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Physical Review Letters

Resonantly Enhanced Multiphoton Ionization and Third-Harmonic Generation in Xenon Gas

John C. Miller, R. N. Compton, M. G. Payne, W. W. Garrett

Published Jul 14, 1980• 178 citations
Publisher

Abstract

Resonantly enhanced multiphoton ionization signals through the $6s[\frac{3}{2}]J=1$ state of Xe rapidly disappear at pressures above 0.30 Torr; concurrently, intense, vacuum-ultra-violet third-harmonic radiation is detected in the forward direction. Laser excitation spectra of the vacuum ultraviolet light exhibit increasing blue shifts and bandwidths with increasing pressure. The observed competition between ionization and third-harmonic generation is discussed in terms of a model involving fast collective emission.

DOI
10.1103/physrevlett.45.114

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Resonantly enhanced multiphoton ionization signals through the 6s[32]J=16s[\frac{3}{2}]J=16s[23​]J=1 state of Xe rapidly disappear at pressures above 0.30 Torr; concurrently, intense, vacuum-ultra-violet third-harmonic radiation is detected in the forward direction. Laser excitation spectra of the vacuum ultraviolet light exhibit increasing blue shifts and bandwidths with increasing pressure. The observed competition between ionization and third-harmonic generation is discussed in terms of a model involving fast collective emission.
In connection with a recent experiment of vacuum-ultraviolet generation in multiphoton resonant ionization of xenon at increasing pressure, a model is elaborated to account for the simultaneous effect of a laser excitation tuned near a three-photon resonance and a pressure-induced emission from the resonant state to the ground state. Under certain assumptions usual in various super-radiance treatments, a system of Bloch equations is derived and numerically solved. The dependence of the ionization probability and third-harmonic production versus the interaction time, gas pressure, dynamical detuning, and laser intensity is extensively studied. A transition between a high and low ionization rate is observed when the pressure increases simultaneously with the disappearance of Rabi oscillations and a saturation of third-harmonic generation. An order-of-magnitude calculation reveals that such phenomena are accessible to experiment and a qualitative comparison with the above-mentioned results in xenon is found to be satisfactory.
Resonantly enhanced multiphoton ionization (MPI) and third-harmonic generation (THG) have been concurrently studied in the rare gases, xenon, krypton, and argon. The disappearance with increasing pressure of the MPI signals resonant with the three-photon allowed 6s6s6s, 5s5s5s, and 4s4s4s states, respectively, of the rare gases is linked to the appearance of THG. Conversely, THG is shown to be partially quenched at certain wavelengths by one- and two-photon absorption leading to ionization.
Two independently tunable, linearly polarized dye lasers have been used to study multiphoton ionization of gaseous xenon. One laser is tuned near three-photon resonance with the allowed 6s[3/2]J=1° resonance, which is not observed with one laser at these pressures because of the destructive interference between the three-photon-excitation and third-harmonic-excitation pathways to the 6s[3/2]J=1° state. The second laser is tuned to resonance with higher allowed np and np′ states of xenon. The missing ionization signal is seen to be dramatically restored by the addition of the second laser beam; however, the signal again disappears as the pressure is increased. These results are discussed in relation to recent experimental and theoretical studies of cancellation effects between three-photon excitation and third-harmonic generation. Spectroscopic information obtained from tuning each dye laser, together with data on the angular distributions resulting from rotating the plane of polarization of one laser relative to that of the second laser, clearly shows that two different ionization mechanisms are operative. In addition, these experiments unambiguously illustrate the importance of dissociative ionization of quasi-dimers of xenon over a rather broad frequency range.
New observations are reported of tunable vacuum ultraviolet light generated in the forbidden region to the red of the xenon $6{s}^{\ensuremath{'}}{[\frac{1}{2}]}_{1}^{0}$ state due to the introduction of a second, resonant laser field. Striking observations of double-resonant ionization signals on the blue side of the xenon $6{s}^{\ensuremath{'}}$ level are also reported. Both sets of data are interpreted in terms of the changes in phase matching and the nonlinear susceptibility induced in the medium by the second laser. These changes are successfully analyzed in terms of the ac Stark effect in the three-photon level due to the second laser field.
Multiphoton ionization in the region near a three-photon resonance is treated for focused, plane-polarized Gaussian beams with diffraction-limited beam divergence. In this situation, a third-harmonic field is generated within the laser beam. At, and very near, three-photon resonance the driving rate for the upper-state probability amplitude due to one-photon absorption of third-harmonic light becomes nearly equal to the corresponding three-photon rate due to the laser field, but these effects are 180\ifmmode^\circ\else\textdegree\fi{} out of phase. As a consequence of this cancellation between two pumping terms, the three-photon resonance line essentially disappears at moderate concentrations and the observed ionization has a line shape that is close to the phase-matching curve for third-harmonic generation. The ionization signal, near but not on the resonance, is due almost entirely to absorption of third-harmonic photons plus other laser photons; three-photon resonantly enhanced multiphoton ionization by the laser is much weaker. This is particularly true on the blue side of the three-photon resonance at detunings where phase matching occurs. The problem is treated quite generally with predictions of the full line shape for nnn-photon ionization and third-harmonic light generation near three-photon resonance, including the rather strong influences of positively dispersive buffer gases. We also show that the cancellation between the one-photon and the three-photon process is partially spoiled in the presence of a counterpropagating beam at the same frequency.