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Physical Review A

Isotopic shift, pressure shift, and pressure broadening of the 7d′ states of neon using Doppler-free two-photon absorption spectroscopy

M. M. Salour

Published Feb 1, 1978• 16 citations
Publisher

Abstract

Doppler-free two-photon transitions between the $3s$, $J=2$ 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.

DOI
10.1103/physreva.17.614

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Doppler-free two-photon transitions between the 3s3s3s, J=2J=2J=2 metastable state and the subconfiguration 7d\ensuremath′7{d}^{\ensuremath{'}}7d\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.
A description is given of the apparatus which represents realization of the well-known principle of cancellation of the Doppler effect in two-photon transitions. A brief review is given of the applications of the Doppler-free two-photon spectroscopy in the measurements of the fine and hyperfme structure of highly excited states, isotopic shifts, etc. Collisional broadening and spectral shift in sodium vapor mixed with various buffer gases is considered. A detailed discussion is given of the application of the Doppler-free two-photon spectroscopy to studies of transient optical processes. The method is extended to the case of many-photon transitions. A description is given of the apparatus suitable for the observation of Doppler-free three-photon transitions. Advantages and shortcomings of the new and existing methods are discussed.
Doppler-free two-photon absorption spectroscopy was applied to study highly-excited D states of Rb atoms. Using a cw dye laser as an excitation source, transitions from the ground 5S state to nd 2D states (n=11-32) were observed, the ionization energy of the highest state being only 117cm-1. These D doublets are not inverted. The fine structure splittings of these states do not vary as (neff) -3, nor as n-3. The isotope shift of the 85Rb, 87Rb ground states is found to be 160±12MHz. No pressure broadening was observed for these transitions within the instrumental resolution of 15 MHz.
The spectral profile of the strongly resonance-broadened transition lambda 585.2 nm of Ne I has been studied in absorption. A narrow-band tunable dye laser probed a weak discharge in natural neon cooled with liquid nitrogen. The Lorentzian width extrapolated to zero density was found to be 108+or-20 MHz, consistent with the value 114+or-4 MHz calculated from the natural widths of the levels. There is no indication of the excess width found in earlier emission experiments in helium and neon. A preliminary result of (1.7+or-0.2)10 -21 MHz atom -1 m 3 was obtained for the broadening constant of lambda 585.2 nm in absorption at 77K. This is consistent with the value found in emission.
Broadening and shift rates for Rb 2S^{2}\mathrm{S}2S and 2D^{2}\mathrm{D}2D Rydberg states with principal quantum number n\ensuremath{\sim}10--50 have been measured for Ne, Kr, and H2{\mathrm{H}}_{2}H2​ perturbers, using the technique of Doppler-free two-photon spectroscopy. From the shift rates at high n, we derived electron scattering lengths of (0.24\ifmmode\pm\else\textpm\fi{}0.01)a0{a}_{0}a0​ for Ne, (-4.0\ifmmode\pm\else\textpm\fi{}0.3)a0{a}_{0}a0​ for Kr, and (1.64\ifmmode\pm\else\textpm\fi{}0.07)a0{a}_{0}a0​ for H2{\mathrm{H}}_{2}H2​. For Ne and Kr, these are in good agreement with other experimental values. Also, the n dependence of broadening and shift rates follows theoretical predictions for Ne and Kr, but not for H2{\mathrm{H}}_{2}H2​.