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Physical Review A

Photoionization of the hydrogen atom near the ionization limit in strong electric fields

H. Rottke, K. H. Welge

Published Jan 1, 1986• 102 citations
Publisher

Abstract

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}}$${\mathrm{H}}^{\mathrm{*}}$ 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 (${n}_{1}$,${n}_{2}$,\ensuremath{\Vert}${m}_{l}$\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{}${10}^{11}$ ${\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}$. 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 ${F}^{3/4}$, with slight but definite deviations. Theoretical analysis of the oscillations yields quantitative agreement with the experiment.

DOI
10.1103/physreva.33.301

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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}\ensuremathωvuv\ensuremath→{\ensuremath{\omega}}_{\mathrm{vuv}\ensuremath{\rightarrow}}\ensuremathωvuv\ensuremath→​H(n=2)+\ensuremath{\Elzxh}\ensuremath{\omega} _{\mathrm{uv}\ensuremath{\rightarrow}}$${\mathrm{H}}^{\mathrm{*}} 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, ESP=\ensuremath−2\ensuremath√F{E}_{\mathrm{SP}=\mathrm{\ensuremath{-}}2\phantom{\rule{0ex}{0ex}}\mathrm{\ensuremath{\surd}}\mathrm{F}}ESP=\ensuremath−2\ensuremath√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 sec\ensuremath−1{\mathrm{sec}}^{\mathrm{\ensuremath{-}}1}sec\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 splitting of the second excited level of atomic hydrogen (with principal quantum number n=3n=3n=3) has been measured by pulsed laser spectroscopy in order to determine small electric fields by optical means. Doppler-free excitation with two counterpropagating laser beams at 205nm205\phantom{\rule{0.3em}{0ex}}\mathrm{nm}205nm allows us to measure the n=3n=3n=3 Stark spectra either by an optogalvanic signal after ionization by a third laser photon or by detection of the Balmer-$\ensuremath{\alpha}$ fluorescence photons emitted by the excited atoms. Three different cases of laser polarization have been investigated in order to evaluate the possibilities and limitations of this one-step laser excitation method for electric field determination, especially at field strengths below 200V∕cm200\phantom{\rule{0.3em}{0ex}}\mathrm{V}∕\mathrm{cm}200V∕cm. The method provides the best field sensitivity achieved with lower excited levels that can be reached directly by two-photon absorption from the ground state (in contrast to the more sensitive Rydberg levels). For this purpose, an advanced tunable pulsed uv laser with narrow bandwidth almost at the Fourier limit has been used. The high spectral resolution allowed us to deduce electric field strengths as small as 50V∕cm50\phantom{\rule{0.3em}{0ex}}\mathrm{V}∕\mathrm{cm}50V∕cm from the frequency shift between two selected isolated Stark components. As a main advantage, this simple analysis of the measured spectra does not rely on knowledge of the line intensities which may be strongly affected by the measuring conditions.
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.
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.
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We have measured certain ratios of transition intensities between excited hydrogen Stark sublevels over a range of electric-field values. CO2{\mathrm{CO}}_{2}CO2​ lasers were used to excite a fast beam of hydrogen atoms. The \ensuremath{\pi}-polarized transitions studied were from extremal Stark sublevels of principal quantum number n=10 to extremal and next extremal sublevels of n=30 and 44, at fields from 2 to 700 V/cm. The observed ratios are compared with those obtained using a non-relativistic zero-field formula attributed to Gordon [Ann. Phys. (Leipzig 2, 1031 (1929)] and with calculations employing matrix diagonalization including fine structure. Even for those relatively high n values, we find at low field significant deviations from results from Gordon's formula due to fine structure in the lower state as well as deviations at high field due to n mixing in the upper state induced by the static electric field. The experimental results and the matrix diagonalization calculations agree to within a few percent, which is the order of magnitude of possible saturation effects.
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