On the basis of the generalized Sturm expansion of the radial part of the Coulomb Green function, a computational method is proposed and numerical results are presented for the dynamic hyperpolarizability γ and the corrections E (4) (quadratic in the light intensity) to the quasi-energy of the ground and excited states of hydrogen with principal quantum numbers n≤5 in a monochromatic light field. In this approach, the problem is reduced to the summation of well-convergent double series of the hypergeometric kind, which ensures reliable numerical results both for states with a large n, and in a wide range of field frequencies ω, including the above-threshold frequency range of ℏω≪|E n | (|E n | is the ionization potential of the state |nlm〉 under investigation). We consider the frequency dependence of γ and E (4), their differences for the cases of linear and circular polarizations of the field, and the relation between their real and imaginary parts, which determine the laser field-induced corrections to the position and width of energy levels. For n=5, the significant role of mixing the |nlm〉 states with different values of l by a laser field in the region of resonances on intermediate bound states is demonstrated. The linear (in intensity) corrections to the photoionization cross section for excited states are analyzed and the threshold intensity corresponding to the onset of atomic level stabilization is estimated for a number of states with n=3 and n=5.
Our recent analysis [J. Phys. B 33, R141 (2000)] of the problem of ${\mathrm{H}}^{\ensuremath{-}}$ in both laser and strong static electric fields, which treated effects that are linear in the laser intensity I (e.g., the dynamic polarizability and the single-photon detachment cross section), is extended here to treat effects of higher order $(\ensuremath{\sim}{I}^{2})$ in the laser intensity (e.g., the dynamic hyperpolarizability, the two-photon detachment cross section, the linear in I corrections to the single-photon detachment rate, etc). We introduce the concept of the dynamic hyperpolarizability of an atom in the presence of a strong electric field based on the complex quasienergy approach with properly normalized, quasistationary quasienergy wave functions. Our analysis of the general structure of the dynamic hyperpolarizability tensor of an atom in a nondegenerate
(S-) state is performed for arbitrary field geometries and laser polarizations. The connection of the hyperpolarizability $\ensuremath{\gamma}(\mathcal{F};\ensuremath{\omega})$ to the complex quasienergy and to atomic ionization rates is established. Analytic results (in terms of Airy functions) are obtained for five irreducible components of a hyperpolarizability tensor (that are independent of the laser polarization and the field geometry) for the case of a weakly bound electron in a three-dimensional, zero-range potential. These results are used for the analysis of the frequency, field geometry, and laser polarization dependence of the two-photon detachment rate as well as of the linear in laser intensity corrections to the single-photon detachment rate. It is shown that the oscillatory behavior of the frequency dependence of both the real and the imaginary parts of $\ensuremath{\gamma}(\mathcal{F};\ensuremath{\omega})$ exists for both the coplanar and orthogonal field geometries, and that this behavior is qualitatively different for frequencies below and above the single-photon detachment threshold. The threshold behavior of the two-photon detachment rate is analyzed in detail and the static electric-field-induced modification of Wigner's threshold law for a short-range potential is discussed.
The stimulated radiative corrections (or ac-Stark shift, or light shift...) of the energy levels of a hydrogenic atom irradiated by an intense, nonresonant, monomode laser field, are evaluated within the framework of the time-dependent perturbation theory, up to and including fourth order. The calculation is performed by using a Sturmian representation of the Coulomb Green's function. Whenever it is possible, comparison is made with other results, and several limiting cases are considered. If the laser frequency $\ensuremath{\omega}\ensuremath{\rightarrow}0$, one recovers the results of the dc-Stark effect. If $2\ensuremath{\omega}$ becomes larger than the ionization energy of the atomic state considered, the fourth-order level shift acquires an imaginary part which may be connected, via an extension of the optical theorem, to the two-photon ionization cross section. We point out also the difficulties encountered, when trying to get sensible estimates from partial summation of the infinite sums entering the perturbative expression of the fourth-order amplitudes. Finally, the order of magnitude of these various corrections is discussed.
General equations are presented for determining the field-dependent variation of the wavefunctions, matrix elements and intensities of dipole transitions between Stark levels of a hydrogen atom in a field range where the fine-structure effects may be neglected. The Sturm-series resolution for the reduced Coulomb-Green function is used to derive analytical expressions for the first-order corrections in terms of parabolic quantum numbers of initial and final states. Simple forms of these expressions as functions of the upper-state quantum numbers are presented explicitly for the Lyman and Balmer series. The selective action of the dc electric field on the intensity of Stark components of hydrogen lines is revealed in numerical calculations for both and types of emitted radiation. This selectivity may cause, in particular, enhancement of the high-frequency and damping of the low-frequency Stark -lines of the Lyman series.
