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Physical Review A

Stark dynamics of two-electron atoms probed by scaled energy spectroscopy

Jeremy Murray-Krezan, J. Kelly, Mary R. Kutteruf, R. R. Jones

Published Jan 2, 2007• 8 citations
Publisher

Abstract

Orbital dynamics in two-electron alkaline earth atoms in a static electric field are studied using scaled-energy recurrence spectroscopy. Photoabsorption spectra for Ba and Ca Rydberg atoms are measured as continuous functions of static electric field and energy. In both Ba and Ca the laser excitation proceeds through the singly excited $nd$ series which is strongly perturbed by doubly excited valence configurations. Clear signatures of the two-electron dynamics associated with these perturbing configurations are identified.

DOI
10.1103/physreva.75.013401

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Orbital dynamics in two-electron alkaline earth atoms in a static electric field are studied using scaled-energy recurrence spectroscopy. Photoabsorption spectra for Ba and Ca Rydberg atoms are measured as continuous functions of static electric field and energy. In both Ba and Ca the laser excitation proceeds through the singly excited ndndnd series which is strongly perturbed by doubly excited valence configurations. Clear signatures of the two-electron dynamics associated with these perturbing configurations are identified.
Coherent short-pulse laser excitation has been used to control the approximate energy and relative proximity of two valence electrons within the same alkaline-earth atom, thereby providing insight into the dynamical evolution of a three-body Coulomb system. Our time-domain experiments enable direct experimental study of the electron dynamics at the classical limit of a two-electron atom. As an example, we look at the mechanism of autoionization for one two-electron configuration class and find that the doubly excited atom decays through a single violent electron-electron collision rather than a gradual exchange of energy between the electrons.
We observe strong energy-dependent quantum defects in the scaled-energy Stark spectra for | M | = 1 Rydberg states of barium atoms at three scaled energies: ε = –2.000, ε = –2.500 and ε = –3.000. In an attempt to explain the observations, theoretical calculations of closed orbit theory based on a model potential including core effect are performed for non-hydrogenic atoms. While such a potential has been uniformly successful for alkali atoms with a single valence electron, it fails to match experimental results for barium atoms in the 6snp Rydberg states with two valence electrons. Our study points out that this discrepancy is due to the strong perturbation from the 5d8p state, which voids the simple approximation for constant quantum defects of principle quantum number n.
We observe strong energy-dependent quantum defects in the scaled-energy Stark spectra for vertical bar M vertical bar = 1 Rydberg states of barium atoms at three scaled energies: epsilon = -2.000, epsilon = -2.500 and epsilon = -3.000. In an attempt to explain the observations, theoretical calculations of closed orbit theory based on a model potential including core effect are performed for non-hydrogenic atoms. While such a potential has been uniformly successful for alkali atoms with a single valence electron, it fails to match experimental results for barium atoms in the 6snp Rydberg states with two valence electrons. Our study points out that this discrepancy is due to the strong perturbation from the 5d8p state, which voids the simple approximation for constant quantum defects of principle quantum number n.
In this work radiative properties of neutral elements with one or two electrons outside closed subshells have been investigated. Using laser techniques in connection with atomic beams selective excitation of Rydberg states was performed. Most of the studied states were populated with two-step excitation. Some states were reached directly from the ground state or from a metastable state and occasionally two-photon absorption was used. The excitation sometimes involved the use of frequency-doubling and Raman- shifting techniques. By time-resolved detection of the decay light from an excited state, primarily information on the radiative lifetime is obtained. With two different experimental arrangements radiative lifetimes in several Rydberg states have been determined. Using the quantum-beat technique time-resolved detection also provides information on energy splittings. This technique was used to measure hyperfine-structure splittings.To obtain information about hyperfine-structure constants and isotope shifts high- resolution spectroscopy on a collimated atomic beam was also employed. The behaviour of highly excited alkali atoms is mostly hydrogen- like and well predicted by theory. Group III A elements have one electron outside a closed subshell and are expected to behave like alkali atoms. The situation is however complicated by the presence of doubly excited states. Configuration interaction can then cause a partial mixing between singly and doubly excited states. In the alkaline-earth atoms (group II A elements), having two electrons outside closed shells, the situation is similar. In a Rydberg series of one excited electron the admixture of doubly excited states can cause large deviations from hydrogenic behaviour. Another complication in the alkaline-earth atoms is the mixture of singlet- and triplet states. - 4 - The presented results from measurements made on Na, Mg, Ca, Sr, Ba, Al, Ga and In will primarily serve as a basis for tests of modern atomic-physics models. Some of the lifetime values are also of astrophysical interest. Keywords: Laser spectroscopy, Rydberg states, time resolved, high resolution, two-step excitation, metastable state, two-photon absorption, frequency doubling, Raman shifting, radiative lifetime, quantum beat, hyperfine structure, isotope shift, Stark shift, alkali atoms, group III A elements, alkaline-earth atoms, configuration interaction, singlet-triplet mixing.
In the past years, scaled energy spectroscopy is under active investigation because this method can simplify the analysis of atomic spectra in the external field based on classic mechanics. A fully computer-controlled experimental system to study the constant scaled-energy spectroscopy was established and described in this paper. The excitation energy E and the strength of the external electric field F were controlled synchronously to keep the scaled-energy epsilon = E/square root of F constant. With this system, constant scaled-energy spectra of Strontium Rydberg atoms at epsilon = -3.0 in a static electric field were successfully recorded for the first time, and the recurrence spectra were obtained by a Fourier transform.
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 ${({n}^{*})}^{\ensuremath{-}3}$ 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 $n{d}^{\ensuremath{'}}$ 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.