Irradiance values have been measured for the onset of laser-induced plasma formation in Xe, Ar, N(2), and O(2) at pressures from 760 to 25 Torr at wavelengths of 1.064, 0.532, 0.355, and 0.266 microm. These values have been compared with the results of other workers who used similar experimental setups. There is agreement within a factor of 4 when irradiance values are compared and within a factor of 2 when ratios of irradiance values for different gasses are compared. Comparisons among workers who used widely different pulse lengths indicate that the onset of plasma formation is measured better by energy fluence than by irradiance.

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Three-level systems in which the middle level has opposite parity from the remaining levels can develop optical gain on the excited-state transition when a two-photon resonant field couples the ground state with the uppermost state. Both population gain, which leads to amplified spontaneous emission, and hyper-Raman gain, which leads to stimulated hyper-Raman scattering, occur.1 Evidence for both types of process appears in two-photon-excited bidirectional emission in atomic xenon.2 This paper presents and compares threshold scaling characteristics, temporal behavior, directional energy distribution patterns, and tuning behavior as evidence for the gain mechanism in xenon. Near threshold, clear evidence for population inversion gain exists. Above threshold, axial emission energy exceeds off-axial (spontaneous emission) energy by a factor which increases with excitation energy. This excess of energy indicates the presence of hyper-Raman and/or four-wave mixing gain.

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.