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Physical Review A

Measurements of velocity-changing collision kernels

Kurt Gibble, Alan Gallagher

Published Feb 1, 1991• 46 citations
Publisher

Abstract

Measurements of velocity-changing collision (VCC) kernels are obtained using velocity-selective optical pumping. This is the first measurement of the shape of an elastic VCC kernel over the full thermal range of velocity changes. Since ground-state collisions are studied (5${\mathit{s}}_{1/2}$ Rb and He, Ne, Ar, Kr, or Xe), very low buffer-gas pressures can be used, and therefore pressure broadening (dephasing collisions) does not obscure the effects of VCC's. The data are deconvolved to eliminate the effects of the natural linewidth and are then extrapolated with respect to buffer-gas pressure to determine the single-collision limit. For small initial velocities, the measured kernels are consistent with a hard-sphere model for large velocity changes, but differ significantly for small velocity changes. The measured VCC kernels for large initial velocities and large velocity changes do not exhibit this agreement with the hard-sphere kernel. This implies that information about the inter- atomic potential can be obtained from a measurement of VCC kernels. We also show the inadequacy of the much-used Keilson-Storer kernel [J. Appl. Math. 10, 243 (1952)].

DOI
10.1103/physreva.43.1366

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Measurements of velocity-changing collision (VCC) kernels are obtained using velocity-selective optical pumping. This is the first measurement of the shape of an elastic VCC kernel over the full thermal range of velocity changes. Since ground-state collisions are studied (5s1/2{\mathit{s}}_{1/2}s1/2​ Rb and He, Ne, Ar, Kr, or Xe), very low buffer-gas pressures can be used, and therefore pressure broadening (dephasing collisions) does not obscure the effects of VCC's. The data are deconvolved to eliminate the effects of the natural linewidth and are then extrapolated with respect to buffer-gas pressure to determine the single-collision limit. For small initial velocities, the measured kernels are consistent with a hard-sphere model for large velocity changes, but differ significantly for small velocity changes. The measured VCC kernels for large initial velocities and large velocity changes do not exhibit this agreement with the hard-sphere kernel. This implies that information about the inter- atomic potential can be obtained from a measurement of VCC kernels. We also show the inadequacy of the much-used Keilson-Storer kernel [J. Appl. Math. 10, 243 (1952)].
We report on a quantitative experimental investigation of velocity-changing collisions by means of velocity-selective optical pumping (VSOP). We have calculated the VSOP line shape for an atom with hyperfine structure with the use of two phenomenological kernels for the collision effects: the Keilson-Storer kernel, and a two-term kernel consisting of a broad Keilson-Storer part and a narrower Gaussian component. Corrections were included to account for the finite absorption in the sample and the backward reflection of the pumping beam. The experiments were carried out in sodium vapor with neon as the perturber gas. The D1{D}_{1}D1​ line of sodium was used for optical pumping, and the orientation of the ground state was detected. Free parameters of the theory were determined by fitting the predicted line shapes to experimental curves. The Keilson-Storer kernel proved unsatisfactory, but the two-term kernel reproduced well the observed line shapes over the entire collision profiles in the neon pressure range 0-57 mtorr. In an independent experiment using rapidly modulated VSOP we also measured directly the cross section of velocity-changing collisions: $\ensuremath{\sigma}=(1.13\ifmmode\pm\else\textpm\fi{}0.10)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}14}$ cm2{\mathrm{cm}}^{2}cm2. The large weight obtained for the narrow Gaussian from the fits, as well as the collision cross section which is three times as large as the cross section deduced from tabulated gas kinetic radii, may indicate the presence of collisions with relatively small velocity changes in addition to hard-sphere encounters.
Measurements of resonant, two-step excitation of sodium in the presence of very-low-pressure buffer gases (He, Ar, Xe, and N2{\mathrm{N}}_{2}N2​) are reported. These data are analyzed to isolate the effects of line broadening and velocity-changing (VC) collisions in the single-collision limit. Velocity dependence of the several line broadenings involved is obtained from this data analysis. The inelastic VC kernels are also obtained as a function of initial velocity.
