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Physical Review

Broadening and Shift of the Second Doublet of the Rubidium Absorption Series Under Different Pressures of Argon and Helium

Shang-Yi Ch'en, D. Kohler

Published Jun 15, 1953• 8 citations
Publisher

Abstract

The shift and broadening of the second doublet of the principal series of rubidium produced by argon and by helium were studied for pressures up to 123.5 atmospheres (rd 52) and up to 97.5 atmospheres (rd 44), respectively. The red shift produced by argon gives a linear relationship with its relative density, rd. The slopes for both components of the doublet are 2.95 ${\mathrm{cm}}^{\ensuremath{-}1}$/rd. The violet shift produced by helium in the high pressure range is greater than linear with the rd. The $^{2}P_{\frac{1}{2}}$ component is shifted more than the $^{2}P_{\frac{3}{2}}$ component.Argon shows a nicely linear broadening for both components over the entire range of rd. For the $^{2}P_{\frac{3}{2}}$ component the broadening is 2.28 ${\mathrm{cm}}^{\ensuremath{-}1}$/rd and for the $^{2}P_{\frac{1}{2}}$ component it is 2.11 ${\mathrm{cm}}^{\ensuremath{-}1}$/rd. Helium appears to give a definite quadratic broadening, particularly for the $^{2}P_{\frac{3}{2}}$ component.

DOI
10.1103/physrev.90.1019

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The Journal of Chemical Physics•Jun 1, 1959•42 citations
The shift and broadening of the second doublet of the principal series of rubidium produced by argon and by helium were studied for pressures up to 123.5 atmospheres (rd 52) and up to 97.5 atmospheres (rd 44), respectively. The red shift produced by argon gives a linear relationship with its relative density, rd. The slopes for both components of the doublet are 2.95 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1/rd. The violet shift produced by helium in the high pressure range is greater than linear with the rd. The 2P12^{2}P_{\frac{1}{2}}2P21​​ component is shifted more than the 2P32^{2}P_{\frac{3}{2}}2P23​​ component.Argon shows a nicely linear broadening for both components over the entire range of rd. For the 2P32^{2}P_{\frac{3}{2}}2P23​​ component the broadening is 2.28 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1/rd and for the 2P12^{2}P_{\frac{1}{2}}2P21​​ component it is 2.11 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}cm\ensuremath−1/rd. Helium appears to give a definite quadratic broadening, particularly for the 2P32^{2}P_{\frac{3}{2}}2P23​​ component.
The displacement, asymmetry, and broadening of the second doublet of the rubidium principal series perturbed by pure helium, neon and argon up to 13 atmospheres are observed. The displacement as well as the broadening of the doublet components are not the same. The 2P12^{2}P_{\frac{1}{2}}2P21​​ component shifts and broadens more conspicuously than the 2P112^{2}P_{1\frac{1}{2}}2P121​​ component (an exception being the broadening by argon). The departure from linear relationship between the shift and the density of the perturbing gas is quite manifest. Both for helium and for neon the line contour shows a distinct asymmetry towards the violet, while for argon the line contour shows a very strong red asymmetry. For helium and neon the violet asymmetries of the 2P12^{2}P_{\frac{1}{2}}2P21​​ component are stronger than that of the 2P112^{2}P_{1\frac{1}{2}}2P121​​ component; the reverse is true for argon. The relationship between the half-width and the relative density is linear for foreign gas concentrations of relative densities up to 8 so far applied.
We present results of the pressure broadening and shift of the rubidium 5s2S1∕2–6p2P3∕25s\phantom{\rule{0.2em}{0ex}}^{2}S_{1∕2}\text{--}6p\phantom{\rule{0.2em}{0ex}}^{2}P_{3∕2}5s2S1∕2​–6p2P3∕2​ (420.2 nm) spectral line by argon and helium buffer gases at pressures below 10 torr. High-resolution absorption measurements were performed with a single-mode external cavity diode laser, having 20-GHz tuning range and a linewidth of about 1 MHz. Pressure broadening and shift parameters of Lorentzian hyperfine components have been determined. We obtained the redshift of hyperfine spectral lines for He and the blueshift for Ar.
The broadening of the resonance lines of rubidium in absorption under pressures up to 150 mm of its own homogeneous vapor was studied by means of a 21-foot grating. Under pressures below 1 mm the broadening of the lines was very symmetrical and the line contours could be described by the dispersion formula, but when the pressure was high the lines exhibited asymmetrical broadening of van der Waals type. The 2P12^{2}P_{\frac{1}{2}}2P21​​ component showed red, while the 2P32^{2}P_{\frac{3}{2}}2P23​​ component showed violet asymmetry. Both lines showed the proportionality of the width with NNN, the concentration of Rb atoms. The experimental width at half-maximum is greater than that predicted by Houston's theory by a factor of 1.5 and the width of the transition from 3P32^{3}P_{\frac{3}{2}}3P23​​ is greater than that from 3P12^{3}P_{\frac{1}{2}}3P21​​ by a factor of 1.6. A narrow diffuse band was observed near the shorter wave-length side of the 2P12^{2}P_{\frac{1}{2}}2P21​​ component and a similar one near the longer wave-length side of the 2P32^{2}P_{\frac{3}{2}}2P23​​ component.
In the presence of heavy foreign gases, such as Kr and Xe, diffused absorption bands were observed at both the short wavelength and the long wavelength side of the first four absorption doublets of the Rb principal series. The red bands were observable when the Rb vapor pressure in the absorption tube was relatively low (10−3 to 10−2 mm Hg). The violet bands were not intense enough until the Rb vapor pressure was increased to 0.1–1 mm Hg. With other lighter gases (H2, He, Ne, A, N2) only violet bands were observed. The positions and the absorption contours of the bands in relation to the member of the absorption series and to the nature of the foreign gases are discussed.
Spectroscopy of alkali-metal--buffer-gas mixtures at high pressures from single-digit to several hundred bars in the regime of substantial collisional broadening is relevant in a wide range of fields, ranging from collisional redistribution cooling to laboratory astrophysics. Here we report on spectroscopic measurements of dense rubidium--noble-gas mixtures recorded in a pressure cell equipped with soldered sapphire optical viewports, which allows for the controlled realization of extreme conditions of high temperature and high pressure in a table top laboratory experiment. In the gas cell, we have recorded absorption and emission spectra of rubidium subject to 188 bars of helium buffer-gas pressure at 548-K temperature. The spectra to good accuracy follow a Boltzmann-type Kennard-Stepanov frequency scaling of the ratio of absorption and emission spectral profiles. Further, the long optical path length in the cell allowed us to both record spectra of rubidium-argon mixtures at moderate temperatures and high pressures and observe redistributional laser cooling in this system.
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.