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Physical Review A

Investigation of the Stark effect in krypton autoionizing Rydberg series with the use of two-step laser excitation

Christian Delsart, Jean-Claude Keller

Published Aug 1, 1983• 26 citations
Publisher

Abstract

The first detailed observation of the perturbations by an electric field of the Rydberg autoionizing resonances of a rare-gas atom is reported. The Stark spectroscopy of autoionizing Rydberg states converging to the second ionization limit $4{p}^{5}^{2}P_{\frac{1}{2}}^{o}$ in Kr I is performed in an atomic beam with the use of a two-step laser excitation from the $4{p}^{5}5s{[\frac{3}{2}]}_{2}^{0}$ metastable state. In addition to the verification of the ${({n}^{*})}^{\ensuremath{-}3}$ dependence of the zero-field width of two autoionizing series and of the linear dependence of the Stark-manifold splittings with the electric field, we have observed an ${(n)}^{0.7}$ law for the dependence of the Stark-manifold splitting along the series, an important narrowing and dissymmetrization of the $n{d}^{\ensuremath{'}}$ resonances, and a nonlinear-field behavior of Stark-manifold components in the vicinity of the first anticrossing. Discussions are carried out with the use of the recent work on Rydberg-Stark spectroscopy and on autoionizing states in two-electron atoms.

DOI
10.1103/physreva.28.845

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Acta Physica Sinica•Jan 1, 1995•0 citations
The first detailed observation of the perturbations by an electric field of the Rydberg autoionizing resonances of a rare-gas atom is reported. The Stark spectroscopy of autoionizing Rydberg states converging to the second ionization limit 4{p}^{5}^{2}P_{\frac{1}{2}}^{o} in Kr I is performed in an atomic beam with the use of a two-step laser excitation from the 4p55s[32]204{p}^{5}5s{[\frac{3}{2}]}_{2}^{0}4p55s[23​]20​ metastable state. In addition to the verification of the (n∗)\ensuremath−3{({n}^{*})}^{\ensuremath{-}3}(n∗)\ensuremath−3 dependence of the zero-field width of two autoionizing series and of the linear dependence of the Stark-manifold splittings with the electric field, we have observed an (n)0.7{(n)}^{0.7}(n)0.7 law for the dependence of the Stark-manifold splitting along the series, an important narrowing and dissymmetrization of the nd\ensuremath′n{d}^{\ensuremath{'}}nd\ensuremath′ resonances, and a nonlinear-field behavior of Stark-manifold components in the vicinity of the first anticrossing. Discussions are carried out with the use of the recent work on Rydberg-Stark spectroscopy and on autoionizing states in two-electron atoms.
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.
We have studied the Stark effect for the bound Rydberg states of xenon (2{(}^{2}(2P3/2{\mathrm{P}}_{3/2}P3/2​ core) in the vicinity of n=17. These are the first detailed measurements of Rydberg-state Stark structure in a heavy rare-gas atom. The experiment was performed by one-photon laser spectroscopy from the metastable 6s'[(1/2)]0{[(1/2)]}_{0}[(1/2)]0​ state in an atomic beam. Laser polarization can be chosen to excite pure M=0 or \ensuremath{\Vert}M\ensuremath{\Vert}=1 levels. Stark maps are presented for electric fields from 0 to 2000 V/cm. The major low-field features are a prominent linear manifold for states with l\ensuremath{\ge}3 and an isolated group of states arising from mixing within the overlapping p and d terms. A simple model of the p,d complex, showing strong mixing at fields as low as 200 V/cm, is used to correlate observed states with the zero-field states. The spectra become exceedingly complex for fields greater than 1000 V/cm because of mixing within the extensive fine structure of xenon.
We report the first observation of significant perturbations by external fields of the autoionizing resonance structure of a two-electron atoms. The effects of electric fields up to 20 kV/cm on autoionizing resonances in Sri were observed by three-photon ionization spectroscopy in an atomic beam. In addition to effects analogous to those for bound Stark states of a one-electron Rydberg atom, we observed a new effect: The characteristic shapes and widths of autoionizing resonances (Fano-Beutler profiles) can be strongly influenced by electric fields.
We present a study of a cold strontium Rydberg gas. The narrowband laser excitation of Rydberg states in the range n = 20–80 from a 6 mK cloud of strontium atoms is detected using the spontaneous ionization of the Rydberg atoms. Using a high-resolution step-scanning technique, we perform detailed measurements of the Stark maps of selected Rydberg states. We find excellent agreement between the measured Stark maps and a numerical calculation based on an independent electron model. Finally we show that excitation of the second valence electron can be used to probe the dynamics of the Rydberg gas with nanosecond temporal resolution via autoionization.
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.
The Stark spectra of Yb atom with m=0 and |m|=1 in the vicinity of n=17 to n=20 have been obtained by using two-step excitation and photoioni-zation method in the applied electric field from 0 to l500V/cm. The Stark splittings and shifts observed in the experiment have been calculated by using numerical integration method. The thoretical results are consistent generally with the experiments. The dependence of the anticrossings of Stark manifolds with quantum defects is investigated. The comparison between the m=0 and |m|=1 Stark structures is furnished.