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Acta Optica Sinica

Effect of polarization spectroscopy in multistep excitation and ionization of atoms on ionization efficiency

XU Pinfang

Published Jan 1, 1993• 0 citations
OpenAlex

Abstract

In this paper, the seventeen real motion equation of atoms were shown for the first time in considering the polarization choices of laser lights. The importance of polarization spectroscopy in the determination of ionization yields of multi-step excitation and ionization of atoms (MSEIA) was shown.

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Traditional schemes for multistep resonance photoionization of atoms let every employed laser beam interact with the atoms simultaneously. In such a situation, analyses via time-dependent Schr\"odinger equation show that high ionization probability requires all the laser beams must be intense enough. In order to decrease laser intensity, we proposed a scheme that the laser beam used to pump the excited atoms (in a higher bound state) into an autoionization state does not interact with the atoms until all the population is transferred by the other lasers from a ground state to the bound state. As an interesting example, we examined three-step photoionization of 235U{}^{235}\mathrm{U}235U with our scheme, showing that the intensity of two laser beams can be lowered by two orders of magnitude without losing high ionization probability.
We analyze the dependence of the rate of associative ionization of two radiatively excited atoms on the polarization properties of the exciting light. This provides a direct relation between the observed ion-production rate as a function of the polarization and the ionization rates for various combinations of the magnetic substates. We consider an atomic beam irradiated by a single laser beam, as well as an atomic vapor. The description applies to a recent experimental observation of a strong polarization dependence of the ionization rate in an atomic beam, and at the same time we suggest alternate experimental methods of analyzing the total cross sections of any inelastic or reactive binary collision of excited atoms as a function of the magnetic quantum numbers.
The dynamical process of photoexcitation and photoionization of alkali atoms is studied with three-step laser pulses, focusing on the similarities and differences between Li and Cs atoms on their properties by making a comparison of them. Based on several excitation schemes, the present work not only establishes the rate equations of atom population for all related transition states, but also obtains the analytical solutions of photoexcitation and photoionization process. The mathematical solutions are simplified significantly by restricting the most general case to the several special cases, either designed or selected carefully, in order to highlight the main factors and obtain the physical insight underlying the complicated mathematical expressions. With self-programming, the possible impact of time configuration of laser pulses on the three-step laser excitation process of the photoexcitation and photoionization is calculated and studied systematically. Variation of the ionization efficiency with the laser parameters is investigated and discussed. With the same time configuration of laser pulses, the dependences of atom population for all the related transition states on the two different excitation paths are compared and analyzed, reflecting the impact of changing the atomic parameters. Under the similar excitation conditions, the differences of ionization efficiency between Li and Cs atoms are explored. Finally, based on the present study, several means for optimizing ionization efficiency are proposed.
Numerical computations of ionization efficiency and isotope selectivity of 176 L u have been carried out for the following three-step ladder type photoionization scheme, 5 d 6 s 2 2 D 3 / 2 ( 0.0 c m − 1 ) − − − ⟶ 540.4068 n m ⁡ 5 d 6 s 6 p 4 F 5 / 2 o ( 18504.58 c m − 1 ) − − − ⟶ 535.0626 n m 5 d 6 s 7 s 4 D 3 / 2 ( 37193.98 c m − 1 ) − − − ⟶ 618.0061 n m 53375 c m − 1 A u t o i o n i z a t i o n S t a t e → L u + , by invoking the density matrix formalism for the laser–atom interactions. Equations of motion have been derived for the odd isotopes by inclusion of hyperfine levels. The line shapes and their effect on the ionization efficiency and isotope selectivity have been discussed in detail. The effects of power of excitation and ionization lasers, spectral bandwidths, pulse delays, Doppler broadening of the atomic ensemble on the ionization efficiency, and degree of enrichment have been presented. Optimum conditions for the power of excitation, detunings, and other system parameters for the selective yet efficient photoionization of 176 L u have been identified.