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Physical Review Letters

Observation of the Simultaneous Additive Effect of Several Xenon Perturbers on the Cs 6s−9p Doublet

John F. Kielkopf, N. F. Allard

Published Jul 16, 1979• 31 citations
Publisher

Abstract

Multiple satellites appear in absorption spectra on both components of the Cs $6s\ensuremath{-}9p$ doublet perturbed by xenon at densities of the order of ${10}^{19}$ atoms/${\mathrm{cm}}^{3}$. The profiles of these perturbed lines computed with the Anderson-Talman theory, and the density dependence of the absorption at the multiple satellite frequencies, definitely identify the origin of the satellites as the combined additive effect of one to four perturbers.

DOI
10.1103/physrevlett.43.196

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arXiv:quant-ph/9803043•Mar 17, 1998•0 citations
Multiple satellites appear in absorption spectra on both components of the Cs 6s\ensuremath−9p6s\ensuremath{-}9p6s\ensuremath−9p doublet perturbed by xenon at densities of the order of 1019{10}^{19}1019 atoms/cm3{\mathrm{cm}}^{3}cm3. The profiles of these perturbed lines computed with the Anderson-Talman theory, and the density dependence of the absorption at the multiple satellite frequencies, definitely identify the origin of the satellites as the combined additive effect of one to four perturbers.
The fluorescent spectra of the Cs principal series lines 4555 and 4593 AA (72P32,1/2/-62S12/) broadened by Kr and Xe were measured up to perturber gas densities of about 4.9*1019 cm-3. In addition, the absorption spectra of the Cs principal series line 3876 AA (62S12/-82P32/) broadened by Xe (1.63*1018<or=NX3<or=1.9*1019 cm-3) were investigated. The existence of secondary satellites was established. The intensity dependence of the quasistatic wings is discussed and qualitatively explained by competitive additive two- and three-body interactions.
An experimental study of the additivity of the phase shift or perturbation energies produced by foreign-gas perturbers in collision with an optical atom is made by measuring the shift and the half-width of the second to the seventh doublet of the Cs absorption series, under various pressures and with various concentration ratios of a mixture of He and Ar. The shift produced by the mixture is found to be about the average of the shifts of the separate gases. The broadening of the fourth absorption doublet of Cs produced by the mixture of He and Ar is about 34\frac{3}{4}43​ of the sum of broadenings due to the constituents.
Experiments have revealed that pressures of noble gases cause bands to appear in both the red and violet wings of the alkali doublet lines. The present paper is devoted to the explanation of these bands and to the shift and shape of the doublet lines which they accompany. In order to examine various qualitative proposals previously put forth to this end, we first ascertain the validity of the statistical theory as applied to the magnetic substates of the alkali resonance lines and develop a criterion for adiabaticity. This criterion indicates that the earlier theories are inadequate. Shift and broadening of the two components of the alkali doublet lines are then calculated as functions of noble gas density by considering the van der Waals energy perturbation due to n simultaneously acting perturbers. The conclusion, which is in agreement with experiments, is that the P322 resonance line is shifted and broadened more than the 2P½ resonance line at moderate pressures. A phenomenological approach is used to construct a more reasonable theory of the ``satellite'' bands. In the absence of reliable knowledge concerning the repulsive portions of the interaction curves, only a semiquantitative understanding of the data is achieved.
Observation of the time-dependence of excitation transfer between Cs 7p 2P1/2 and 2P3/2 levels caused by collisions with xenon are reported. The 2P levels were selectively excited with an N2 laser-pumped dye laser, and the spectrum of the fluorescence radiation was observed with 5 nsec time resolution. The lifetimes of the levels were found to be (2P1/2) 154±2 nsec and (2P3/2) 135±2 nsec, and the 2P1/2 to 2P3/2 transfer cross section at 325±10 °K is 0.150±0.002 Å2. An analysis of the time-dependent decay versus xenon partial pressure shows that the cross section for quenching or collision induced radiation is less than 4×10−3 Å2. This demonstrates that collision induced transitions cannot be important in the formation of near red satellites on the Cs 6s–7p lines perturbed by Xe. In addition, the radiative decay constant for the satellite is identical to that for the line within experimental uncertainty. The correspondence of satellite and line decay curves provides a method of identifying satellites with their parent line.
Rabi frequencies for multiphoton absorption by atoms or molecules that can be characterized as two- or three-level systems are obtained in the cases of single and double laser perturbations. If the ambiguity in the origin of absolute energy is conveniently gauged off in the three-level model, there appears an additional non linear frequency which is originated from the separate evolution of a relative-frequency component induced in the whole system by the simultaneous action of the two perturbations.