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Journal of the Optical Society of America B

High-frequency two-photon ionization of helium and cesium

M. Marinescu, H. R. Sadeghpour, A. Dalgarno

Published Jun 1, 1993• 9 citations
Publisher

Abstract

Calculations of the two-photon ionization of metastable levels of helium and the first three s levels of cesium are presented. The calculations are carried out to second order in a perturbation expansion and are valid for low laser intensities. The behavior of the ionization cross section at high photon frequencies ω is studied, and it is found that the N-photon ionization cross section behaves as σ(N) ∝ ω−(2N+1/2). This analytic asymptotic behavior is verified numerically in the case of two-photon ionization.

DOI
10.1364/josab.10.000988

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Calculations of the two-photon ionization of metastable levels of helium and the first three s levels of cesium are presented. The calculations are carried out to second order in a perturbation expansion and are valid for low laser intensities. The behavior of the ionization cross section at high photon frequencies ω is studied, and it is found that the N-photon ionization cross section behaves as σ(N) ∝ ω−(2N+1/2). This analytic asymptotic behavior is verified numerically in the case of two-photon ionization.
Multipole interference effects are predicted in the generalized cross sections, and in the ratio $\frac{{\stackrel{^}{\ensuremath{\sigma}}}_{C}}{{\stackrel{^}{\ensuremath{\sigma}}}_{L}}$ of the cross sections for circularly and linearly polarized laser light for the case of the two-photon ionization of the n=2n=2n=2 singlet metastable helium atoms in the wavelength range 5036-5050 \AA{}.
This paper discusses the general theory of two-photon ionization of a hydrogenic state in the nonrelativistic dipole approximation. An application is made to the photoionization of the metastable 2S2S2S state of atomic hydrogen by optical radiation, for example, by the light from a ruby laser. The sum over intermediate states is carried out exactly by means of an implicit technique. The results are given for a range of wave-lengths from the threshold at 7290 down to 4556 \AA{}. At 6943 \AA{}, the total cross section per unit intensity is found to be 5.35\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}29}$ cm4{\mathrm{cm}}^{4}cm4 ${\mathrm{W}}^{\ensuremath{-}1}$. The lowest order damping corrections to the perturbation-theory results are worked out.
There have been relatively few investigations of multiphoton ionization from metastable helium. Of particular interest has been the work of Haberland et al. 1987 and Haberland and Oschwald 1988. In both the 1987 and 1988 papers they have described the two photon ionization of metastable helium. In each of these studies they have reported the occurrence of unexplained structure along the wings of their resonance profiles. Upon the performance of similar measurements by this study, the unexplained structure is not seen and the agreement of the experiment's measurements with the theoretical shape of the resonance curves has been good. To experimentally verify these resonance effects, we have used a tunable dye laser in conjunction with a time of flight mass spectrometer to create and detect ions from metastable helium by two-photon absorption. The use of a metastable state instead of the ground state is advantageous because of its proximity to the ionization continuum and its extended lifetime. Using a metastable state as a starting point for multiphoton absorption requires fewer photons to reach the ionization threshold. The extended lifetime of the state also makes it easy to access experimentally. For helium the singlet metastable state 2$\sp1$S lies at 20.61 eV above the ground level with a natural lifetime of close to a millisecond. Two photons of 501.7 nm and 504.35 nm are required for the ionization processes in resonance with the 3$\sp1$P and the 3$\sp1$D states. This thesis is the accounting of the experimental process involved in the measurement of the dipole and quadrupole resonances of two photon ionization from singlet metastable helium. The study includes the description of the laser, electron gun assembly for metastable helium creation, and the time of flight mass spectrometer. A discussion of the theory of multiphoton processes is included along with the discussion of the data, its reduction and analysis, and a comparison with theoretical prediction. This study has not only involved the acquisition of definitive atomic spectra data sets, but has also established a facility for resonant ionization spectroscopy at The American University.
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.