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Optics Communications

Saturation and rabi oscillations in resonant multiphoton ionization

P. L. Knight

Published Aug 1, 1977• 56 citations
Publisher
DOI
10.1016/0030-4018(77)90013-x

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Photo-ionization probability is an important factor in the practical use of resonance enhanced multiphoton ionization (REMPI). To a certain experimental condition, it depends on the competition between spontaneous radiation and ionization of the excited particles. In this work, we investigate the influence of laser resonance detuning, Rabi frequency and ionization rate on spontaneous radiation and ionization in the process of REMPI with the theory of density matrix equation. A model of three energy level system is adopted. It is found that the spontaneous radiation and ionization probability increase with the decrease of laser resonance detuning. They get to the maximum when resonance detuning equals zero. The line width of spontaneous emission will decrease with the increase of ionization rate due to the competition between spontaneous radiation and ionization. In addition, the spontaneous radiation and ionization probability increase with Rabi frequency until gets to saturation. Laser resonance detuning has no influence on the saturation value. It only influences the Rabi frequency for saturation. If Rabi frequency increases further after saturation, the spontaneous radiation will decrease because of the phenomena of energy level splitting in strong laser field. Now that resonant absorption and large laser intensity can increase the ionization probability greatly, so we must select suitable laser frequency and large laser intensity in the practical use of REMPI, in order to get optimum detection result.
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.
With quantum calculations, we have investigated the multiphoton nonsequential double ionization of helium atoms in intense laser fields at ultraviolet wavelengths. Very surprisingly, we find a so-far unobserved double-circle structure in the correlated electron momentum spectra. The double-circle structure essentially reveals multiphoton Rabi oscillations of two electrons, which are strongly supported by the oscillating population of a certain doubly excited state and by the oscillating double ionization signals. This two-electron multiphoton Rabi effect provides profound understandings of electronic correlations and complicated multiphoton phenomena and is expected to be a new tool for broad applications, such as quantum coherent control.