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Physical Review Letters

Doubly Excited Autoionizing Rydberg States of Sr

William E. Cooke, Thomas F. Gallagher, S. A. Edelstein, R. M. Hill

Published Jan 16, 1978• 296 citations
Publisher

Abstract

We report the observation of doubly excited autoionizing Rydberg states of Sr, belonging to the configuration $5{p}_{\frac{1}{2}}$, $\mathrm{nl}$. Our procedure involves a three-step optical excitation process which incorporates Stark switching to reach higher $l$ states not normally accessible because of dipole selection rules. Quantum defects are reported for several $5{p}_{\frac{1}{2}}$, $\mathrm{ns}$ and $5{p}_{\frac{1}{2}}$, $\mathrm{nd}$ states. The lifetimes of the $5{p}_{\frac{1}{2}}$, $\mathrm{ns}$ states are shown to scale as ${({n}^{*})}^{3}$, and the lifetimes of the $5{p}_{\frac{1}{2}}$, $16l$ states are shown to increase dramatically with increasing $l$.

DOI
10.1103/physrevlett.40.178

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The authors demonstrate that, for excited-core Rydberg states of high angular momentum lll, a simple relationship exists between the autoionization rate and the quantum defect of the corresponding ground-core state. For many cases, both quantities can be expressed in terms of the dipole polarizability of the core. The autoionization rates of the excited-core Sr (5pnl5\mathrm{pnl}5pnl) states are calculated as an example, and compared to existing experimental data.
Rydberg atoms have a long history of scientific research, but they have recently seen a resurgence in popularity due to their advantages when dealing with coupled internal Rydberg states, or externally-coupled Rydberg atoms. The use of convenient RF and/or microwave generation techniques allows for straightforward coupling of many nearby Rydberg states, enabling quantum simulation studies, such as the generation of a synthetic lattice. Strontium is particularly attractive for Rydberg atom studies due to its optically active core, which allows for two-electron excited states and its conveniently accessible transition frequencies that match those available using commercial diode lasers. Before these experiments and applications can be realized however, precise knowledge of Rydberg state energies and quantum defects is required. Therefore, this work undertakes an extensive study of the quantum defects of both singly and doubly-excited strontium Rydberg atoms for a wide range of n and l. Precision microwave spectroscopy between nearby Rydberg states produces an improved self-consistent set of quantum defects for singly-excited 1S0, 1P1, 1D2, and 1F3 states, described by their corresponding Rydberg-Ritz parameters. Quantum defects and lifetimes for autoionizing two-electron-states are also presented. These elucidate the effects of core penetration by the “outer” excited Rydberg electron on transitions within the core ion and on the Rydberg level itself.
Rydberg atoms are increasingly being used as a means of introducing long-range, tunable interactions into atomic systems through their strong dipole-dipole interactions. When creating such interactions, however, there are a variety of potential effects that can occur, such as state (n and/or L) changing or Penning ionization, which can complicate the dynamics of the system. In the following work, such interactions are investigated for Rydberg-Rydberg collisions using very high-n, n ~300, strontium Rydberg atoms in an atomic beam configuration. By exploiting Rydberg blockade and the inherent distribution of atomic velocities present in an atomic beam, it is possible to create a 1D array of moving Rydberg atoms which will naturally overtake each other over time. Measurements of both Penning ionization and state changing for such collisions are made and compared with classical trajectory Monte-Carlo (CTMC) simulations, with both indicating large collisional cross sections on the order of 1 x 10-6 cm2 for Penning ionization and nearly 8 x 10-5 cm2 for state changing interactions. In a second series of experiments, previous work involving doubly-excited Rydberg states is expanded upon by investigating autoionization with high-n, L > 3, Rydberg states. Past research involving autoionization has shown that the effect is strongly L-dependent, with high-L states having significantly smaller autoionizing rates. To create well-defined, L > 3 states, the use of microwave fields to drive various high-n, n ~ 150, n1F3 → (n+1)1G4, (n+2)1H5 transitions is investigated, with spectroscopic measurements of these transitions providing quantum defect values for n1G4 and n1H5 states. These measurements provide a basis for future studies into the L-dependence of high-n, n ~ 300, autoionizing Rydberg atoms, with the eventual goal of creating a long-lived, doubly-excited “planetary” Rydberg state.
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.
We report here the first observation of Na2{\mathrm{Na}}_{2}Na2​ Rydberg states with an excited Na2+{\mathrm{Na}}_{2}^{+}Na2+​ 1 $^{2}\mathrm{\ensuremath{\Pi}}_{\mathit{u}}$ The principle of our experiment is to prepare a Rydberg state associated with the ion in its ground state and then to excite the Na2+{\mathrm{Na}}_{2}^{+}Na2+​ core with a tunable laser. The autoionization processes occurring in these states as well as the internal energy redistribution of the singly excited Rydberg states are discussed. Finally, the energy levels of the 1 $^{2}\mathrm{\ensuremath{\Pi}}_{\mathrm{u}}$ state of Na2+{\mathrm{Na}}_{2}^{+}Na2+​ are deduced.