Physical Review A

Many-body approach to two- and three-photon double ionization and excitation of xenon

Anne L’Huillier, Goran P. Wendin

Published Dec 1, 1987• 11 citations

Abstract

We investigate different processes which may be responsible for ejection of two electrons from the external shell of xenon through the absorption of two and three photons, namely two-photon direct double ionization and three-photon sequential double ionization via the ion in an excited state or in the ground state. We calculate the cross sections of the ionization processes involved, using many-body perturbation theory. These cross sections are then used within a rate equation model for comparing the relative efficiencies of the different double-ionization mechanisms.

DOI: 10.1103/physreva.36.5632

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Physical Review A

Many-body approach to two- and three-photon double ionization and excitation of xenon

Anne L’Huillier, Goran P. Wendin

Published Dec 1, 1987• 11 citations

Publisher

Abstract

DOI: 10.1103/physreva.36.5632

Related papers

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Two-photon absorption cross sections of ground-state xenon atoms to the 2

{p}_{5}

(J=0), 2

{p}_{6}

(J=2), and 2

{p}_{9}

(J=2) states in the 5${p}^{5}

6p configuration and photoionization cross sections at 193 and 248 nm from the 2

{p}_{5}$ and 2

{p}_{6}

states have been determined and are compared with previous experimental and theoretical values where such exist. Fluorescence depletion spectroscopy as a method for determining excited-state photoionization cross sections is described and discussed and shown to have many attractive features. Based on our cross-section measurements, we calculate that (2+1)-photon photoionization in Xe with a laser intensity of 30 MW/

{\mathrm{cm}}^{2}

during 25 ns at 249.6 nm, using the 2

{p}_{5}

(J=0) state as an intermediate state, can produce a fractional ionization of 10%.

We present accurate cross sections for two-photon double ionization of helium at photon energies above and below the threshold for sequential double ionization. Above this threshold

(54.4\phantom{\rule{0.3em}{0ex}}\mathrm{eV})

, sequential ionization competes with nonsequential ionization. Remarkably, even below

54.4\phantom{\rule{0.3em}{0ex}}\mathrm{eV}

, sequential ionization leaves a clear signature in the magnitude and shape of both the total and energy-sharing cross sections---even though at these energies it is only a virtual process.

2{s}^{2}

valence shell electrons in the presence of a fully occupied

1{s}^{2}

frozen core shell. The relative contributions of the two-photon direct and sequential process are systematically explored by varying both pulse duration and central frequency. The energy and angular differential ionization yields reveal the signatures of both mechanisms, as well as the role of electron correlation in both the single and double ionization continua. In contrast with previous results on the helium atom, the presence of an electronic core strongly affects the final state leading to back-to-back electron emission even in the a priori less correlated two-photon sequential mechanism. In particular, a dominant pathway via excitation ionization through the

{\mathrm{Be}}^{+}(2p)

determines the profiles and pulse-duration dependencies of the energy and angle differential yields.

Above

54.4\phantom{\rule{0.3em}{0ex}}\mathrm{eV}

, two-photon double ionization of helium is dominated by a sequential absorption process, producing characteristic behavior in the single and triple differential cross sections. We show that the signature of this process is visible in the nuclear recoil cross section, integrated over all energy sharings of the ejected electrons, even below the threshold for the sequential process. Since nuclear recoil momentum imaging does not require coincident photoelectron measurement, the predicted images present a viable target for future experiments with new short-pulse vacuum ultraviolet (vuv) and soft x-ray sources.