Hydrogenic spectra A good starting point is photoexcitation from the ground state of H. The problem naturally divides itself into two regimes: below the energy of classical ionization limit, where the states are for all practical purposes stable against ionization, and above it where the spectrum is continuous. As an example, we consider first the excitation of the n = 15 Stark states from the ground state in a field too low to cause significant ionization of n = 15 states. From Chapter 6 we know the energies of the Stark states, and we now wish to calculate the relative intensities of the transitions to these levels. One approach is to calculate them in parabolic coordinates. This approach is an efficient way to proceed for the excitation of H; however, it is not easily generalized to other atoms. Another, which we adopt here, is to express the n = 15 nn 1 n 2 m Stark states in terms of their nℓm components using Eqs. (6.18) or (6.19) and express the transition dipole moments in terms of the more familiar spherical n ℓ m states. In the excitation of the Stark states of principal quantum number n from the ground state only p state components are accessible via dipole transitions, so the relative intensities for light polarized parallel and perpendicular to the static field, π and σ polarizations, are proportional to the squared transformation coefficients |〈 nn 1 n 2 m | n ℓ m 〉| 2 from the nn 1 n 2 m parabolic states to the n ℓ m states for ℓ = 1 and m = 0 and 1. In Fig. 8.1 we show the relative intensities by means of the squared transformation coefficients |〈15 n 1 n 2 m |15 p m 〉| 2 for m = 0 and 1.
The Stark spectroscopy of the hydrogen atom has been investigated near the ionization threshold in static homogeneous external electric fields from \ensuremath{\sim}1000 to \ensuremath{\sim}8000 V/cm with use of a two-step excitation H(n=1)+\ensuremath{\Elzxh}${\ensuremath{\omega}}_{\mathrm{vuv}\ensuremath{\rightarrow}}$H(n=2)+\ensuremath{\Elzxh}\ensuremath{\omega} $_{\mathrm{uv}\ensuremath{\rightarrow}}$
H∗ with vuv and uv laser radiation, independently tunable and linearly polarized either parallel (\ensuremath{\pi}) or perpendicular (\ensuremath{\sigma}) with respect to the external field. Different from other, nonhydrogenic atoms, the hydrogen atom is a peculiar case insofar as the initial states of H(n=2), from which excitation takes place, are essentially of parabolic character at the field strengths employed in this study.Individual sublevels (
n1,
n2,\ensuremath{\Vert}
ml\ensuremath{\Vert}) have been prepared in the n=2 state with sub-Doppler resolution. Photoionization spectra have been obtained with \ensuremath{\pi}- and \ensuremath{\sigma}-polarized uv radiation from the four possible sublevels of the n=2 Stark manifold: \ensuremath{\Vert}1,0,0〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉, \ensuremath{\Vert}0,1,0〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉, \ensuremath{\Vert}0,0,\ifmmode\pm\else\textpm\fi{}1〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉, and \ensuremath{\Vert}0,0,\ensuremath{\mp}1〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉. All spectra show sharp line structures of quasistable field-ionizing states superimposed on continua in the energy region between the classical saddle point, ${E}_{\mathrm{SP}=\mathrm{\ensuremath{-}}2\phantom{\rule{0ex}{0ex}}\mathrm{\ensuremath{\surd}}\mathrm{F}}$ a.u., and the zero-field ionization threshold E=0 a.u. Employing existing theoretical treatments, the quasistable spectral structures are quantitatively completely analyzed and accounted for, as long as their field ionization rate is less than \ensuremath{\sim}5\ifmmode\times\else\texttimes\fi{}
1011 ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$. Field-ionization rates of quasistable states have been measured and are compared with theory. Oscillatory resonance structures of the ionization cross section near the zero-field threshold are observed with pronounced modulation degree only in the spectrum from the \ensuremath{\Vert}1,0,0〉 \ensuremath{\Vert}\ifmmode\pm\else\textpm\fi{}1/2〉 sublevel excited with the uv \ensuremath{\pi}-polarized. The energy spacing of the oscillations has been measured as a function of the electric field strength F and found to be nearly proportional to
F3/4, with slight but definite deviations. Theoretical analysis of the oscillations yields quantitative agreement with the experiment.
The dichroic effects in the multiphoton ionization of the ground state hydrogen atom by a coherent superposition of a laser beam and its third harmonic, are studied via perturbative calculations. The final state of the photoelectrons, which has the energy E = E 1 + 3ℏω ( E 1 the ground state energy and ω the laser frequency), is reached by two interfering quantum paths: (a) absorption of one harmonic photon and (b) absorption of three laser photons. In the chosen regime of field intensities, the radiative corrections to the absorption of one harmonic photon may be disregarded. Our numerical results illustrate the influence of the laser frequency, of the relative intensity and of the harmonic phase upon the dichroic signal.