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Annual Meeting Optical Society of America

Collisional effects on xenon 6p fluorescence

M. Rankin, Jon P. Davis, Christopher Giranda, Lloyd C. Bobb

Published Jan 1, 1986• 0 citations
Publisher

Abstract

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.

DOI
10.1364/oam.1986.thj11

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Physical Review A•Feb 1, 1990•34 citations
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.
Excitation of xenon near the two-photon resonance between the ground state and the 6p(1/2,0) state produces forward conical emission at a wavelength close to the 828-nm 6p(1/2,0)—6s(3/ 2,1) excited-state transition. We describe experimental features of this process as excited by 600-ps pulses of 250-nm radiation from a frequency-doubled dye laser with intensity up to 1.3 × 108 W/ cm2 in xenon at pressures of 1-20 Torr. The conical emission occurs most prominently when the driving field is a few gigahertz above the frequency at which spontaneous emission from the excited 6p state peaks. The cone angle increases with xenon pressure in the 1-10-Torr range. The dependence appears consistent with the predictions based on noncollinearly phase-matched four-wave mixing. In this interpretation, the fourth wave would be near resonance with the 146.9-nm first resonance transition of xenon and detuned to the low-frequency side. The conical emission co-exists (and may compete with) an axial stimulated process which may be either two-photon driven amplified spontaneous emission or stimulated hyper-Raman scattering. The different tuning characteristics for the two processes make the extent of their competition unclear.
The destruction rates of the xenon $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{0}$ metastable and $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{1}$ resonance atoms by collisions with ground-state xenon atoms have been measured by studying the temporal dependence of the number densities of the $6{s}^{\ensuremath{'}}$ and 6p6p6p atoms. The studies have been made both during the earlier afterglow of a xenon pulsed discharge and after the selective production of the $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{0,1}$ atoms by a laser excitation in the late afterglow. An original optical pumping technique, using a tunable pulsed dye laser, was employed to populate the $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{0,1}$ levels by excitation of the 6s[32]26s{[\frac{3}{2}]}_{2}6s[23​]2​ long-lived metastable atoms to $6{p}^{\ensuremath{'}}$ levels. The pressure dependence of the decay frequencies of these $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{0,1}$ atoms was analyzed in the xenon pressure range of 0.04 to 1 torr and a kinetic model describing the evolution of the densities of these atoms after their production was established. The rate coefficients for the relaxation of the $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{0}$ metastable and $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{1}$ resonance atoms by two-body collisions involving a ground-state xenon atom are (8.45\ifmmode\pm\else\textpm\fi{}0.85) \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}12}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{sec}}^{\ensuremath{-}1}$ and (6.65 \ifmmode\pm\else\textpm\fi{} 1.00) \ifmmode\times\else\texttimes\fi{} ${10}^{\ensuremath{-}11}$ cm3{\mathrm{cm}}^{3}cm3 ${\mathrm{sec}}^{\ensuremath{-}1}$, respectively. Results show that, in fact, at least 75% of this relaxation is a transfer of population to the 6p[12]16p{[\frac{1}{2}]}_{1}6p[21​]1​ level following ${\mathrm{Xe}}^{*}(6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{0,1})+\mathrm{Xe}\ensuremath{\rightleftarrows}{\mathrm{Xe}}^{*}(6p{[\frac{1}{2}]}_{1})+\mathrm{Xe}\ensuremath{-}\ensuremath{\Delta}E$. These collisional transfer processes have been explained by means of Mulliken's xenon molecular potential curves.
Observation of the time-dependence of excitation transfer between Cs 7p 2P1/2 and 2P3/2 levels caused by collisions with xenon are reported. The 2P levels were selectively excited with an N2 laser-pumped dye laser, and the spectrum of the fluorescence radiation was observed with 5 nsec time resolution. The lifetimes of the levels were found to be (2P1/2) 154±2 nsec and (2P3/2) 135±2 nsec, and the 2P1/2 to 2P3/2 transfer cross section at 325±10 °K is 0.150±0.002 Å2. An analysis of the time-dependent decay versus xenon partial pressure shows that the cross section for quenching or collision induced radiation is less than 4×10−3 Å2. This demonstrates that collision induced transitions cannot be important in the formation of near red satellites on the Cs 6s–7p lines perturbed by Xe. In addition, the radiative decay constant for the satellite is identical to that for the line within experimental uncertainty. The correspondence of satellite and line decay curves provides a method of identifying satellites with their parent line.
A pressure-broadening study of three-photon and one-photon resonances was performed using counterpropagating, linearly polarized laser beams. Self-broadening, as well as the collision-induced effects due to the presence of a second noble gas, was investigated for the 6s, 6s′, 5d and 7s of xenon and the 5s′ of krypton. A multiphoton ionization scheme in a calibrated proportional counter is the basis of a new technique by which collisional processes can be investigated for high pressure regimes which have previously been inaccessible to investigation, particularly for self-broadening where the mean free path of the photons is of the order of 10−3 cm for pressures as low as 1 Torr. Using this technique, we have recorded the collision-induced widths and shifts of the resonance for pressures up to 1000 Torr. In the hundreds of torr range, asymmetric, self-broadening line shapes were observed with full widths and shifts which were greater than five times the laser bandwidth (0.002-0.005 nm).
Two-photon absorption cross sections of ground-state xenon atoms to the 2p5{p}_{5}p5​(J=0), 2p6{p}_{6}p6​(J=2), and 2p9{p}_{9}p9​(J=2) states in the 5${p}^{5}6pconfigurationandphotoionizationcrosssectionsat193and248nmfromthe26p configuration and photoionization cross sections at 193 and 248 nm from the 26pconfigurationandphotoionizationcrosssectionsat193and248nmfromthe2{p}_{5}$ and 2p6{p}_{6}p6​ states have been determined and are compared with previous experimental and theoretical values where such exist. Fluorescence depletion spectroscopy as a method for determining excited-state photoionization cross sections is described and discussed and shown to have many attractive features. Based on our cross-section measurements, we calculate that (2+1)-photon photoionization in Xe with a laser intensity of 30 MW/cm2{\mathrm{cm}}^{2}cm2 during 25 ns at 249.6 nm, using the 2p5{p}_{5}p5​(J=0) state as an intermediate state, can produce a fractional ionization of 10%.