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Le Journal de Physique Colloques

CONTINUUM STARK SPECTROSCOPY

Louis F. DiMauro, T. H. Bergeman, Patrick J. McNicholl, H. Metcalf

Published Nov 1, 1982• 3 citations
Publisher

Abstract

We have studied experimentally and theoretically two-step photoionization through the 3P state of sodium in an electric field of up to 3.90 kV/cm. The apparatus uses an atomic beam crossed by two pulsed laser beams, one at 589 nm for the first step, and the other swept through the zero field threshold Eo near 409 nm for the ionization. We observe broad undulations in the photocurrent above Eo that narrow with decreasing energy and eventually sharpen into well-defined but asymmetric transitions to Stark-shifted Rydberg states. We calculate the oscillator strength density for the appropriate transitions using modified hydrogenic wave functions and find excellent agreement for the position and relative strength of all the spectral features. We model the asymmetries as Fano-type interferences between quasi-discrete and continuum ionization channels. Using appropriate core potentials, and taking into account core-induced coupling of both discrete-to-continuum and continuum-to-continuum states, we obtain estimates of Fano's q and Ɖ that agree reasonably well with our measurements.

DOI
10.1051/jphyscol:1982213

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Physical Review A•Jun 1, 1988•78 citations
We have studied experimentally and theoretically two-step photoionization through the 3P state of sodium in an electric field of up to 3.90 kV/cm. The apparatus uses an atomic beam crossed by two pulsed laser beams, one at 589 nm for the first step, and the other swept through the zero field threshold Eo near 409 nm for the ionization. We observe broad undulations in the photocurrent above Eo that narrow with decreasing energy and eventually sharpen into well-defined but asymmetric transitions to Stark-shifted Rydberg states. We calculate the oscillator strength density for the appropriate transitions using modified hydrogenic wave functions and find excellent agreement for the position and relative strength of all the spectral features. We model the asymmetries as Fano-type interferences between quasi-discrete and continuum ionization channels. Using appropriate core potentials, and taking into account core-induced coupling of both discrete-to-continuum and continuum-to-continuum states, we obtain estimates of Fano's q and Ɖ that agree reasonably well with our measurements.
We observed well-resolved spectral features in the stepwise ionization of Na in an applied electric field near the zero-field ionization threshold. A 5890-A pulse excites atoms to the 32P3^{2}P32P state and a~4085-A pulse, swept through threshold ionizes them. Using the method of Luc-Koenig, we calculated the oscillator strength density versus blue laser frequency and compared it with our data. The agreement is excellent. Parabolic quantum numbers have been assigned to the spectrum and the Fano profiles have been analyzed.
Nous présentons l'étude expérimentale et théorique de la photoionisation par échelon via l'état 3P du sodium dans des champs électriques jusqu'à 3,90 kV/cm. L'appareillage utilise un jet atomique et l'excitation est réalisée à l'aide de deux lasers pulsés dont les faisceaux sont orthogonaux au jet atomique. Le premier laser à 589 nm permet l'excitation des niveaux P. Le second laser autour de 409 nm permet la photoionisation autour de la limite d'ionisation Eo, en champ nul. Nous avons observé des ondulations de grande largeur dans le courant photoélectrique au-delà de Eo. Leur largeur décroit lorsque l'énergie décroit. Dans certains cas elles s'affinent en des raies bien définies mais asymétriques correspondant aux états de Rydberg déplacés par effet Stark. Nous avons calculé la densité de force d'oscillateur pour ces transitions en utilisant des fonctions d'ondes hydrogénoïdes modifiées. L'accord avec les résultats expérimentaux est excellent. Nous avons considéré les asymétries comme le résultat d'interférences de Fano entre la partie quasi-discrète du spectre et les canaux d'ionisation. En utilisant des potentiels du coeur appropriés, et en tenant compte du couplage entre états discrets-continus et continus-continus induits par l'interaction avec le coeur, nous avons obtenu des valeurs q et Ɖ des paramètres de Fano en bon accord avec nos mesures.
Stark spectra of barium Rydberg states above the classical field-ionization limit have been recorded at high density of states employing high-resolution laser spectroscopy. The spectra, taken at a binding energy of about \ensuremath{\varepsilon}\ensuremath{\approxeq}-55 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ with respect to zero-field threshold and at electric-field strengths F\ensuremath{\approxeq}100 V/cm exhibit dramatic variations in line profiles with increasing external field strength. The WKB quantum-defect theory of the Stark effect of nonhydrogenic atoms was used to analyze the recorded spectra, and excellent agreement between measured and calculated line profiles was achieved. Core-induced coupling of closed and open hydrogenic Stark channels was found to contribute dominantly to the linewidth of the recorded Stark resonances. In addition, a reformulation of this theory by McNicholl, Ivri, and Bergeman (unpublished) in terms of a configuration-interaction model was employed to analyze a particular avoided crossing of several Stark components. In this way recorded line profiles were parametrized within a limited model to obtain resonance energies, linewidths, and Fano q parameters.
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∗{\mathrm{H}}^{\mathrm{*}}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{n}_{1}n1​,n2{n}_{2}n2​,\ensuremath{\Vert}ml{m}_{l}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{10}^{11}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{F}^{3/4}F3/4, with slight but definite deviations. Theoretical analysis of the oscillations yields quantitative agreement with the experiment.
The Stark spectra of autoionizing Rydberg states of Xe converging to the second ionization limit 5p5{p}^{5}p5 2P1/2^{2}P_{1/2}2P1/2​ have been investigated as a function of applied electric field over the range 26--2362 V/cm. Single-photon excitation from the Xe ground state was achieved using coherent radiation near 92.5 nm, generated by frequency tripling the pulsed output of a frequency-doubled dye laser in a free jet of rare-gas atoms. For the lowest electric field only the ns' and nd' series were observed. As the electric field was increased the np' series appeared because of the mixing of wave functions with different l values. Further increase of the electric field caused the appearance of hydrogenlike Stark manifolds. The Stark spectrum was simulated in a two-step procedure with no adjustable parameters. Using a jl-coupling basis set the Hamiltonian matrix was diagonalized to determine the energy levels and corresponding eigenfunctions for a given electric field strength. The intensities and line shapes were then calculated using the formalism developed by Fano for a many-discrete-level--single-continuum configuration interaction. This treatment was sufficient to reproduce the positions, widths, and shapes of most observed features. At field strengths between 1000 and 2000 V/cm, however, an additional modulation structure with a spacing of about 2.7 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ appeared on top of the \ensuremath{\Vert}M\ensuremath{\Vert}=1 autoionizing resonances, which could not be explained by our simple theoretical model.