We report on an experimental investigation of the collision kernels governing the effects of velocity-changing collisions, fine-structure-changing collisions, and their interplay, for Na--noble-gas pairs. The velocity distributions in the two Na excited-state fine-structure levels and in the Na ground-state hyperfine levels have been measured in the presence of a pump laser which produces velocity-selective excitation. For interpretation of these experiments we use a rate-equation model developed in the context of light-induced drift: the velocity-changing collisions are accounted for by a composite Keilson-Storer kernel describing large-angle and small-angle collisions and the fine-structure-changing collisions are treated in the sudden limit. The model is valid for arbitrarily high pump laser intensities and uses only a single adjustable parameter characterizing the small-angle scattering. It is found that the theory describes the experimental velocity distributions in all four Na levels over a wide range of experimental parameters for each Na--noble-gas pair. The relevance of the collision kernels deduced in the present work is discussed in the context of light-induced drift.
We report the results of an experimental study of the effects of velocity-changing collisions on two-photon and stepwise-absorption line shapes. Excitation spectra for the $3{S}_{\frac{1}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}\ensuremath{\rightarrow}4{D}_{\frac{1}{2}}$ transitions of sodium atoms undergoing collisions with foreign gas perturbers are obtained. These spectra are obtained with two cw dye lasers. One laser, the pump laser, is tuned 1.6 GHz below the $3{S}_{\frac{1}{2}}\ensuremath{\rightarrow}3{P}_{\frac{1}{2}}$ transition frequency and excites a nonthermal longitudinal velocity distribution of excited 3P123{P}_{\frac{1}{2}}3P21​​ atoms in the vapor. Absorption of the second (probe) laser is used to monitor the steady-state excited-state distribution which is a result of collisions with rare gas atoms. The spectra are obtained for various pressures of He, Ne, and Kr gases and are fit to a theoretical model which utilizes either the phenomenological Keilson-St\"orer or the classical hardsphere collision kernel. The theoretical model includes the effects of collisionally aided excitation of the 3P123{P}_{\frac{1}{2}}3P21​​ state as well as effects due to fine-structure state-changing collisions. Although both kernels are found to predict line shapes which are in reasonable agreement with the experimental results, the hard-sphere kernel is found superior as it gives a better description of the effects of large-angle scattering for heavy perturbers. Neither kernel provides a fully adequate description over the entire line profile. The experimental data is used to extract effective hard-sphere collision cross sections for collisions between sodium 3P123{P}_{\frac{1}{2}}3P21​​ atoms and helium, neon, and krypton perturbers.
The velocity changing collisions (vcc) play an important role in the description of velocity redistribution of particles caused by nearly resonant interaction with the laser light and collisions (1). Collision relaxation rates are conveniently described by collision kernels which, in turn, depend on interatomic potential and scattering amplitudes and is proportional to the collision cross section. The population kernel gives the probability density per unit time that an active particle in state 1 i> undergoes collisions with perturbers (usually a noble gas atom or impurity), which changes the active particle velocity from v′ to v. Due to the fact that perturber-active particle interaction is state dependent the collisions cause different changes in the ground and excited states of active particle. Although the shape of the populations distributions resembles those from well-known Bennett hole theory, the distribution of the total population has two peaks and obviously is asymmetrical (2). Vcc together with velocity selective laser excitation lead to the asymmetry of the ground and excited state population. The flux of excited particles has properties which are different from that of ground state because of interaction collision potentials for both states. The intensity of the laser light strongly influences the velocity distributions of the ground and excited state populations.
Line-shape expressions for two-step resonant excitation in the presence of low-pressure perturbers are derived. These expressions allow for velocity-dependent broadening rates and are well suited for studying the line-shape contributions due to coherent excitation, incoherent excitation (due to dephasing collisions), interference between coherent and incoherent excitation, and velocity-changing collisions. Using the sodium 3S-3P-4D system perturbed by noble-gas atoms as an example and assuming C6{C}_{6}C6​ interaction potentials, line shapes at a variety of laser detunings (Doppler selected atomic velocities) are numerically calculated to study variation in the line shape due to competing excitation paths and speed-dependent collision rates. In order to deal with both the line core and the line wing a composite collision kernel consisting of a Lorentzian kernel for small \ensuremath{\Delta}vz{v}_{z}vz​ collisions and a Keilson-Storer kernel for large \ensuremath{\Delta}vz{v}_{z}vz​ collisions is used. It is also demonstrated how the inelastic (3P3/2{P}_{3/2}P3/2​-3P1/2{P}_{1/2}P1/2​) velocity-changing collision kernel may be obtained from experimental data at low pressures. Theoretical line shapes and broadening rates are compared with experiment.