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Topical Meeting on Laser Techniques in the Extreme Ultraviolet

Multiphoton Ionization of Alkali Atoms

R. N. Compton, Adila Dodhy, John A. D. Stockdale, Cornelius E. Klots

Published Jan 1, 1984• 0 citations

Abstract

Multiphoton ionization (MPI) of alkali atoms has played a pivotal role in our understanding of the interaction of intense electromagnetic radiation with matter. The "hydrogen-like" energy levels and absence of low-lying autoionizing states make the alkali atom theoretically tractable. The low ionization potential of these atomic species and the ease with which one can produce atomic beams of alkali atoms facilitate the experimental studies. Many of the early MPI studies involved high-powered fixed-frequency lasers. Presently, the availability of tunable dye lasers with wavelength extension (i.e., frequency doubling, Raman shifting, etc.) makes it possible to study one- to six-photon ionization of the alkali atom with continuously tunable radiation. Also, harmonic generation in these systems which may be present during ionization can be recorded more easily than in other systems since the radiation generated is in the visible or near ultraviolet spectral region. The ability to tune the laser to high Rydberg states with even or odd numbers of photons accesses electronic states of both parities. Stepwise excitation is capable of selectively producing states of high orbital angular momentum. Experiments in which highly excited states are produced in external electric or magnetic fields allow one to test fundamental ideas about the electron–Coulomb system in the quasi–continuum.3

DOI: 10.1364/euv.1984.mb5

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Multiphoton ionization (MPI) of alkali atoms has played a pivotal role in our understanding of the interaction of intense electromagnetic radiation with matter. The "hydrogen-like" energy levels and absence of low-lying autoionizing states make the alkali atom theoretically tractable. The low ionization potential of these atomic species and the ease with which one can produce atomic beams of alkali atoms facilitate the experimental studies. Many of the early MPI studies involved high-powered fixed-frequency lasers. Presently, the availability of tunable dye lasers with wavelength extension (i.e., frequency doubling, Raman shifting, etc.) makes it possible to study one- to six-photon ionization of the alkali atom with continuously tunable radiation. Also, harmonic generation in these systems which may be present during ionization can be recorded more easily than in other systems since the radiation generated is in the visible or near ultraviolet spectral region. The ability to tune the laser to high Rydberg states with even or odd numbers of photons accesses electronic states of both parities. Stepwise excitation is capable of selectively producing states of high orbital angular momentum. Experiments in which highly excited states are produced in external electric or magnetic fields allow one to test fundamental ideas about the electron–Coulomb system in the quasi–continuum.3

Abstract Experiments involving resonantly enhanced multiphoton ionization (REMPI) of alkali atoms contained in a heat pipe are discussed with reference to the quantum defect theory modification of the hydrogen atom energy levels. Quantum defects for the ns and nd levels are extracted from the data. This experiment is an excellent introduction to atomic spectroscopy and the selection rules involved. Ionization potentials are extracted from the Rydberg spectra. In the second part of this chapter a Raman shifter is employed to produce IR photons for multiphoton excitation of the low-lying p states of cesium. Three-photon excitation also produces third harmonic generation. The use of heat pipes for the production of alkali metal atom vapor is discussed as well as the use of a simple pick-up wire for ion detection.

Multiphoton ionization (MPI) of barium atom using an excimer-pumped pulsed dye laser has been studied in the wavelength range 570-608 nm at a laser intensity approximately 10.0 GW cm -2 . Resonances in MPI were recorded by monitoring either the ions produced in the multiphoton process using a thermionic detector or fluorescence from the ions formed in their various excited states of Ba + . The observation of photoion and fluorescence spectra were made on Ba vapour in the heat-pipe oven in the moderate-density regime ( approximately 10 13 atoms/cm 3 ) so that the collisional effects are negligible. Fine-structure resolution of the final ionic state (6p 2 P 1/2,3/2 ), produced after four-photon autoionizing decay was obtained. The decay of the Ba atom after four-photon absorption preferentially populates the 6p 2 P 3/2 state relative to the 6p 2 P 1/2 state.

Multiphoton ionization (MPI) via two-photon resonance with high-lying Rydberg levels is observed on Na and K atoms in modest (12--120 V/cm) dc electric fields. The field-induced MPI signals are manifested to such an extent that the nominally forbidden MPI via two-photon resonance with the np levels is induced at the same signal levels as or more intensely than the allowed MPI via the ns and nd Rydberg levels. The intensity inversion between the allowed and the forbidden MPI signals is observed on the K atoms in the wavelength region where the two-photon energy is very close to the field-ionization limit.

Discrete atomic energy levels lying between the first and second ionization potentials which are metastable against both auto-ionization and radiative decay have been observed in the alkali elements. These levels arise from the excitation of an electron from the outermost closed shell of the atom and have characteristic lifetimes in the microsecond region. A beam of metastable alkali atoms is produced by electron bombardment of neutral ground-state atoms and is detected by collecting the charged products of the decay. Stern-Gerlach magnetic-deflection experiments have been performed to show unambiguously that the signals arise from paramagnetic atoms and not from possible stray-photon effects in the apparatus. The excitation energies, electron-bombardment production cross sections, natural lifetimes, and the tentative spectroscopic assignments of these atoms are listed below: The energy and lifetime of the metastable lithium atom are in good agreement with the available theoretical estimates. The metastable states in the heavier alkali atoms are classified in relation to the known

{\mathrm{I}}^{b}

spectral terms. Magnetic and electric fields have been found to be effective in reducing the lifetime of the metastable atoms. The Zeeman quenching is discussed in a separate paper. The Stark quenching rate has been found to be proportional to the square of the electric field and to increase rapidly with atomic number

Z

. It is suggested that the Stark quenching results from a second-order interaction which involves the product of the electric field and the spin-orbit or other magnetic operators.

An approximate non-perturbative theory of multiphoton ionization of a hydrogen atom by two strong radiation fields is outlined. The special case is then considered for when one of the fields is of low intensity and high frequency and the other field is of high intensity and low frequency. A set of representative calculations has been performed for this case; that is, (a) angular distributions for given numbers of absorbed and emitted low-frequency photons and different geometries; (b) total cross-sections versus the strong-field intensity; (c) angular distributions summed over all the low-frequency photon exchanges, showing a fourfold symmetry in a geometry in which each ionization channel exhibits, instead, only a twofold symmetry; (d) the average energy gained by the ejected electrons. Calculations are performed for a strong low-frequency field of arbitrary polarization. In many respects, the present calculations are expected to complement those of single-field multiphoton ionization. It is hoped that the results of the calculations reported here may prompt systematic measurements also in this new class of processes, as the predictions are well within the state of the art of present multiphoton-ionization experiments.