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arXiv:2304.12803 · Physical Review A

Two-photon excitation and absorption spectroscopy of gaseous and supercritical xenon

Thilo vom Hövel, Franz Huybrechts, Eric Boltersdorf, Christian Wahl, Frank Vewinger, Martin Weitz

Published Jul 28, 2023• 1 citation
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Abstract

Spectroscopy of gases under high-pressure conditions is of interest in various fields such as plasma physics and astrophysics. Recently, it has also been proposed to utilize a high-pressure noble gas environment as a thermalization medium to extend the wavelength range of photon Bose-Einstein condensates to the vacuum-ultraviolet regime, from the presently accessible visible and near-infrared spectral regimes. In this work, we report on experimental results of two-photon spectroscopy of gaseous and supercritical xenon for pressures as high as 95 bar, probing the transitions from the $5{p}^{6}$ electronic ground-state to the $5{p}^{5}6p$ and $5{p}^{5}6{p}^{\ensuremath{'}}$ excited-state configurations. Aiming at the exploration of possible pumping schemes for future vacuum-ultraviolet photon condensates, we have recorded degenerate two-photon excitation spectra of such dense xenon samples. In further measurements, we have investigated whether irradiation of an auxiliary light field can enhance the reabsorption of the emission on the second excimer continuum of xenon, which is subject to a large Stokes shift. To this end, absorption measurements have been conducted, driving the $5{p}^{6}\ensuremath{\rightarrow}5{p}^{5}6p$ two-photon transitions nondegenerately.

