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Physical Review Letters

Absorption Line-Narrowing Experiment between Atoms of Two Different Species

J. L. Picqué, Raymond J. Vetter

Published Aug 13, 1979• 3 citations
Publisher

Abstract

An experiment analogous to a three-level absorption line-narrowing experiment is performed between atoms of two different species (krypton and xenon) connected by a resonant excitation transfer. Results show that the hole burned in the velocity distribution of krypton atoms is transferred to xenon ones. This effect is interpreted by introducing a cross-collision kernel. Analysis of the experimental line shapes is consistent with a Gaussian shape of this kernel, whose width is found to be pressure independent.

DOI
10.1103/physrevlett.43.508

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Optics Letters•Oct 15, 2002•1 citation
An experiment analogous to a three-level absorption line-narrowing experiment is performed between atoms of two different species (krypton and xenon) connected by a resonant excitation transfer. Results show that the hole burned in the velocity distribution of krypton atoms is transferred to xenon ones. This effect is interpreted by introducing a cross-collision kernel. Analysis of the experimental line shapes is consistent with a Gaussian shape of this kernel, whose width is found to be pressure independent.
Three-photon excitation and multiphoton ionization techniques have been used to measure self-broadening for several resonance lines in xenon and krypton. Tabulations of widths and shifts of the xenon lines at 146.9, 129.6, 119.2, and 117.0 nm were made for pressures between 50 and 900 Torr. Similar measurements were made for the krypton resonance line at 116.5 nm. For pressures less than 500 Torr the widths were found to be in reasonable agreement with theoretical results, which were extrapolated into regions of concentration where the criteria for their validity are at best questionable. We have also found the lines to be shifted to the high-energy side of the unperturbed line. For four of the five lines studied, the blue shifts increased nearly linearly with increasing pressure. In the four cases where the shift could be measured the ratio of shift to width was close to (1/2. Our experimental technique is very simple, but it has yielded what we believe to be the first resonance broadening data based on absorption under conditions where there is strong trapping of the resonance radiation.
Saturated-absorption profiles of the lines at lambda =557 nm involving the lowest metastable level of krypton show intense and broad Gaussian backgrounds due to thermalising collisions. These backgrounds are greatly reduced by the addition of xenon atoms which quench the metastable level. The variation of the amplitude of the background relative to the amplitude of the narrow absorption resonance versus pressure is quadratic in pure krypton and linear in mixtures of krypton and xenon. An interpretation of the results is given taking into account transit-time effects, while making use of published results for the quenching cross section.
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.
Self-broadening of the 146.96 nm xenon line and 123.58 nm krypton line is studied in the density range 1-100 amagat (2.7 x 1019 — 2.7 × 1021 at. cm-3). The absorption profile is deduced from reflection experiments by a modified Kramers-Krönig analysis. A detailed discussion of the criteria for validity of available theories is given, allowing the determination of the extent to which the cases studied are related to many-body interactions and/or pure resonance forces. The quasistatic theory, in the nearest neighbour approximation, is shown to be valid for interpreting the far wings. Thus it is possible at increasing density, to underline the specific effect of the various kinds of forces : resonance, Van der Waals and repulsive, and to specify the 1u excited state potential which is found weakly attractive for Xe2 and Kr2.
The role of collision-induced transfer of electronic state coherence on the spectral response of an atomic vapor is investigated. It is shown that such collisional effects can lead to the appearance of narrow resonances in the nonlinear spectroscopy of three-level systems. Collisional transfer between different multipoles of electronic state coherence is shown to lead to a breakdown of several percent in Becquerel's relation between the Faraday rotation and dispersion of a vapor. All calculations are carried out in the impact limit of pressure broadening theory. Particular emphasis is given to the order in which the various averages over the velocity distributions of both the active atoms and perturbers must be performed. In particular, for the effects described herein, the various collisional transfer rates vanish when averaged over the active atom velocity distribution. It is essential, therefore, to obtain the final line-shape formulas, including velocity-dependent collisional transfer rates, before carrying out the average over the active atom velocity distribution. The experimental observation of these spectral features would provide direct evidence for the existence of these collisional transfer processes.