Collision-free multiple photon ionization of atoms and molecules at 193 nm

The nonlinear coupling of 193-nm radiation to a range of atomic and molecular materials has been experimentally explored up to a maximum intensity on the order of \ensuremath{\sim}${10}^{17}$ W/${\mathrm{cm}}^{2}$. Studies of collision-free ion production clearly exhibit anomalous behavior which strongly implies that the atomic shell structure is the principal determinant in the observed response. On the basis of the observed coupling strength and the measured atomic-number (Z) dependence, the experimental evidence points to a coherent atomic motion involving several electrons, possibly an entire shell, as the main physical mechanism enabling the scale of energy transfers seen. Therefore, states representing multiple excitations appear to play a central role in the coupling, a consideration that fundamentally distinguishes the nonlinear interaction of a multielectron atom from that of a single-electron system. Comparison of the experimental findings with standard theoretical treatments, of either a perturbative or nonperturbative nature, does not produce satisfactory agreement. Conversely, the formulation of a simple classical estimate qualitatively conforms to several features of the observed behavior including the shell character of the interaction, the maximum energy transfer, the dependence of the average energy transfer on the intensity of irradiation, the frequency dependence of the observed energy transfer, and the weak influence of polarization.