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Multiphoton detachment of negative alkaline ions

Natalia Vinci

Published Jan 1, 2001• 0 citations
OpenAlex

Abstract

The aim of this thesis is to extend the study of multiphoton processes to the heavier negative ions of the alkali-metal atoms and thus, Na"- and K"- were natural candidates for this investigation. The main idea is to achieve an homogeneous description of negative alkaline ions and their response to an intense laser field. This idea has been suggested by recent experimental findings for negative alkaline ions which have revealed a rich structure of their scattering and photodetachment spectra, showing the existence of high-lying temporary negative ion states. Moreover, dramatic effects due to excess photon detachment have been observed yielding additional information on the dynamics of these highly correlated systems

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•Jan 1, 1989•0 citations
The aim of this thesis is to extend the study of multiphoton processes to the heavier negative ions of the alkali-metal atoms and thus, Na"- and K"- were natural candidates for this investigation. The main idea is to achieve an homogeneous description of negative alkaline ions and their response to an intense laser field. This idea has been suggested by recent experimental findings for negative alkaline ions which have revealed a rich structure of their scattering and photodetachment spectra, showing the existence of high-lying temporary negative ion states. Moreover, dramatic effects due to excess photon detachment have been observed yielding additional information on the dynamics of these highly correlated systems
Excited states of atoms and molecules exhibit a rich array of diverse phenomena. This dissertation examines two exotic states of atoms at such excited levels: Rydberg molecules and atomic negative ions. Rydberg molecules are formed by a Rydberg atom and one or more ground state atoms, and can be highly polar due to their unusual electronic wave functions and enormous bond lengths. This dissertation expands the theory of these molecules by studying the formation and structure of polyatomic molecules, multichannel Rydberg molecules formed from divalent atoms, and spin effects and relativistic interactions. It also details intermolecular forces between Rydberg molecules, their manipulation via external fields, and their dependence on the intricacies of electron-atom scattering. This electron-atom interaction is also the main component of the latter portion of this thesis, which studies doubly excited states of alkali negative ions in very polarizable and nearly degenerate atomic states. Photodetachment of these states reveals electron correlation and long-range forces stemming from their high excitation.
Multiphoton excitation with elliptically polarized light brings out more information in the photodetachment or photoionization processes than linearly polarized light. This information can be reached by recording photoelectron angular distributions for several values of the ellipticity angle, and fitting the whole set of data with an analytic formula. We give here the appropriate formula, valid for any number N of exciting photons, with the assumptions of (1) an initially even and momentumless (J equals 0) atom or ion and (2) that after excitation of an electron, the residual core be left in an odd state. These are the conditions met by multiphoton detachment from halogen negative ions. With elliptically polarized light of (lambda) equals 1064.2 nm, we have measured the angular distributions of three-photon detached electrons from the ion I-, and four-photon detached electrons from Cl- and F-. The experimental results are quantitatively analyzed and commented on.
The R-matrix Floquet approach is applied to study the negative and ions in a light field. Detachment rates are obtained for detachment processes involving up to three photons. The results obtained in the present approach are compared to other experimental and theoretical results. For two- and three-photon processes reasonable agreement with other calculations has been found, while for two-photon detachment the results agree with the experimental cross sections. The three-photon results are in less good agreement with experiment although the larger error bars make accurate comparisons more difficult. The changes in the detachment behaviour for these ions are compared to each other as well as to the detachment behaviour of .
Multiphoton detachment of ${\mathrm{Te}}^{\mathrm{\ensuremath{-}}}$ is studied utilizing two optical fields of wavelengths \ensuremath{\sim}694 and \ensuremath{\sim}1064 nm, respectively. Three-photon detachment is resonantly enhanced when the Raman condition is satisfied for coupling of the ${\mathrm{Te}}^{\mathrm{\ensuremath{-}}}$ 5p5{\mathit{p}}^{5}p5 2^{2}2P3/2{\mathit{P}}_{3/2}P3/2​ and 2^{2}2P1/2{\mathit{P}}_{1/2}P1/2​ fine-structure states. The fine-structure splitting is determined to be 5004.7\ifmmode\pm\else\textpm\fi{}0.2 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$, which represents a 25-fold improvement over earlier measurements. The possibilities for extended spectroscopic measurements, as well as general perspectives for multiphoton experiments at high intensities, are briefly discussed.
In the first part of this thesis, a new variational principle is presented for the calculation of perturbative transition amplitudes of any order but free from any singularities. Applications are made to the multiphoton ionization and harmonic generation for atomic hydrogen. Its formulations in hyperspherical coordinates as well as in Hartree-Fock representation are also presented. In the second part of this thesis, theories for multiphoton detachment in a static electric or magnetic field are developed. They are based on the analytic solutions of an electron in the combined field of a laser and a static electric or magnetic field, and, therefore, are nonperturbative in both the laser intensity and the static electric or magnetic field strength. Heretofore unexpected cyclotron resonances, which are due to the infinite range character of the electron-photon coupling induced by the external magnetic field, are shown to exist under certain conditions.