewidth and shift. The results for the excitation dependence of the linewidth agree with an estimate based on a quasistatic picture of the collisions.

DOI
10.1103/physrevlett.77.3327

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We have experimentally investigated the resonance line shape of a partially excited dense atomic rubidium vapor at a density where the binary collision approximation starts to break down. The overall spectral shape is well represented by a simple expression for the dielectric function that includes an excitation-dependent linewidth and shift. The results for the excitation dependence of the linewidth agree with an estimate based on a quasistatic picture of the collisions.
We discuss recently published results of experimental studies of dipole-dipole broadened line shapes in excited atomic vapors. The Lorentz local-field shift and self-broadened width were measured in optically excited potassium and rubidium vapors. Strong reduction of the shift and width was observed. This effect allowed resolve electromagnetically induced dressed states inside the self-broadened spectral profile. The experimental results were interpreted using well-known models of the dipole-dipole interactions.
We study the frequency derivatives of selective reflection from high-density rubidium vapor using a hole-burning technique. Saturation dips are observed inside the self-broadened line shapes. The line self-broadening is a combination of static width and collision width. By analyzing saturation dips, we can separate power broadening and collision width. Our experimental results support the theory of inhomogeneous dipole-dipole induced broadening of transitions in a dense atomic gas, published by J. A. Leegwater and S. Mukamel [Phys. Rev. A 49 (1994) 146].
In this paper, our experimental studies of dipole-dipole interactions in excited resonance gases are discussed. In weakly excited gas the dipole broadening of optical transitions is proportional to its density N. A gas medium can be identified by its density N as rarefied gas, where dipole broadening of atomic transitions is much less than Doppler width, or as dense gas, where dipole broadening is much more than Doppler width. According to our experiments the dipole broadening in rarefied gas does not depend on the optical excitation. This behavior is in a good agreement with predictions of standard theory for impact atomic collisions. In excited dense gas we observed the strong reduction of the dipole broadening. These experimental results are not described by standard theory for impact collisions. We suggested a simple description of the optical properties for excited dense gas.
We study the dipole–dipole spectral broadening of a resonance line at high atomic densities when the self-broadening dominates. The selective reflection spectrum of a weak probe beam from the interface of the cell window and rubidium vapour is recorded in the presence of a far-detuned pump beam. The excitation due to the pump reduces the self-broadening. We found that the self-broadening reduction dependence on the pump power is atomic density independent. These results provide experimental evidence for the disordered exciton based theory of self-broadening, and can be useful for the description of the interaction of a strong optical field with a dense resonance medium.
In the limit of a dipole-dipole interaction between neutral atoms and the binary-collision approximation, we present a theory of pressure broadening in which the multiplet structure of the atomic levels is considered. The appropriate Schr\"odinger equations for the collision problem are numerically integrated to obtain solutions for both resonant and foreign gas broadening. The presence of radiation fields is neglected in the first half of the paper, where the collisional time rate of change of the density matrix is found. The pertinent collisional decay parameters are extracted from these equations. The ratios of the parameters of the average magnetic dipole to electric quadrupole moment obtained were 1.21\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the entire ensemble in resonant broadening, 0.966\ifmmode\pm\else\textpm\fi{}0.012 for the relaxation of the initially excited atoms in resonant broadening, and 1.12\ifmmode\pm\else\textpm\fi{}0.02 for the relaxation of the initially excited atoms in foreign gas broadening. In the second half of the paper, the collisional broadening results are incorporated in a systematic evaluation of (i) spectral profiels (effects arising from the velocity and recoil of the emitting atom are neglected), (ii) Hanle-effect line shapes, and (iii) laser phenomena. For the case of resonant broadening, the radiation trapping process is reviewed and its influence on line shapes discussed. Finally, a detailed comparison of the theory with experimental findings as well as with previous theoretical results is made. We conclude that the dipole-dipole interaction is sufficient to explain most cases of resonant and some cases of foreign gas broadening.
The dipole–dipole broadening of the spectrum of the selective reflection of intense resonance light from the interface between a transparent dielectric and a gas of the natural mixture of Rb isotopes has been studied experimentally. The case of a high gas density where the Doppler broadening can be neglected has been investigated. It has been shown that dipole–dipole broadening is reduced with increasing the number density of excited atoms. When the laser beam intensity is much higher than the saturation intensity of a resonance transition, a significant broadening due to the very high laser beam intensity has not been observed in the reflection spectrum from the transparent dielectric/gas interface. The observed intensity dependence of the spectral width has been explained by the quenching collisions of the excited atoms with the interface.