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Physical Review A

Multiphoton Ionization of Atomic and Molecular Hydrogen at 0.53 μ

M. LuVan, G. Mainfray, C. Manus, I. I. Tugov

Published Jan 1, 1973• 64 citations
Publisher

Abstract

This work reports multiphoton ionization and dissociation of molecular hydrogen under the influence of laser radiation at 0.53 $\ensuremath{\mu}$. The six-photon ionization probability of hydrogen atoms is derived for laser radiation acting upon atomic hydrogen from a molecular hydrogen beam which is up to 80% dissociated by radio-frequency power. The experimental six-photon ionization probability of atomic hydrogen has been found to be in good agreement with the corresponding probability calculated using time-dependent perturbation theory if the statistical properties of the incident light are taken into account.

DOI
10.1103/physreva.7.91

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This work reports multiphoton ionization and dissociation of molecular hydrogen under the influence of laser radiation at 0.53 \ensuremathμ\ensuremath{\mu}\ensuremathμ. The six-photon ionization probability of hydrogen atoms is derived for laser radiation acting upon atomic hydrogen from a molecular hydrogen beam which is up to 80% dissociated by radio-frequency power. The experimental six-photon ionization probability of atomic hydrogen has been found to be in good agreement with the corresponding probability calculated using time-dependent perturbation theory if the statistical properties of the incident light are taken into account.
The resonantly enhanced multiphoton ionization of atomic hydrogen is studied for the case of four-photon ionization (three-photon resonant). The time-dependent probabilities, the shape of the resonance profile at different intensities, and the nonlinear index are computed for coherent light at frequencies around the resonance (365 nm). The systematic dependence of the cross section as a function of the principal quantum number of the resonant state (as this tends towards the Rydberg states) is investigated at zero detuning. The probabilities of absorption of one photon more than necessary for the four-photon ionization process (resonantly enhanced above-threshold ionization) is computed and the relevant branching ratios are examined. Then it is shown that the effect of the spatio-temporal structures of the laser pulse is to red shift the maximum of the resonance profile, whereas that of an ideal chaotic light is to blue shift and broaden the resonance peak. The shape, shift, and width of the profile resulting from both these effects are in very fair agreement with the experimental ones.
A perturbation theory of the ionization of atoms by simultaneous absorption of several photons, each of whose energy is less than the ionization potential, is developed from the evolution-operator formalism. A precise computation is made for the hydrogen atom, giving transition rates as a function of photon energy for two- through twelve-photon photoionization. The eighth-order ionization rate (in cgs units) at the 1.78-eV ruby-laser line is found to be \ensuremath{\sim}${10}^{\ensuremath{-}244}$\ifmmode\times\else\texttimes\fi{}(photonflux)8{(\mathrm{photon}\mathrm{flux})}^{8}(photonflux)8 and should be observable using available techniques. Good agreement is obtained with Zernik's exact calculation of the two-photon ionization rate of metastable 2S2S2S hydrogen. Approximate calculations are made for the rare gases. Assuming "typical" experimental conditions of a gas density of \ensuremath{\sim}1020{10}^{20}1020 atoms ${\mathrm{cm}}^{\ensuremath{-}3}$ and a ruby laser focused into a volume of \ensuremath{\sim}${10}^{\ensuremath{-}8}$ cm3{\mathrm{cm}}^{3}cm3, we find that the flux required to liberate one electron during a 10-nsec pulse is \ensuremath{\sim}1029{10}^{29}1029 ${\mathrm{cm}}^{\ensuremath{-}2}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ for Xe, Kr, and Ar and \ensuremath{\sim}5\ifmmode\times\else\texttimes\fi{}1030{10}^{30}1030 photons ${\mathrm{cm}}^{\ensuremath{-}2}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ for Ne and He. These gases ionize with the simultaneous absorption of 7, 8, 9, 13, and 14 photons, respectively. The predicted rate for Xe is found to be in excellent agreement with the recent direct measurements of Voronov and Delone. We conclude that multiphoton ionization provides the initial electrons required for the optical breakdown of gases, though it does not account for the over-all growth of the discharge except possibly at very low pressures. Impurity atoms (particularly heavy rare gases) may be the source of "initiating" electrons in Ne and He.
We have discussed the problems of non linear interaction between electromagnetic radiations with atoms from semi-classical point of view. Time dependent Schrödinger equation for single electron system is solved by using perturbative technique to obtain transition probability. Higher order perturbation is also discussed which is used in multiple processes, in which two or more quanta are emitted instead of a single photon. The theory is based on assumption that the perturbation is small. From this transition probability ionization rate and absorption cross-section of hydrogen atom is calculated. Its variation with photon energy and field strength is analyzed which agrees very well with experimental observations.The Himalayan PhysicsVol. 3, No. 32012Page : 40-43
Within the framework of time-dependent perturbation theory, general expressions are derived for the cross section of multiphoton processes induced by radiation acting on a hydrogen atom. Bound-bound transitions involving emission of a single quantum and bound-free transitions are calculated for a wide range of photon energies. In the case of resonance, the transition probability is also discussed. The procedure used to evaluate the sums over intermediate states is described. The numerical computation allows one to compare the results obtained for various competing processes.
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.