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Physical Review A

Resonant photoionization of Ni I into autoionizing states

Peter Lievens, Erno Vandeweert, Peter Thoen, Roger E. Silverans

Published Sep 1, 1996• 26 citations
Publisher

Abstract

Two-step resonant photoionization of free Ni atoms is studied by one-color and two-color processes, using pulsed lasers with photon energies around half the ground-state ionization energy. Two-color two-step resonance ionization from the ground state a${\mathrm{}}^{3}$${\mathit{F}}_{4}$ and the first metastable state a${\mathrm{}}^{3}$${\mathit{D}}_{3}$ via the triplet states z${\mathrm{}}^{3}$${\mathit{G}}_{3,4,5}^{0}$ was used to probe the autoionizing states just above the ionization limit. Several strong lines in the one-color ionization spectrum are explained as direct two-photon transitions to autoionizing states. Photoionization cross sections were deduced from saturation measurements. The large cross sections observed for specific one-color two-step transitions are due to the near double resonant excitation into autoionizing states. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.54.2253

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Two-step resonant photoionization of free Ni atoms is studied by one-color and two-color processes, using pulsed lasers with photon energies around half the ground-state ionization energy. Two-color two-step resonance ionization from the ground state a{\mathrm{}}^{3}$${\mathit{F}}_{4} and the first metastable state a{\mathrm{}}^{3}$${\mathit{D}}_{3} via the triplet states z{\mathrm{}}^{3}$${\mathit{G}}_{3,4,5}^{0} was used to probe the autoionizing states just above the ionization limit. Several strong lines in the one-color ionization spectrum are explained as direct two-photon transitions to autoionizing states. Photoionization cross sections were deduced from saturation measurements. The large cross sections observed for specific one-color two-step transitions are due to the near double resonant excitation into autoionizing states. \textcopyright{} 1996 The American Physical Society.
We have examined the stepwise-resonant three-photon-ionization spectrum of neutral Zirconium atoms using three separately-tunable pulsed visible dye lasers. The ground-level (first-step) transitions were chosen on the basis of demonstrated 91Zr selectivity. Lifetimes of even-parity levels around 36000 cm-1, measured with the delayed- photoionization technique, range from 10 to 100 nsec. Direct ionization cross sections appear to be less than 10-17 cm2; newly-detected autoionizing levels give peak ionization cross sections (inferred from saturation fluences) up to 10-15 cm2. Portions of Rydberg series converging to the 315 and 763 cm-1 levels of Zr+ were identified. 'Clumps' of autoionizing levels are thought to be due to Rydberg-valence mixing.
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A two-laser theory is formulated for the photoionization of Li atoms. The first laser is tuned above the ionization threshold of Li(2s)\mathrm{Li}(2s)Li(2s). The second laser probes the ionized target. Stimulated recombination into Li(ns)\mathrm{Li}(\mathrm{ns})Li(ns) occurs near the Raman-type resonance point ${\ensuremath{\epsilon}}_{\mathrm{ns}}\ensuremath{-}{\ensuremath{\epsilon}}_{2s}\ensuremath{-}{\ensuremath{\epsilon}}_{1}+{\ensuremath{\epsilon}}_{2}=0$ (where n>2n>2n>2 and ${\ensuremath{\epsilon}}_{q}$ is a photon energy). Near the resonance point the ionization probability is characterized by a line profile which resembles that for an autoionizing resonance.
We have performed an experimental study of the atomic system ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$, for which the ground state 5s2{\mathit{s}}^{2}s2 is coupled to the autoionizing state 5${\mathit{p}}_{1/2}$6s by means of a strong resonant laser field. The investigations are based on irradiation of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ with intense (I\ensuremath{\le}1.5\ifmmode\times\else\texttimes\fi{}1010{10}^{10}1010 W/cm2{\mathrm{cm}}^{2}cm2) laser pulses of duration \ensuremath{\sim}1 ns. Single-photon detachment of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ is suppressed due to the Fano interference between transitions directly to the continuum and transitions via the autoionizing state. In contrast, two-photon absorption is at the same time resonantly enhanced since no such destructive interference is present in this process. These observations constitute experimental evidence of general features predicted from theoretical considerations of autoionizing states in strong laser fields. Furthermore, we discuss the role of autoionizing states in multiphoton double-ionization processes. Electron spectroscopy has been used to show that double ionization of ${\mathrm{Rb}}^{\mathrm{\ensuremath{-}}}$ primarily is the result of a sequential removal of the two electrons via an excited Rb state. The perspectives for direct two-electron ionization in negative ions are briefly discussed.
We have observed ionization of Mg by both direct and stepwise two-photon excitation of the 3p2{p}^{2}p2 1{\mathrm{}}^{1}1S state. The line shape of the single-color direct process is strongly modified by the resonance denominator associated with the intermediate virtual state. The measured energy and width of this resonance as determined by the stepwise two-color technique agree well with previous determinations.