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Journal of Physics B Atomic Molecular and Optical Physics

Foreign gas pressure broadening and shifts of the 2S–4S two-photon transition in lithium

W. DeGraffenreid, Sarah C Campbell, Craig J. Sansonetti

Published May 7, 2003• 7 citations
Publisher

Abstract

We have observed broadening and shift of the 2S–4S Doppler-free two-photon transition of atomic Li by collisions with neon and argon buffer gases in a heat-pipe oven. Measured broadening and shift rates are presented and compared with theoretical predictions calculated in the impact approximation using three different interaction potentials. A superposition of polarization and modified Fermi potentials gives good agreement with the experimental data.

DOI
10.1088/0953-4075/36/10/318

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We have observed broadening and shift of the 2S–4S Doppler-free two-photon transition of atomic Li by collisions with neon and argon buffer gases in a heat-pipe oven. Measured broadening and shift rates are presented and compared with theoretical predictions calculated in the impact approximation using three different interaction potentials. A superposition of polarization and modified Fermi potentials gives good agreement with the experimental data.
Our recent treatment [Phys. Rev. A 18, 1066 (1978)] of the broadening and shift of alkali-metal-atom two-photon $S\ensuremath{-}S$ transitions is applied to the Na $3S\ensuremath{-}\mathrm{nS}$ transitions ($n=6\ensuremath{-}9$) perturbed by Ar, Kr, and Xe rare gases. Comparison with recent experimental data [A. Flusberg et al., Phys. Rev. A 19, 1607 (1979)] on the Na-Ar pair for $n\ensuremath{\le}7$ shows good agreement. However, for transitions to n>8n>8n>8 the calculated pressure effects no longer agree well with experimental data; presumably the pressure effects cannot be adequately described by a simple two-body long-range impact theory.
The broadening and shift of two-photon $S\ensuremath{-}S$ transitions (e.g., in alkali-metal atoms perturbed by rare gases) are shown to be readily calculable. These calculations employ (a) newly available expressions for alkalimetal-rare-gas long-range potential coefficients C6{C}_{6}C6​, C8{C}_{8}C8​, and C10{C}_{10}C10​; and (b) the (herein discussed) appropriate form of impact theory (particularly simple since only a single potential curve is involved and inelastic processes are not usually important). It is demonstrated in particular that the influence of C8{C}_{8}C8​ and C10{C}_{10}C10​ terms on the broadening and shift is significant though not dominant. Comparison with recent experimental data on the Na-rare-gas pairs shows reasonable agreement for the heavy rare gases.
Doppler free two photon absorption spectroscopy was employed to measure the pressure broadening and frequency shift rates of the 5S1/2 (F = 3) → 5D5/2 (F = 5, 4, 3, 2, 1) (778.105 nm) and the 5S1/2 (F = 2) → 7S1/2 (F = 2) (760.126 nm) two photon transitions in 85Rb by the noble gases and N2. To our knowledge, these rates are reported on for the first time. The self-broadening and shift rate of the 5S1/2 (F = 3) → 5D5/2 (F = 5, 4, 3, 2, 1) transition and self -broadening rate of the 5S1/2 (F = 2) → 7S1/2 (F = 2) transition were also measured. The temperature dependence of the self-frequency shift (Rb-Rb collisions) of these transitions is presented. Helium diffusion rates through Quartz and Pyrex cells are also calculated and the implication of helium diffusion through glass vapor cells is discussed in regards to atomic frequency standards based on these transitions. Experimental pressure broadening and shift rates are compared to theoretically calculated rates assuming a 6, 8 or 6, 8, 10 difference potential and pseudo potential model. Reasonable agreement is achieved between experimental and theoretical values.
The experiment of Liran, Levin, Erez, and Jortner is clearly very interesting. Nevertheless, we feel that the numerical values which has been found for the broadening of the sodium $3S\ensuremath{-}4D$ two-photon transition by collisions with argon atoms is wrong. Using Doppler-free two-photon spectroscopy we have measured this cross-section to be 1050\ifmmode\pm\else\textpm\fi{}110 A˚2{\mathrm{\AA{}}}^{2}A˚2. This value is in good agreement with other experiments and with theoretical predictions. We present several possible interpretations of the value obtained by Liran et al.
We apply two-photon resonant nondegenerate four-wave mixing with a resonant intermediate state for observing the broadening and the shifting of the barium Rydberg 6snd 1D2 series by collision with argon. The collision broadenings and the collision shifting cross sections are measured for n=1633. This technique is a purely optical means, and can achieve Doppler-free resolution of narrow spectral structures of Rydberg levels when the incident lasers have narrow bandwidths. Different from other experimental methods of studying the pressure dependence of the longitudinal relaxation rate of Rydberg states, our method is to investigate the pressure dependence of the transverse relaxation rate of the transition.
Doppler-free two-photon transitions between the 3s3s3s, J=2J=2J=2 metastable state and the subconfiguration $7{d}^{\ensuremath{'}}$ of neon are studied with a pulsed-dye-laser oscillator-amplifier system which was synchronized with a chopped rf discharge in neon vapor. The isotopic shifts for these transitions are measured, and based on these measurements we have made a systematic study of Ne-Ne and Ne-He collisional broadening and shift of these very narrow Doppler-free two-photon resonances.