A perturbation theory of the ionization of atoms by simultaneous absorption of several photons, each of whose energy is less than the ionization potential, is developed from the evolution-operator formalism. A precise computation is made for the hydrogen atom, giving transition rates as a function of photon energy for two- through twelve-photon photoionization. The eighth-order ionization rate (in cgs units) at the 1.78-eV ruby-laser line is found to be \ensuremath{\sim}${10}^{\ensuremath{-}244}$\ifmmode\times\else\texttimes\fi{}
(photonflux)8 and should be observable using available techniques. Good agreement is obtained with Zernik's exact calculation of the two-photon ionization rate of metastable
2S hydrogen. Approximate calculations are made for the rare gases. Assuming "typical" experimental conditions of a gas density of \ensuremath{\sim}
1020 atoms ${\mathrm{cm}}^{\ensuremath{-}3}$ and a ruby laser focused into a volume of \ensuremath{\sim}${10}^{\ensuremath{-}8}$
cm3, we find that the flux required to liberate one electron during a 10-nsec pulse is \ensuremath{\sim}
1029 ${\mathrm{cm}}^{\ensuremath{-}2}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ for Xe, Kr, and Ar and \ensuremath{\sim}5\ifmmode\times\else\texttimes\fi{}
1030 photons ${\mathrm{cm}}^{\ensuremath{-}2}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ for Ne and He. These gases ionize with the simultaneous absorption of 7, 8, 9, 13, and 14 photons, respectively. The predicted rate for Xe is found to be in excellent agreement with the recent direct measurements of Voronov and Delone. We conclude that multiphoton ionization provides the initial electrons required for the optical breakdown of gases, though it does not account for the over-all growth of the discharge except possibly at very low pressures. Impurity atoms (particularly heavy rare gases) may be the source of "initiating" electrons in Ne and He.
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
A single-transverse-mode
Q-switched Nd-glass laser, which can operate over a number of longitudinal modes variable from 1 to 100, has been used to investigate laser temporal-coherence effects on the 11-photon ionization of xenon atoms. When the laser pulse has an over-all bandwidth of 4 ${\mathrm{cm}}^{\ensuremath{-}1}$, the number of ions formed is enhanced by ${10}^{6.9\ifmmode\pm\else\textpm\fi{}0.3}$ over that produced by a monomode laser pulse with the same average laser intensity. The observed enhancement in the number of ions due to the change in temporal coherence of the pulse is in good agreement with recent theoretical prediction.
The review is devoted to new effects discovered recently in the course of studying the process of nonlinear ionization of atoms in the field of laser radiation—above-threshold ionization, manifestation of multielectron structure of complex atoms, formation of multiply charged ions, tunneling ionization, and emission of short-wavelength radiation. The main experimental data and their theoretical interpretation are presented. A discussion is given of the criteria for the applicability of the lowest non-vanishing order of non-steady-state perturbation theory to the description of the interaction of an atom with the electromagnetic field.