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Journal of the Optical Society of America

Emission and absorption measurements of the anomalous cesium principal-series doublet oscillator-strength ratios

O Chun-Sing, Gabor F. Fulop, Olav Redi, H. Henry Stroke

Published Sep 1, 1981• 7 citations
Publisher

Abstract

The doublet oscillator-strength ratios ρn of the cesium principal series (62S1/2−n2P3/2,1/2) have been measured for principal quantum number n = 7–21. Both emission and absorption spectroscopic measurements were performed with a 9.1-m focal-length spectrometer. The results show that ρn increases monotonically with n. Discrepancies between emission and absorption results are attributed to collisional mixing of the excited-state populations. Oscillator strengths of both fine structure lines were obtained from the absorption measurements. These agree substantially with similar work by Lorenzen and Niemax [ J. Phys. B11, L723 ( 1978)]. Fano X parameters derived from the measured results are found to decrease monotonically with n. The value of X, extrapolated to the ionization potential, is 2.05 ± 0.03, in good agreement with recent laser-excited atomic-beam results of Raimond et al. [ J. Phys. B11, L765 ( 1978)]. This makes unlikely the existence of a pole of ρn in the discrete spectrum, which requires that X have the value 2.

DOI
10.1364/josa.71.001072

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Physical Review•Sep 5, 1968•55 citations
The doublet oscillator-strength ratios ρn of the cesium principal series (62S1/2−n2P3/2,1/2) have been measured for principal quantum number n = 7–21. Both emission and absorption spectroscopic measurements were performed with a 9.1-m focal-length spectrometer. The results show that ρn increases monotonically with n. Discrepancies between emission and absorption results are attributed to collisional mixing of the excited-state populations. Oscillator strengths of both fine structure lines were obtained from the absorption measurements. These agree substantially with similar work by Lorenzen and Niemax [ J. Phys. B11, L723 ( 1978)]. Fano X parameters derived from the measured results are found to decrease monotonically with n. The value of X, extrapolated to the ionization potential, is 2.05 ± 0.03, in good agreement with recent laser-excited atomic-beam results of Raimond et al. [ J. Phys. B11, L765 ( 1978)]. This makes unlikely the existence of a pole of ρn in the discrete spectrum, which requires that X have the value 2.
The oscillator strengths of the principal series doublets of Rb 5 2 S 1/2 -n 2 P 3/2 and 5 2 S 1/2 -n 2 P 1/2 (6<or=n<or=20) have been measured in absorption using a high-resolution spectrometer. The absolute f values and the ratios of the doublet components rho =f 3/2 /f 1/2 are compared with available theoretical and other experimental results. At n=15 a pronounced perturbation in the monotonic increase of the oscillator strength ratio rho as a function of the principal quantum number n is found.
Space-charge amplification of the indirect ionization resulting from photoabsorption in cesium vapor has been shown to offer to conventional techniques of absorption spectroscopy a useful complement of highest sensitivity. It was used in this work together with a xenon continuum source filtered to a linewidth of 0.14 \AA{} to measure the relative absorption probabilities for transitions of the cesium-principal-series ($6^{2}S\ensuremath{-}n^{2}P_{\frac{1}{2},\frac{3}{2}}$) doublets. Anomalous pressure effects on the resulting line-strength ratios, resulting in part from polarization molecules of Cs2{\mathrm{Cs}}_{2}Cs2​*, were examined over a range of cesium-atom concentration varying from 1.2\ifmmode\times\else\texttimes\fi{}1014{10}^{14}1014 to 1.5\ifmmode\times\else\texttimes\fi{}1015{10}^{15}1015 ${\mathrm{cm}}^{\ensuremath{-}3}$. From the corrected doublet line-strength ratios for $11\ensuremath{\le}n\ensuremath{\le}16$, the segment of the curve of Fano XXX parameters corresponding to discrete energies was constructed. Interpolation between these results and those from electron-polarization experiments served to locate the pole in the principal-series, doublet line-strength ratio near 192P19^{2}P192P.
Recent absorption measurements of the self-broadening of Rb principal series lines [C. H. Greene, E. L. Hamilton, H. Crowell, C. Vadla, and K. Niemax, Phys. Rev. Lett. 97, 233002 (2006)] verified the existence of minima in highly excited long-range potentials of Rb2{\text{Rb}}_{2}Rb2​ which were predicted theoretically as bound Rydberg molecule [C. H. Greene, A. S. Dickinson, and H. R. Sadeghpour, Phys. Rev. Lett. 85, 2458 (2000)]. The present paper reports on the extension of these experimental studies to principal series lines of K broadened by K as well as Cs broadened by Cs. In addition, the broadening of some lower members of the K, Rb, and Cs principal line series due to heteroatomic interactions was investigated. The analysis of the measured satellite structures in the quasistatic line wings and their comparison to the previously published analogous data for ${\text{Rb}}^{\ensuremath{\ast}}+\text{Rb}$ system lead to the conclusion that one can expect existence of potential minima in homo- and heteroatomic alkali-metal ${A}^{\ensuremath{\ast}}+B$ systems in a wide range of principal quantum numbers, starting with K, Rb, and Cs excited to the third resonance states. The positions and strengths of the satellite structures indicate that the potential minima are due to scattering of the valence electron by ground-state perturbers.
Oscillator strengths f3/2n and f1/2 n for the principal series of rubidium are calculated using relativistic wave functions obtained by means of the relativistic parametric-potential method. Three different approaches are used pointing out that the separation between relativistic and correlation effects is not unique and somewhat arbitrary. The calculations were carried out up to the principal quantum number n = 80 showing that the ratio Rn = f3/2n / f1/2 n increases rapidly with n towards a limiting value, a result in agreement with a recent experiment on highly excited Rydberg states.
Absorption profiles of cesium resonance lines at 8521 and 8944 \AA{} have been measured for the wavelength range from 0.5 to 30 \AA{} from the line centers using a tungsten ribbon light source, cell lengths LLL from 0.31 to 6.1 cm, and Cs densities NNN from 2 \ifmmode\times\else\texttimes\fi{} 1014{10}^{14}1014 to 2 \ifmmode\times\else\texttimes\fi{} 1016{10}^{16}1016 ${\mathrm{cm}}^{\ensuremath{-}3}$. The wavelength dependence of the absorption coefficients are consistent with a Lorentzian form and values of $\frac{\ensuremath{\gamma}f}{N}=1.08\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}7}$ and 0.30 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}7}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{sec}}^{\ensuremath{-}1}$ are obtained for 8521 and 8944 \AA{} lines. Here $\ensuremath{\gamma}$ is the collisional (or Lorentzian) half-width and fff is the oscillator strength. The values of $\frac{\ensuremath{\gamma}f}{N}$ deduced from total fractional absorption data agree with those determined from the line profiles. Our results agree well (to within 15%) with those of Gregory and with theory, but disagree with more recent data. A source of error in some previous determinations of half-widths is the fact that even when the calculated absorption is very large, the measured transmission at the line center is significant; about 3.5 \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}2}$ compared to \ensuremath{\sim} ${10}^{\ensuremath{-}100,000}$ predicted from our measurements in the wings of the lines for $N=1.14\ifmmode\times\else\texttimes\fi{}{10}^{15}$ ${\mathrm{cm}}^{\ensuremath{-}3}$ and L=5.9L=5.9L=5.9 cm. This effect is shown to result from transmission through the monochromator at wavelengths in the far wings of the instrument function.