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Journal of the Optical Society of America B

High-resolution Rydberg-state spectroscopy of stable alkaline-earth elements

R. Beigang

Published Dec 1, 1988• 6 citations
Publisher

Abstract

High-resolution Rydberg-state spectroscopy was applied to investigate high-lying Rydberg states of the alkaline-earth elements Mg, Ca, Sr, and Ba up to principal quantum numbers n > 200. In this energy range interactions dominate that are negligible at low n. It is shown that the hyperfine interaction can be used as a sensitive probe for configuration interactions, singlet–triplet mixing, and hyperfine-induced n mixing.

DOI
10.1364/josab.5.002423

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Journal of Physics B Atomic Molecular and Optical Physics•Jun 14, 1988•14 citations
High-resolution Rydberg-state spectroscopy was applied to investigate high-lying Rydberg states of the alkaline-earth elements Mg, Ca, Sr, and Ba up to principal quantum numbers n > 200. In this energy range interactions dominate that are negligible at low n. It is shown that the hyperfine interaction can be used as a sensitive probe for configuration interactions, singlet–triplet mixing, and hyperfine-induced n mixing.
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.
High-resolution two-photon spectroscopy was applied to investigate the msns 1S0^{1}S_{0}1S0​ Rydberg states of the alkaline-earth elements Ca, Sr, and Ba. It is shown for 43Ca^{43}\mathrm{Ca}43Ca, 87Sr^{87}\mathrm{Sr}87Sr, 135Ba^{135}\mathrm{Ba}135Ba, and 137Ba^{137}\mathrm{Ba}137Ba that the hyperfine interaction causes a level shift between odd- and even-mass isotopes. A theoretical interpretation is presented which relates the energy-level shift for odd isotopes to the singlet-triplet separation which in turn is a function of the principal quantum number, and good agreement with the experimental results is found.
We report precision spectroscopy of ionic-core transitions in alkaline-earth Rydberg atoms. We demonstrate high-resolution measurements of isotope shifts and hyperfine splitting of dipole transitions in ionic cores which have not been explored so far. A key element of this work is the reduction of the linewidth by more than two orders of magnitude enabled by dynamical control of Rydberg electron's orbit which significantly enhances the spectral resolution. Furthermore, to unambiguously identify the frequency shift, we directly compare core ion's spectrum with a signal from a single trapped ion serving as an ultimate frequency reference. This work provides an important foundation for quantum control of inner-core transitions, which offer an useful tool in manipulating Rydberg atom as well as a sensitive probe for electron-core interactions in atomic and molecular systems.
The Stark effects of the Rydberg states in the alkaline-earth atoms are studied theoretically. Using a method similar to the treatment of alkali atoms, the properties of the Stark states of Mg, Ca, Sr and Ba atoms in the regions far away from the perturbers are investigated. The Stark maps for Mg ( n = 16, M = 0), Ca ( n = 10, M = 0), Sr ( n = 12, M = 0) and Ba ( n = 13, | M | = 0, 1) are presented. Topics such as the general methods of calculation, the treatment of fine structure and the structure of level anti-crossings are discussed. The comparison between the theoretical and experimental Stark maps is satisfactory.
In extremely high Rydberg states of odd alkaline-earth isotopes, the Fermi constant a ms is comparable to the energy separation between levels belonging to different principal quantum numbers n and hyperfine interactions dominate the structure of the levels. The multichannel quantum defect theory of fine structure has been developed and applied to hyperfine structure and thus the HFS can be analysed directly by MQDT. A two-channel quantum defect model for extremely high Rydberg msns 1 S 0 and msns 3 S 1 series in odd alkaline-earth isotopes for F=I is described. The U i(F)i matrix is given analytically and the relationship between the eigenquantum defects of HFS and the quantum defects of fine structure is derived. The HFS of two extremely high Rydberg 5sns 1 S 0 and 3 S 1 series in 87 Sr has been calculated by the model and an excellent agreement between the theoretical and experimental results has been achieved. The HFS of extremely high Rydberg msns 1 S 0 and 3 S 1 series in 43 Ca, 135 Ba and 137 Ba are also analysed by the model.