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Physical Review A

Selective ionization: Effects of power broadening, laser bandwidth, and interaction time on selectivity

Bo-nian Dai, P. Lambropoulos

Published Nov 1, 1986• 38 citations
Publisher

Abstract

We present an analysis of the factors that affect selectivity in resonant multiphoton ionization. After a discussion of the formalism in terms of the density matrix in the context of two-photon-resonant three-photon ionization, we apply the theory to Li and Sr, demonstrating the effects of laser bandwidth, power broadening, and pulse duration.

DOI
10.1103/physreva.34.3954

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We present an analysis of the factors that affect selectivity in resonant multiphoton ionization. After a discussion of the formalism in terms of the density matrix in the context of two-photon-resonant three-photon ionization, we apply the theory to Li and Sr, demonstrating the effects of laser bandwidth, power broadening, and pulse duration.
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We theoretically study intensity-saturation effects in resonant harmonic generation and multiphoton ionization. A first laser excites a two-photon resonance which is coupled by a second laser to an autoionizing state. Starting from an effective Hamiltonian for the three resonant atomic states, we derive a set of equations for the density matrix of the gaseous medium and the electromagnetic field within a semiclassical framework. We present and discuss analytical and numerical solutions of these equations which show a variety of line profiles depending critically on the intensities of the incident laser pulses.
I present a perturbation theory of multiphoton ionization based on the resolvent operator. The theory is applied to a detailed study of two-photon ionization under near-resonance conditions. It is shown that a distinction must be made between linear level shifts and widths, and resonance shifts and widths which appear in the transition probability. The resonance shifts and widths exhibit saturation effects and their values tend to be much smaller than those of the linear level shifts and widths. Using numerical examples corresponding to tunable dye lasers and alkali-metal atoms, we show that the above shifts can have a dramatic effect on the ionization rate even when the laser is not in exact resonance with the intermediate level. The question of "one-step" vs "two-step" two-photon ionization is also discussed. It is shown that exact resonance does not necessarily imply a two-step process. In fact, in most cases it is quite the opposite. A quantitative criterion for this distinction is established. Finally, a distinction is made between instrumental saturation and saturation of the transition probability. The two are shown to be of different nature. Further extensions of the work are also discussed.
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.
We present a theoretical analysis of multiphoton ionization through resonant intermediate states shifted through resonance during a short, intense pulse. The resonant structure in the photoelectron spectra is compared with what it would be if the peak intensity or the frequency of the laser were scanned, and the various differences are discussed in detail. The dynamical behavior is described in terms of a density matrix evolving under a realistic temporal and spatial pulse shape. Our results, on atoms with realistic parameters, show structure similar to that observed in recent experiments. Results for circularly polarized light are also presented. The limitations and advantages of the model are discussed.