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Physical Review A

Stark structure in Rydberg states of xenon

Randall D. Knight, Liangguo Wang

Published Aug 1, 1985• 30 citations

Abstract

We have studied the Stark effect for the bound Rydberg states of xenon ${(}^{2}$${\mathrm{P}}_{3/2}$ 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'${[(1/2)]}_{0}$ 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.

DOI: 10.1103/physreva.32.896

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We have studied the Stark effect for the bound Rydberg states of xenon

{(}^{2}$${\mathrm{P}}_{3/2}

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}

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.

The Stark spectra of autoionizing Rydberg states of Xe converging to the second ionization limit 5

{p}^{5}

^{2}P_{1/2}

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.

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.