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Soviet Journal of Quantum Electronics

Collisional-radiative cooling and heating of a gas

Faris Gel’mukhanov, А. И. Пархоменко, В. Е. Прокопьев, Anatolii M. Shalagin

Published Oct 31, 1980• 5 citations
Publisher

Abstract

An analysis is made of a new effect resulting in cooling or heating of a resonant gas in a radiation field. The effect is due to collisions of resonant atoms with particles of a buffer gas. The magnitude of the effect depends on the ratio of the transport cross sections of the excited and ground states. Qualitative estimates of the degree of cooling or heating are obtained.

DOI
10.1070/qe1980v010n10abeh010585

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Physical Review A•Sep 1, 1993•2 citations
An analysis is made of a new effect resulting in cooling or heating of a resonant gas in a radiation field. The effect is due to collisions of resonant atoms with particles of a buffer gas. The magnitude of the effect depends on the ratio of the transport cross sections of the excited and ground states. Qualitative estimates of the degree of cooling or heating are obtained.
We describe experiments on the laser cooling of both helium-rubidium and argon-rubidium gas mixtures by collisional redistribution of radiation. Frequent alkali-noble gas collisions in the ultradense gas, with typically 200 bar of noble buffer gas pressure, shift a highly red detuned optical beam into resonance with a rubidium Dline transition, while spontaneous decay occurs close to the unshifted atomic resonance frequency. The technique allows for the laser cooling of macroscopic ensembles of gas atoms. The use of helium as a buffer gas leads to smaller temperature changes within the gas volume due to the high thermal conductivity of this buffer gas, as compared to the heavier argon noble gas, while the heat transfer within the cell is improved.
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 interaction of an intense optical-maser field with excited atoms in a gas discharge leads to a considerable change in the population of those levels which are resonant at the maser frequency. This will cause a change in the population of other levels that are connected to the maser levels through collision-induced nonradiative as well as radiative transitions. Using the 1.15-\ensuremath{\mu} optical maser, these effects have been studied in detail for the 2s2s2s levels of neon where the changes are completely due to collisions. By analyzing the intensity changes in spontaneous emission originating from a gas-discharge cell placed within the maser resonator, we have observed the approach to a partial thermalization of two closely spaced levels. In this way we have been able to obtain the atomic-collision cross section for excitation transfer between the 2s22{s}_{2}2s2​ and 2s32{s}_{3}2s3​ levels. In pure neon this has been found to be ${\ensuremath{\sigma}}_{23}=(2.3\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2. For a helium-neon mixture the measured cross section is ${\ensuremath{\sigma}}_{23}=(1.8\ifmmode\pm\else\textpm\fi{}0.3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}16}$ cm2{\mathrm{cm}}^{2}cm2. The experimental method used to determine these cross sections eliminates the uncertainties caused by the effects of electron-atom collisions and radiative cascade. These techniques also yield the ratio of the Einstein coefficients for the transitions $2{s}_{2}\ensuremath{\rightarrow}2{p}_{10}$ and $2{s}_{3}\ensuremath{\rightarrow}2{p}_{10}$. The measured ratio is $\frac{{A}_{2}}{{A}_{3}}=3.0\ifmmode\pm\else\textpm\fi{}0.4$.
A theory is given of radiative collisions, i.e., of elementary events in which the emission of a photon occurs in the course of a collision. Special attention is paid to radiative collisions stimulated by a laser field. Simple but clear approaches formulated in the forties or fifties are described briefly. This theory applies, in particular, to collisions in a strong electromagnetic field which affect the collision dynamics. Chemical radiative collisions, i.e., chemical reactions stimulated by photons absorbed in the course of a collision, are reviewed. An analysis is made of several recent experiments in which the theoretically predicted effects were observed: these include the radiative-collisional transfer of excitation from atom to atom, nonlinear effects due to the influence of the field on the collision dynamics, and photosubstitution of one of the atoms in a halogen molecule with an inert gas atom.
We propose a method to study the rotational relaxation of polar molecules [here taking fluoromethane (CH3F)({\mathrm{CH}}_{3}\mathrm{F})(CH3​F) as an example] in collisions with 3.5 K buffer-gas helium (He) atoms by using an electrostatic guiding technique. The dependence of the guiding signal of CH3F{\mathrm{CH}}_{3}\mathrm{F}CH3​F on the injected He flux and the dependence of the guiding efficiency of CH3F{\mathrm{CH}}_{3}\mathrm{F}CH3​F on its rotational temperature are investigated both theoretically and experimentally. By comparing the experimental and simulated results, we find that the translational and rotational temperatures of the buffer-gas cooled CH3F{\mathrm{CH}}_{3}\mathrm{F}CH3​F molecules can reach to about 5.48 and 0.60 K, respectively, and the ratio between the translational and average rotational collisional cross sections of ${\mathrm{CH}}_{3}\mathrm{F}\ensuremath{-}\mathrm{He}$ is $\ensuremath{\gamma}={\ensuremath{\sigma}}_{t}/{\ensuremath{\sigma}}_{r}=36.49\ifmmode\pm\else\textpm\fi{}6.15$. In addition, the slowing, cooling, and boosting effects of the molecular beam with different injected He fluxes are also observed and their forming conditions are investigated in some detail. Our study shows that our proposed method can not only be used to measure the translational and rotational temperatures of the buffer-gas cooled molecules, but also to measure the ratio of the translational collisional cross section to the average rotational collisional cross section, and even to measure the average rotational collisional cross section when the translational collisional cross section is measured by fitting the lifetime of molecule signal to get a numerical solution from the diffusion equation of buffer-gas He atoms in the cell.
The transfer of energy from the translational to the internal degrees of freedom or vice versa is analyzed for radiatively assisted inelastic collisions among atoms in a gas. For a specific atomic-level configuration, it is shown that the absorption of a laser photon may induce a transition between two levels that are displaced by the collisional interaction (a dipole-dipole potential in this treatment) if a fraction of the kinetic energy of the atomic relative motion is simultaneously absorbed. The process thus results in a cooling of the atomic kinetic temperature. In other level configurations, energy goes in the opposite direction, with a heating of the kinetic temperature. This mechanism is described by means of the Wigner-function formalism, which allows a passing to the quasiclassical limit for the atomic motion in a simple way.