DOI
10.1103/physreva.108.012821

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Spectroscopy of gases under high-pressure conditions is of interest in various fields such as plasma physics and astrophysics. Recently, it has also been proposed to utilize a high-pressure noble gas environment as a thermalization medium to extend the wavelength range of photon Bose-Einstein condensates to the vacuum-ultraviolet regime, from the presently accessible visible and near-infrared spectral regimes. In this work, we report on experimental results of two-photon spectroscopy of gaseous and supercritical xenon for pressures as high as 95 bar, probing the transitions from the 5p65{p}^{6}5p6 electronic ground-state to the 5p56p5{p}^{5}6p5p56p and 5p56p\ensuremath′5{p}^{5}6{p}^{\ensuremath{'}}5p56p\ensuremath′ excited-state configurations. Aiming at the exploration of possible pumping schemes for future vacuum-ultraviolet photon condensates, we have recorded degenerate two-photon excitation spectra of such dense xenon samples. In further measurements, we have investigated whether irradiation of an auxiliary light field can enhance the reabsorption of the emission on the second excimer continuum of xenon, which is subject to a large Stokes shift. To this end, absorption measurements have been conducted, driving the 5p6\ensuremath→5p56p5{p}^{6}\ensuremath{\rightarrow}5{p}^{5}6p5p6\ensuremath→5p56p two-photon transitions nondegenerately.
Bose-Einstein condensation, an effect long known for material particles as cold atomic gases, has in recent years also been observed for photons in microscopic optical cavities. Here, we report absorption and emission spectroscopic measurements on the lowest electronic transition ($5{p}^{6}\ensuremath{\rightarrow}5{p}^{5}6s$) of xenon, motivated by the search for a thermalization medium for photon Bose-Einstein condensation in the vacuum-ultraviolet spectral regime. We have recorded pressure-broadened xenon spectra in the 135- to 190-nm wavelength regime at conditions near the critical point. The explored pressure and temperature ranges include high-pressure gaseous xenon below the critical pressure and supercritical xenon at room temperature as well as liquid xenon close to the boiling point near the critical pressure.
Between the absorption and the emission spectral lineshapes of dense atomic and molecular media, such as dye solutions and alkali-noble buffer gas mixtures at high pressure, in many cases there exists a universal scaling, the Kennard-Stepanov relation, which is a manifestation of detailed balance. This relation plays a crucial role in recent Bose-Einstein condensation experiments of visible-spectral-photons in e.g.~dye-solution-filled optical microcavities. It has recently been proposed to use high-pressure xenon-noble gas mixtures as a thermalization medium for vacuum-ultraviolet regime photons, so as to extend the achievable wavelength range of such Bose-Einstein-condensed optical sources from the visible to the vacuum-ultraviolet regime. In this work, we report two-photon excitation spectroscopy measurements of ground state (5p65p^65p6) xenon atoms subject to up to 80bar of helium or krypton buffer gas pressure, respectively, in the 220-260nm wavelength range. The study of such two-photon spectra is of interest e.g.~for the exploration of possible pumping schemes of a future vacuum-ultraviolet photon Bose-Einstein condensate. We have also recorded absorption and emission spectra of the 5p6↔5p56s5p^6 \leftrightarrow 5p^56s5p6↔5p56s single-photon transition near 147nm wavelength of xenon atoms subject to 80bar of krypton buffer gas pressure. We find that the ratio of absorption and emission shows a Kennard-Stepanov scaling, which suggests that such gas mixtures are promising candidates as a thermalization medium for a Bose-Einstein condensate of vacuum-ultraviolet photons.
Other than for the three-dimensonal case of blackbody radiation, low-dimensional photon gases can exhibit Bose- Einstein condensation, as been experimentally demonstrated in the visible spectral regime first in 2010 using a dye-filled optical microcavity [1]. Here a short, wavelength sized spacing of cavity mirrors provides a low- frequency cutoff imprinting a spectrum of photon energies restricted to well above the thermal energy, and photons thermalize by repeated absorption and (re-)emission processes on the dye molecules to room temperature. As a prominent feature, a Bose-Einstein condensate of photons is as a coherent light source. This is of special interest in the vacuum-ultraviolet spectral regime (100 nm-200 nm, VUV), as it is difficult to realize lasers in this wavelength range. This is mainly due to the1/ω31/\omega^{3}1/ω3-scaling of excited state lifetimes, which requires increasingly high pump powers at short wavelengths to create population inversion in a laser medium.
The experiment demonstrates at low pressure the resonant excitation of the 3 P 1 atomic state of xenon by three-photon absorption; as the pressure increases the xenon molecules in the ground state intervene in the absorption process. The emission spectra present the VUV continua characteristic of the excimer. In the same experimental conditions but with observation along the excitation axis, the frequency tripling phenomenon is seen close to the resonance line at 147 nm and the authors have measured new values of the phase matching parameter C Xe between 145 and 147 nm.
We describe collision studies on the two-photon excitation and fluorescence of the xenon 6p[1/2,0] excited state. Molecular nitrogen is the major collision partner. The 250-nm second harmonic of a line-narrowed Hansch-type dye laser excites the 6p state of xenon by two-photon absorption. Sample mixtures contain xenon at a partial pressure of 1 Torr and nitrogen at partial pressures of up to several hundred Torr. Time-resolved and time-integrated measurements of the intensity of the 828-nm 6p[1/2,0]—6s[3/2,1] allowed transition are obtained with photomultipliers, a transient digitizer, and a computerized data acquisition system. We extract pressure-dependent and pressure-independent components of the fluorescence lifetime and fluorescence yield from measurements over a range of nitrogen pressures. When the excitation power density is of the order of 104 W/cm2, the excited xenon atoms decay spontaneously. For spontaneous fluorescence, we obtain an inelastic (quenching) collision cross section of ~10–14 cm2 for xenon-nitrogen collisions, and a pressure-broadening coefficient of ~3 × 107 Hz/(Torr N2) for the two-photon transition rate. For excitation intensities above 2.6 × 106 W/cm2, the xenon atoms radiate cooperatively in a subnanosecond pulse. The fluorescence yield of this cooperative emission increases with nitrogen pressure rather than decreasing as in the spontaneous case. Mechanisms 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.