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Physical Review Letters

Intermediate and Wannier Excitons in Fluid Xenon

P. Laporte, J. L. Subtil, Uri Asaf, I. T. Steinberger, Shalom J. Wind

Published Dec 29, 1980• 41 citations
Publisher

Abstract

Reflectivity spectra of Mg${\mathrm{F}}_{2}$---fluid-xenon interfaces obtained for a wide range of densities revealed that the $n=2$ Wannier exciton starts to appear at densities above 400 amagat (1 amagat of density for xenon corresponds to 2.7067\ifmmode\times\else\texttimes\fi{}${10}^{19}$ atoms/${\mathrm{cm}}^{3}$). The ${n}^{\ensuremath{'}}=1$ exciton appears at densities above about 100 amagats on the low-energy side of the parent $5{p}^{5}6s$ [$K=\frac{1}{2}$] atomic state. The occurrence and evolution of these bands and of the previously reported $n=1$ band with density are discussed with use of conductivity relaxation times obtained by Huang and Freeman.

DOI
10.1103/physrevlett.45.2138

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Reflectivity spectra of MgF2{\mathrm{F}}_{2}F2​---fluid-xenon interfaces obtained for a wide range of densities revealed that the n=2n=2n=2 Wannier exciton starts to appear at densities above 400 amagat (1 amagat of density for xenon corresponds to 2.7067\ifmmode\times\else\texttimes\fi{}1019{10}^{19}1019 atoms/cm3{\mathrm{cm}}^{3}cm3). The n\ensuremath′=1{n}^{\ensuremath{'}}=1n\ensuremath′=1 exciton appears at densities above about 100 amagats on the low-energy side of the parent 5p56s5{p}^{5}6s5p56s [K=12K=\frac{1}{2}K=21​] atomic state. The occurrence and evolution of these bands and of the previously reported n=1n=1n=1 band with density are discussed with use of conductivity relaxation times obtained by Huang and Freeman.
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.
We present the method by which we can describe the many exciton system transparently by making the best use of the boson like character of Wannier excitons. Basing upon this method, the total energy of this system and the number of bose-condensed excitons are calculated as a function of the total concentration of excitons, and we show how the boson like character of Wannier excitons is reflected on the emission spectrum from this system and on the absorption spectrum in the presence of these excitons at finite density.
The kinetics of formation and decay of Cs-Xe molecules in their $\ensuremath{\Sigma}$ and $\ensuremath{\Pi}$ bound states produced in Cs-Xe mixtures irradiated with a short-pulse dye laser tuned around the $7P\ensuremath{-}6S \mathrm{Cs}$ resonance transition has been investigated by fluorescence decay measurements. The time-resolved spectra of the 4600- and 5720-\AA{} molecular fluorescent bands were studied in relation to xenon density, which ranged from 0.9 to 6.9 amagats. Quantitative collisional cross sections are derived from the measured transition rates with peak values around ${10}^{\ensuremath{-}17}$ cm2{\mathrm{cm}}^{2}cm2.