The selectivity of three-step pulse photo-ionization of atoms versus the detuning delta of exciting radiation frequencies from intermediate resonance is investigated in powerful laser fields where the power broadening of the resonant transitions is at least of the order of isotope shifts. The Doppler broadening of the resonant transitions is taken into account and it is assumed that the sum frequency of both exciting laser radiations is tuned to the line centre of the two-photon transition of a selected isotope. It is shown that in this situation the photo-ionization selectivity increases so greatly with the absolute detuning mod delta mod that even in such strong fields the process of photo-ionization can be highly selective. The optimization of selective photo-ionization of atoms is discussed in connection with the decrease in the selective isotope yield with increase of the absolute detuning mod delta mod . Analytical consideration of selective three-step pulse photo-ionization in powerful laser fields, based on the density matrix formalism, is presented together with the results of numerical simulation of the 40 Ca- 48 Ca laser isotope separation process as an example.
A semiclassical treatment of collision-induced three-photon ionization of atoms with a near two-photon resonance is presented. The system is described by an effective two-level system. The wavelength dependence of the ionization yield does not obey a power law. When the first excited state is far from resonance, and with a
R6C6 interatomic potential, a first-order correction to the expected $\ensuremath{-}\frac{3}{2}$ power law obeys a - \textonehalf{} power law. This three-photon process promises to be an extremely sensitive method for the study of collisional effects in the far wing of two-photon $S\ensuremath{-}S$ and $S\ensuremath{-}D$ transitions, and without the requirement of high densities.