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Journal of Physics B Atomic Molecular and Optical Physics

Three-photon excitation of the3P1state of krypton and of related molecular states. Spectroscopic and temporal analysis of post-luminescence

Y. Salamero, Abderrazak Kerdoussi, André Birot, Jocelyne Galy A, P. Millet

Published Oct 28, 1990• 7 citations
Publisher

Abstract

At low pressures, excitation is due to the absorption of three photons and causes emission of the resonance line and the related first continuum ( lambda approximately 125 nm). At higher pressures, excitation mainly arises from a photon of the third harmonic of the laser wave and the second continuum ( lambda approximately 148 nm) is detected. Luminescence attenuations in the excitation spectra can be explained by the absorption of a fourth photon. The natural lifetime of the 3 P 1 is determined using Holstein's theory. The role of two and three-body collisions is demonstrated in the decay of the 3 P 1 state as in the role of three-body collisions for the 3 P 2 state. The corresponding rate constants are determined and the lifetime of the 1 u ( 3 P 2 ) state evaluated.

DOI
10.1088/0953-4075/23/20/019

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At low pressures, excitation is due to the absorption of three photons and causes emission of the resonance line and the related first continuum ( lambda approximately 125 nm). At higher pressures, excitation mainly arises from a photon of the third harmonic of the laser wave and the second continuum ( lambda approximately 148 nm) is detected. Luminescence attenuations in the excitation spectra can be explained by the absorption of a fourth photon. The natural lifetime of the 3 P 1 is determined using Holstein's theory. The role of two and three-body collisions is demonstrated in the decay of the 3 P 1 state as in the role of three-body collisions for the 3 P 2 state. The corresponding rate constants are determined and the lifetime of the 1 u ( 3 P 2 ) state evaluated.
The first decay frequency, 1/r i is attributed to the Xe(3P ) ) state. In this case, 1/k i corresponds to the apparent lifetime of the resonant state (1.„ = 3.98 µs) and k51 is the 3-body rate constant of formation of the Xe[0+„ CPO] excimer. The second one, 1/T2 is attributed to the Xe(3P2) state. Then, 1/1(12 corresponds to the lifetime of the metastable state and k52 is the 3-body rate constant of formation of the Xe 1„ (3P2)] excimer. These results are in good agreement with those obtained with 3-photon selective excitation of Xeelp i ) state [3]. In both cases, no 2-body collision rate constant term is found.
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.
Neutral krypton atoms are excited from the ground state to the 4p56p[3/2]2 state by two-photon absorption from an ArF excimer laser operating at 193.41 nm. The third photon ionizes the krypton atoms. Excitation and ionization yields are theoretically computed employing the standard laser rate-equations analysis. Measurements are made on both the excitation and ionization yields. The experimental results are in good agreement with the theoretical predictions of our formulations, as well as with those of other authors.
The time-dependent theory of the three-step absorption of three different light pulses in the electronic four-level systems is considered using the time-dependent perturbation theory. The first, the second, and the third pulse are in resonance with transitions from level 0 to level 1, from level 1 to level 2, and from level 2 to level 3, respectively. The spectral and temporal behaviour of the probability that the fourth level is excited at the moment of time t depends on the energy relaxation constants of the excited electronic levels, the frequencies of the maxima, the spectral widths (and so the durations) of the light pulses, and the time delays between the pulses. To conclude, there are 12 parameters that affect the spectra in the simple model used. We calculate and analyse the case where the frequencies of the maxima of the first and the second pulse are fixed and the frequency of the maximum of the third pulse varies. On the whole, three lines may exist, one of which corresponds to the coherent contribution and the others do not.
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.
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.