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Topical Meeting on Laser Techniques in the Extreme Ultraviolet

Frequency Conversion Processes in Hydrogen

Yves Gontier, M. Trahin

Published Jan 1, 1982• 0 citations
Publisher

Abstract

Multiphoton Raman-like transitions taking place above and below the ionization threshold of an atom can be useful for generating energetic photons of well-defined energies. In these processes, the atomic electron makes a bound-bound transition. It first absorbs N photons of the incoming light and then reemits a photon whose energy depends on N and on the discrete final state.

DOI
10.1364/euvs.1982.mb2

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Multiphoton Raman-like transitions taking place above and below the ionization threshold of an atom can be useful for generating energetic photons of well-defined energies. In these processes, the atomic electron makes a bound-bound transition. It first absorbs N photons of the incoming light and then reemits a photon whose energy depends on N and on the discrete final state.
Transition amplitudes corresponding to bound-bound multiphoton transitions with the emission or absorption of one and two Raman photons in the hydrogen atom have been evaluated following a recent method of Reiss. Results show that the transition probability varies smoothly for low values of NNN, where NNN is the number of intense photons absorbed or emitted during the transition. For larger values of NNN the amplitude, however, has oscillatory behavior. A particular feature of the present method of calculation is that we find the "reduced" transition amplitude for induced emission of two Raman photons is enhanced compared with single-Raman-photon emission. Another distinctive feature is the appearance of many more extrema in the transition amplitude for higher transitions for multiphoton processes at high intensity.
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.
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
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
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.