An approximation scheme is proposed to incorporate the influence of the Coulomb potential on the photoelectron in a nonperturbative treatment of multiphoton ionization rates. The method involves an approximation to an exact rate expression; when the latter is expanded in powers of the binding potential, the zeroth-order term is the commonly used Keldysh rate. The approach is applied to hydrogenlike atoms. Photoelectron angular distributions are calculated; these compare favorably with experimental measurements and with results of some other theoretical approaches.
We formulate a computationally feasible method for calculating multiphoton ionization rates for atoms exposed to intense fields in the intensity regime where perturbation theory ceases to apply. The method is based on the time-independent picture of ionization, which starts with the Floquet ansatz. The question of the gauge of the radiation field is discussed in some detail. Various expressions for the ionization amplitude are derived from a variational principle, with the radiation field expressed in the velocity gauge. We consider in particular an approximation in which the wave vector developing from the initial state is replaced by a trial vector that is the Floquet expansion truncated just below the threshold for ionization, and in which the wave vector developing into the final state is replaced by a trial vector that is just the wave vector appearing in the Kroll-Watson low-frequency approximation in scattering theory. We have applied this approximation to hydrogen and we present some results for both nonresonant and resonant multiphoton ionization. We argue that the experimentally observed resonance structure in the above-threshold peaks of the ionization signal occurs through the electron jumping from one dressed-state energy-eigenvalue curve to another.
The Keldysh-Faisal-Reiss theory of nonresonant multiphoton ionization seems to give reasonably good agreement with experiments for production rates in the above-threshold-ionization peaks. The theory has some conceptual difficulties, since physically equivalent Hamiltonians give radically different results when treated by this method. An alternate form of the S matrix is used here in which approximation must be made upon the exact wave function evolving from the initial state rather than the time-reversed form used in the Keldysh-Reiss treatment. The exact initial state is approximated by an adiabatic form which results in an S matrix that eliminates the conceptual difficulties described above.
Multiphoton ionization of hydrogen atoms by a strong multimode field when several final continuum states are populated is treated theoretically within a model based on the S-matrix formalism. The field is taken in dipole approximation, with zero bandwidth. Field-dressed Coulomb wave functions are used for the electron final states. Ionization rates are calculated for different numbers of photons absorbed in excess of the minimum number required to go into the continuum. In general, the calculated quantities are in good qualitative agreement with the corresponding experimental observations.
A general framework for description of quantum systems in strong external fields is established. The most important application of the theory is concerned with the multiphoton ionization of atoms and molecules. The adiabatic approximation is developed. The Hamiltonian of the system is diagonalized by a time-dependent unitary transformation, which generates an interaction energy vanishing for very slow fields. A general analysis of the photoionization rates is performed. A specific model is considered: one-dimensional motion in the δ-function potential and external harmonic electric field. This model allows the exact solution for time-dependent eigenvalues and eigenfunctions. These solutions are compared with the conventional free electron approach to the ionization states.
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.