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Physical Review A

High-density resonant shift of atomic lines of krypton and xenon in the wavelength range 118-150 nm

P. Laporte, Nicole Damany, Henri Damany

Published Nov 1, 1975• 4 citations
Publisher

Abstract

Absorption spectra of high-density pure krypton and xenon gases, in the wavelength range 118-150 nm and the density range 1-80 amagat, exhibit a red shift of all the atomic lines. The shifts are interpreted by taking into account the high-density interactions with the help of the local field correction of Lorentz introduced in classical dispersion theory.

DOI
10.1103/physreva.12.1944

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Annual Meeting Optical Society of America•Jan 1, 1990•0 citations
Absorption spectra of high-density pure krypton and xenon gases, in the wavelength range 118-150 nm and the density range 1-80 amagat, exhibit a red shift of all the atomic lines. The shifts are interpreted by taking into account the high-density interactions with the help of the local field correction of Lorentz introduced in classical dispersion theory.
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.
The resonance broadening of a transition between two excited states of a radiator in a high density gas is investigated. The important many body shielding contributions are included to all orders, and the two body correlations for the close collisions are approximately taken into account. Corrections to the line width and shift at moderately high densities are calculated. The results agree with the experimental data for krypton. The density dependence of the width parameter is examined at very high densities also. It is found that this parameter, after reaching a peak value, decreases with further increase in the density. Moreover, the square root dependence of the line widths on the density is not valid over any extended range of gas densities.
Reflection spectra of homogeneous fluid xenon are presented for the wavelength region $115<\ensuremath{\lambda}<165$ nm and densities ranging from that near the critical point to that at the triple point. For each atomic line in this spectral region two bands are observed: one broadened and somewhat shifted band corresponding to the atomic transition, and another distinct band corresponding in position to that of the exciton observed in the triple-point liquid. Dispersion analysis of the two (atomic and excitonic) 3P1^{3}P_{1}3P1​ bands yielded the optical constants ${\ensuremath{\epsilon}}^{\ensuremath{'}}$, ${\ensuremath{\epsilon}}^{\ensuremath{'}\ensuremath{'}}$, nnn, and kkk as a function of photon energy as well as parameters of the absorption bands. The results are interpreted in terms of exciton transitions appearing in momentary clusters of the fluid. The analysis of the parameters of the absorption bands was compared with the statistical fluctuations of the fluid density. It was estimated from this comparison that the 3P1^{3}P_{1}3P1​ exciton can be formed in a momentary cluster of atoms provided two conditions are fulfilled: the cluster has at least the volume of 1.5\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}21}$ cm3{\mathrm{cm}}^{3}cm3 and contains at least ten atoms.
The Lorentz-Lorenz equation predicts that the dispersion feature of an isolated optical resonance should have a density-dependent frequency shift toward the red end of the spectrum. We have investigated the dispersion feature experimentally by observing the frequency dependence of the Fresnel reflection (selective reflection) from the boundary between a dense atomic potassium vapor and the window of the vessel containing the vapor. We find that the selective-reflection features of both the S1/2-P1/2 (770.1 nm) and S1/2-P3/2 (766.7 nm) lines of potassium shift increasingly toward the red and broaden as the number density of the vapor is increased to 2 × 1017 atoms/cm3. We compare the results of the experiment to theoretical predictions for the selective reflection. The broadening is well described by conventional binary collision theory; however, the observed red shift of both of the lines is somewhat larger than that predicted by the Lorentz-Lorenz equation. It is possible that other mechanisms that lead to frequency shifts are occurring.