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Journal of Physics B Atomic and Molecular Physics

Resonant multiphoton ionisation and third-harmonic generation in mercury vapour

Didier Normand, J. Morellec, Jürgen Reif

Published Apr 28, 1983• 34 citations
Publisher

Abstract

The interaction of intense dye laser radiation (up to about 100 GW cm -2 ) with Hg vapour in the pressure region of 10 15 to 10 -1 Torr leads to competition between multiphoton ionisation-dominant at low pressure-and third-harmonic generation ( approximately 1850AA) prevailing at high pressure. In particular, third-harmonic generation enhanced by a four-photon resonance is-to the authors' knowledge-reported for the first time.

DOI
10.1088/0022-3700/16/8/004

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The interaction of intense dye laser radiation (up to about 100 GW cm -2 ) with Hg vapour in the pressure region of 10 15 to 10 -1 Torr leads to competition between multiphoton ionisation-dominant at low pressure-and third-harmonic generation ( approximately 1850AA) prevailing at high pressure. In particular, third-harmonic generation enhanced by a four-photon resonance is-to the authors' knowledge-reported for the first time.
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.
A competition between resonant multiphoton ionization (MPI) and third harmonic generation (THG) involving three-photon resonances was first reported by Miller et al.1 Recently, a similar competing process involving four-photon resonances was observed in the multiphoton ionization of Hg2. In this paper we report a similar observation in the three- and four-photon excitation spectra of Kr and Ar. Both the multiphoton ionization and the VUV radiation generated in the focal volume are measured over a broad range of gas pressures (0.01-100 Torr) and laser fluences. The 5s, 5f, and 6p′ levels of Kr and the 4s, 4p′, and 7p levels of Ar are investigated. The spectral lines are observed to broaden and to shift from line center as a function of increasing gas pressure and laser intensity. The effect observed in three-photon resonant lines is explained by the occurrence of a competition between MPI and THG.1 A similar effect observed in the four-photon resonances is interpreted as the result of THG enhanced by the four-photon levels—a five-photon process. However, it is not clear why the four-photon spectral line-width becomes narrower when the gas pressure is further increased; this is discussed.
Harmonic-generation processes at high laser intensity are strongly affected by resonant multiphoton ionization. In this paper coexistence of these phenomena at low pressure and high intensity is taken into account with use of a mean-field theory. New consequences of this model are derived, especially for resonances strongly damped by ionization. Available experimental data on mercury agree qualitatively with this model. A second approach, called the quasistatic approximation, is used to get analytical solutions for mean-field equations, in good agreement with numerical results. Furthermore, possible applications of the quasistatic approximation to the study of harmonic generation at both high pressure and high laser intensity are mentioned.
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.
Three-photon resonance enhancement of third-harmonic generation and multiphoton ionization is treated for a slab geometry configuration. Striking pressure effects which become important at concentrations $n\ensuremath{\gtrsim}{10}^{12}$ /cm3{/\mathrm{c}\mathrm{m}}^{3}/cm3 for narrow-bandwidth short-pulse lasers are predicted for both the third-harmonic signal and the multiphoton ionization. For example, part of the third-harmonic signal exists the slab simultaneously with the laser pulse while another part is time delayed for small detunings from resonance. At intermediate detuning from the three-photon resonance the two parts can interfere. Multiphoton ionization yields near three-photon resonance are strongly suppressed under certain conditions, and peaks may occur for proper detunings on both sides of the three-photon resonance. A detailed experimental verification is suggested for Xe.