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Laser-Atom Interaction at High Intensities

Thomas J. Mcilrath, C. W. Clark

Published May 20, 1991• 0 citations
OpenAlex

Abstract

A general program has been developed to calculate multiphoton processes in atomic hydrogen to arbitrarily high order in perturbation theory. This program can be used to calculate quantities in intense field multiphoton processes, such as the generalized cross section of multiphoton absorption, the a.c. Stark effect (shift and the broadening of the level due to the field interaction), and the parameters in nonlinear optics such as the nonlinear index of refraction and the nonlinear susceptibility. Effective parametrization of high-order susceptibilities has been achieved over a wide range of frequencies, utilizing concepts from quantum defect theory to express the results of lengthy calculations in a compact form that also permits extrapolation across thresholds and resonance poles. Significant progress has been made in direct numerical solution of the time-dependent Schroedinger equation. In addition, contributions have been made in: understanding the role of spatial dimensionality in the solution of model systems (e.G., the one-dimensional delta-function potential); the development of a general R-matrix code for perturbative computations of multiphoton processes in many-electron atoms; and multiphoton ionization with two commensurate laser frequencies.

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A general program has been developed to calculate multiphoton processes in atomic hydrogen to arbitrarily high order in perturbation theory. This program can be used to calculate quantities in intense field multiphoton processes, such as the generalized cross section of multiphoton absorption, the a.c. Stark effect (shift and the broadening of the level due to the field interaction), and the parameters in nonlinear optics such as the nonlinear index of refraction and the nonlinear susceptibility. Effective parametrization of high-order susceptibilities has been achieved over a wide range of frequencies, utilizing concepts from quantum defect theory to express the results of lengthy calculations in a compact form that also permits extrapolation across thresholds and resonance poles. Significant progress has been made in direct numerical solution of the time-dependent Schroedinger equation. In addition, contributions have been made in: understanding the role of spatial dimensionality in the solution of model systems (e.G., the one-dimensional delta-function potential); the development of a general R-matrix code for perturbative computations of multiphoton processes in many-electron atoms; and multiphoton ionization with two commensurate laser frequencies.
The variationally stable procedure for Nth-order perturbative-transition-matrix elements introduced by the authors [Phys. Rev. Lett. 61, 404 (1988)] is presented here in detail. Its key features are that it is noniterative, involves only two unknown functions regardless of the value of N, is stable even near intermediate-state resonances (due to the presence of energy numerators rather than energy denominators), and uses the inverse of the perturbation operator for N\ensuremath{\ge}3. Explicit formulas are presented for application to high-order multiphoton processes in atomic hydrogen. Numerical results for multiphoton-ionization cross sections (for two, three, and seven photons), for the frequency dependence of the nonlinear susceptibilities for harmonic generation (for the third, fifth, and seventh harmonics), and for harmonic-generation transition rates up to 11th order for \ensuremath{\lambda}=1064 nm are presented for the atomic hydrogen ground state and compared with results of others by more standard procedures. We also present detailed analyses of the Z scaling of our results for hydrogenic systems, of the use of the imaginary part of the appropriate 2N-photon nonlinear susceptibility to obtain N-photon-ionization cross sections, and of the relation of the variational principle presented here to variational principles for scattering processes of Nuttall and Cohen [Phys. Rev. 188, 1542 (1969)] and of Schwinger [Phys. Rev. 72, 742 (1947)].
The present paper applies the method of high-intensity quantum electrodynamics developed earlier to several problems of current experimental interest. In this paper the intensitydependent shifts and widths of atomic levels are calculated and applied to a given transition near resonance. The technique is demonstrated with three examples: the multiphoton ionization of atomic cesium and hydrogen in atomic beams and third-harmonic production in an atomic vapor. It is found that the multiphoton-ionization rate in a relatively weak laser beam (of order 108{10}^{8}108 W/cm2{\mathrm{cm}}^{2}cm2) is determined by the intensity-dependent level width (6f6f6f configuration) as well as the interference of the fine-structure states, and that the rates for hydrogen, in a much more intense beam (of order 1012{10}^{12}1012 W/cm2{\mathrm{cm}}^{2}cm2) are determined by both the intensity-dependent widths and shifts as‘\stackrel{\mathrm{`}}{\mathrm{s}}s‘ well as the wave-function renormalization constants. The agreement of these two examples of calculations with the experiments done recently is satisfactory. For third-harmonic production the role of two-photon resonance is emphasized, and the dependence of the generated third-harmonic intensity on the intensity and frequency of the fundamental is discussed. Near resonance, the ratio of third-harmonic intensity to fundamental intensity saturates.
The non linear interaction between an intense laser radiation and atoms leads to ionization through the absorption of N photons from the laser radiation via laser-induced virtual states. The multiphoton ionization rate varies as a function of the laser intensity I as IN. We discuss the two most important effects which govern multiphoton ionization processes : resonance effects and laser-coherence effects. In a moderate laser intensity range (107 - 109 W cm-2) corresponding to the two, three or four-photon ionization of atoms, resonance effects play a dominant role while the photon statistics of the laser radiation are relatively unimportant. On the contrary, in the very high intensity range (1012 - 1013 W cm-2) required to observe large Nth - order ionization processes, coherence effects play a dominant role through N! enhancement in the N-photon ionization rate, while resonance effects are completely damped due to the high laser intensity. We conclude by reviewing the possible applications of multiphoton absorption processes in other fields.
In the first part of this thesis, a new variational principle is presented for the calculation of perturbative transition amplitudes of any order but free from any singularities. Applications are made to the multiphoton ionization and harmonic generation for atomic hydrogen. Its formulations in hyperspherical coordinates as well as in Hartree-Fock representation are also presented. In the second part of this thesis, theories for multiphoton detachment in a static electric or magnetic field are developed. They are based on the analytic solutions of an electron in the combined field of a laser and a static electric or magnetic field, and, therefore, are nonperturbative in both the laser intensity and the static electric or magnetic field strength. Heretofore unexpected cyclotron resonances, which are due to the infinite range character of the electron-photon coupling induced by the external magnetic field, are shown to exist under certain conditions.
The infinite summations over the complete set of unperturbed atomic states appearing in the Nth-order time-dependent perturbation theory are performed using the Green's function formalism. In order to test the method extended calculations of the cross section for two- and three-photon ionization for atomic hydrogen are made and numerical comparison is shown with the values obtained by different methods. The resonant character of the process is made evident since the poles of the radial part of the Green's function represent the actual energy spectrum of the atom. The relevant transition matrix elements are written in closed form and then computed exactly without averaging over the intermediate states. The cross sections vanish for circularly polarized light near some energies which explains the form of the cross sections for circularly and linearly polarized light.
The infinite summations over the complete set of unperturbed atomic states appearing in the NNNth-order perturbation theory for multiphoton ionization are performed using the Dalgarno-Lewis method. The relevant transition matrix elements are written in a closed integral form exhibiting all the analytic properties of the amplitude as a function of incident photon energy. The cross sections for two- and three-photon ionization for atomic hydrogen are calculated for both linearly and circularly polarized light with a wide range of photon energy spectrum including the near resonance, and numerical comparison is made with the values obtained by different methods.