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Journal de physique

High density self-broadening of the first xenon and krypton resonance line

P. Laporte, Henri Damany

Published Jan 1, 1979• 48 citations
Publisher

Abstract

Self-broadening of the 146.96 nm xenon line and 123.58 nm krypton line is studied in the density range 1-100 amagat (2.7 x 1019 — 2.7 × 1021 at. cm-3). The absorption profile is deduced from reflection experiments by a modified Kramers-Krönig analysis. A detailed discussion of the criteria for validity of available theories is given, allowing the determination of the extent to which the cases studied are related to many-body interactions and/or pure resonance forces. The quasistatic theory, in the nearest neighbour approximation, is shown to be valid for interpreting the far wings. Thus it is possible at increasing density, to underline the specific effect of the various kinds of forces : resonance, Van der Waals and repulsive, and to specify the 1u excited state potential which is found weakly attractive for Xe2 and Kr2.

DOI
10.1051/jphys:019790040010900

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Journal of Physics B Atomic and Molecular Physics•Aug 28, 1978•3 citations
Self-broadening of the 146.96 nm xenon line and 123.58 nm krypton line is studied in the density range 1-100 amagat (2.7 x 1019 — 2.7 × 1021 at. cm-3). The absorption profile is deduced from reflection experiments by a modified Kramers-Krönig analysis. A detailed discussion of the criteria for validity of available theories is given, allowing the determination of the extent to which the cases studied are related to many-body interactions and/or pure resonance forces. The quasistatic theory, in the nearest neighbour approximation, is shown to be valid for interpreting the far wings. Thus it is possible at increasing density, to underline the specific effect of the various kinds of forces : resonance, Van der Waals and repulsive, and to specify the 1u excited state potential which is found weakly attractive for Xe2 and Kr2.
Three-photon excitation and multiphoton ionization techniques have been used to measure self-broadening for several resonance lines in xenon and krypton. Tabulations of widths and shifts of the xenon lines at 146.9, 129.6, 119.2, and 117.0 nm were made for pressures between 50 and 900 Torr. Similar measurements were made for the krypton resonance line at 116.5 nm. For pressures less than 500 Torr the widths were found to be in reasonable agreement with theoretical results, which were extrapolated into regions of concentration where the criteria for their validity are at best questionable. We have also found the lines to be shifted to the high-energy side of the unperturbed line. For four of the five lines studied, the blue shifts increased nearly linearly with increasing pressure. In the four cases where the shift could be measured the ratio of shift to width was close to (1/2. Our experimental technique is very simple, but it has yielded what we believe to be the first resonance broadening data based on absorption under conditions where there is strong trapping of the resonance radiation.
Reports the results of interferometric investigation of collisional broadening and shift of the resonance line of thallium ( lambda =377.68 nm) by krypton and xenon. The measurements were performed at low density of the perturbing gases (3-53*10 16 cm -3 ) and both Doppler and collisional broadening of the line were determined. The results are compared with those calculated on the basis of the van der Waals, Lennard-Jones and Czuchaj-Sienkiewicz potentials. The measured values of the broadening and shift by krypton and xenon are lower than those computed for the van der Waals and Lennard-Jones potentials. Calculations based on realistic potentials reported by Czuchaj and Sienkiewicz give values of the broadening coefficient in good agreement with the experimental data.
Saturated-absorption profiles of the lines at lambda =557 nm involving the lowest metastable level of krypton show intense and broad Gaussian backgrounds due to thermalising collisions. These backgrounds are greatly reduced by the addition of xenon atoms which quench the metastable level. The variation of the amplitude of the background relative to the amplitude of the narrow absorption resonance versus pressure is quadratic in pure krypton and linear in mixtures of krypton and xenon. An interpretation of the results is given taking into account transit-time effects, while making use of published results for the quenching cross section.
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.