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Physical Review A

Scheme for multistep resonance photoionization of atoms

Bo Liu, Xi‐Jing Ning

Published May 30, 2001• 6 citations
Publisher

Abstract

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 ${}^{235}\mathrm{U}$ with our scheme, showing that the intensity of two laser beams can be lowered by two orders of magnitude without losing high ionization probability.

DOI
10.1103/physreva.64.013401

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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.
A theoretical model of two-step resonant ionization which includes an autoionizing state is developed. The effects examined include interactions with a multimode laser and Zeeman and hyperfine multiplets. We approach this problem starting from first principles by treating the atom-radiation system as a unit. Theoretical analysis and numerical calculations of ionization probabilities are given. The intermode scattering is investigated in detail, and a simple physical interpretation of the dynamical effect is given. Comparisons of ionization probabilities for two-step processes with first-step excitations by single-mode or two-mode lasers are made. It is found that, if the mode spacing in a multimode-laser beam is less than the Doppler width of the atom, the multimode laser can more effectively produce ions than a single-mode laser does. This leads to the conclusion that the resonance effect is more important than the power-broadening effect. This is shown to be also true when Zeeman and hyperfine multiplets are included.
Previous studies on strong-field autoionization involving high-order ionization processes are mainly investigated for the cases of CW laser irradiations. This paper extends those studies to the cases of square laser pulses with arbitrary widths. Populations of the ground state and the line shapes of the autoionizing resonance are discussed. It is shown that strong-field autoionization and the high-order ionization processes are drastically affected not only by the intensities but also by the time of interaction between atoms and laser field.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.
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.
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 a3{\mathrm{}}^{3}3F4{\mathit{F}}_{4}F4​ and the first metastable state a3{\mathrm{}}^{3}3D3{\mathit{D}}_{3}D3​ via the triplet states z3{\mathrm{}}^{3}3G3,4,50{\mathit{G}}_{3,4,5}^{0}G3,4,50​ 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.