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Physical Review A

Two-photon double ionization of helium: An experimental lower bound of the total cross section

Philippe Antoine, Emmanuel Foumouo, Bernard Piraux, Toshihiko Shimizu, Hirokazu Hasegawa, Yasuo Nabekawa, Katsumi Midorikawa

Published Aug 22, 2008• 53 citations
Publisher

Abstract

We report on the experimental estimation of a lower bound of helium. Our experiment differs from a previous one described by Hasegawa et al. [Phys. Rev. A 71, 023407 (2005)]. The photons that correspond to the 27th harmonic of a Ti:sapphire laser have an energy of $41.8\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$. The extraction of the cross section rests on a theoretical model, based on the rate equations, that fully includes the contribution from the sequential channels and the macroscopic effects. Some of the experimental parameters are very difficult to measure accurately. For those parameters, we deliberately consider values compatible with their experimental determinations and that lead systematically to an underestimation of the two-photon double ionization cross section. Our estimation of this lower bound is higher than a bunch of various theoretical results. It stays, however, too close to these latter ones to draw any definite conclusion about their validity, even though it clearly indicates that the actual value of the double ionization cross section is higher than expected.

DOI
10.1103/physreva.78.023415

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We report on the experimental estimation of a lower bound of helium. Our experiment differs from a previous one described by Hasegawa et al. [Phys. Rev. A 71, 023407 (2005)]. The photons that correspond to the 27th harmonic of a Ti:sapphire laser have an energy of 41.8eV41.8\phantom{\rule{0.3em}{0ex}}\mathrm{eV}41.8eV. The extraction of the cross section rests on a theoretical model, based on the rate equations, that fully includes the contribution from the sequential channels and the macroscopic effects. Some of the experimental parameters are very difficult to measure accurately. For those parameters, we deliberately consider values compatible with their experimental determinations and that lead systematically to an underestimation of the two-photon double ionization cross section. Our estimation of this lower bound is higher than a bunch of various theoretical results. It stays, however, too close to these latter ones to draw any definite conclusion about their validity, even though it clearly indicates that the actual value of the double ionization cross section is higher than expected.
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 (54.4eV)(54.4\phantom{\rule{0.3em}{0ex}}\mathrm{eV})(54.4eV), sequential ionization competes with nonsequential ionization. Remarkably, even below 54.4eV54.4\phantom{\rule{0.3em}{0ex}}\mathrm{eV}54.4eV, 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.
A joint experimental and theoretical study of three-photon ionization of the 1s2p3Po1s2p{\phantom{\rule{0.16em}{0ex}}}^{3}{P}^{o}1s2p3Po(${M}_{L}=0,\ifmmode\pm\else\textpm\fi{}1$) states of helium is presented. The ion yield is recorded in the 690--730 nm wavelength range for different laser pulse energies, using an excited helium beam produced by photodetachment of helium negative ions. Two series of asymmetric peaks due to two-photon resonances with 1snp1snp1snp and 1snf1snf1snf Rydberg states are observed. In one series, the peaks have tails towards higher frequencies, while in the other series the tails change direction for higher Rydberg states. An effective Hamiltonian is built in the dressed state picture, and a numerical model simulating the traversal of the helium atom across the laser pulse is developed. The simulated and observed ion yields are in good qualitative agreement. The observed behavior is shown to result from the contributions of two different resonantly enhanced multiphoton ionization processes, depending on the magnetic quantum number ML{M}_{L}ML​ of the initial state. The asymmetry reversal is explained by the strong 1s2p1s2p1s2p--1s3s1s3s1s3s dynamic Stark mixing for ML=0{M}_{L}=0ML​=0.
We present a quantitative theory with detailed calculations pertaining to multiphoton ionization of helium under moderately strong uv radiation of photon energy 13eV13\phantom{\rule{0.3em}{0ex}}\mathrm{eV}13eV. Employing both, the nonperturbative solution of the time-dependent Schr\"odinger equation, as well as perturbation theory, we obtain detailed results for all processes expected to be of quantitative relevance within the range of intensities and pulse durations in this work, which have been chosen so as to match the conditions of a recent experiment on exactly this problem [T. Laarman et al., Phys. Rev. A 72, 023409 (2005)]. The conclusion, in connection with the experimental data, which our results lead to is that, without the presence of the second harmonic of the fundamental in the radiation, it is impossible to reconcile the reported observations with fundamental features of the processes involved. A more general conclusion seems to be that the presence of these harmonics, even at intensities less than 1% of that of the fundamental, are apt to produce profound side effects that will mask multiphoton processes by the fundamental.
We study resonant two-color two-photon ionization of helium via the 1s3p (1)P(1) state. The first color is the 15th harmonic of a tunable Ti:sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the phase of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.
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We investigate the two-photon double ionization of beryllium atom induced by ultrashort pulses. We use a time-dependent formalism to evaluate the ionization amplitudes and generalized cross sections for the ejection of the 2s22{s}^{2}2s2 valence shell electrons in the presence of a fully occupied 1s21{s}^{2}1s2 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 Be+(2p){\mathrm{Be}}^{+}(2p)Be+(2p) determines the profiles and pulse-duration dependencies of the energy and angle differential yields.