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Multiphoton processes in complex atoms and ions

David H. Glass

Published Jun 1, 1997• 0 citations
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Singly and doubly charged Ca ions have been produced by multiphoton excitation of Ca vapour with 5 ns, low intensity (⩽3 × 10 11 W cm −2 ) dye-laser pulses in the 675–685 nm wavelength range, including the four-photon 4s 2 1 S 0 → 4p 2 1 S 0 excitation. The intensity and wavelength dependence of the ion yields was recorded as well as the fluorescence emission from excited states of the Ca ion in an effort to identify the excitation pathways leading to single and double ionization. Unambiguous evidence for the absorption of at least two photons above the first ionization threshold was recorded, in agreement with earlier results for Mg and Sr obtained under similar conditions. However, certain characteristics of the process differ significantly from those of the earlier results, despite the apparent similarity in both the atomic structure and the excitation scheme. The most striking and unexpected finding is that for a certain wavelength, the Ca 2+ yield is observable well before the saturation intensity of Ca + and, moreover, it grows with intensity and saturates in parallel with the Ca + yield. Possible mechanisms behind this outcome are discussed in detail as well as their implications for the multiphoton multiple ionization of complex atoms. Our tentative conclusion is that the occurrence of doubly charged ion production before the singly charged ion saturation should not be considered as 'synonymous' with direct (or non-sequential) multiphoton double ionization.
The study of the creation of doubly charged ions upon the laser-induced multiphoton ionization of alkaline-earth metals is reviewed. The results show that the features of the creation of the doubly charged ions depend on the spectral range of the ionizing laser radiation. In the ionization of the alkaline-earth atoms by the visible laser radiation, the cascade creation of the doubly charged ions is predominantly implemented when the ions result from the multiphoton ionization of singly charged ions created in the presence of the same laser pulse. In the multiphoton ionization of the alkaline-earth atoms by the IR laser radiation, the two-electron process occurs when the doubly charged ions are directly created from neutral atoms owing to the ionization via induced resonances with strongly perturbed states of these atoms.