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Review of Scientific Instruments

Use of autoionization to measure microwave-driven transitions between high-n strontium Rydberg states

R. Brienza, G. Fields, F. B. Dunning

Published Jul 1, 2021• 2 citations
Publisher

Abstract

The use of autoionization as a tool to quantitatively analyze transitions between high-n strontium Rydberg states with low-to-intermediate values of L is described and is demonstrated through observations of Rabi oscillations when driving 5snf 1F3 → 5s(n + 1)g 1G4, 5snf 1F3 → 5s(n + 2)h 1H5, and 5snp 1P1 → 5s(n + 1)d 1D2 transitions using microwave fields. The technique is shown to offer advantages when compared to selective field ionization and can be used with other alkaline-earth and alkaline-earth-like metals.

DOI
10.1063/5.0051443

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The use of autoionization as a tool to quantitatively analyze transitions between high-n strontium Rydberg states with low-to-intermediate values of L is described and is demonstrated through observations of Rabi oscillations when driving 5snf 1F3 → 5s(n + 1)g 1G4, 5snf 1F3 → 5s(n + 2)h 1H5, and 5snp 1P1 → 5s(n + 1)d 1D2 transitions using microwave fields. The technique is shown to offer advantages when compared to selective field ionization and can be used with other alkaline-earth and alkaline-earth-like metals.
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.
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.
Cold gases of Rydberg atoms are an ideal system in which to study the novel effects of strong interatomic interactions. This thesis describes the design and construction of the world's first experiment to study Rydberg states in a cold gas of an alkaline earth metal, in this particular case strontium. We have studied a wide range of Rydberg states, and have developed a sensitive ``step-scan" spectroscopic technique that detects the spontaneous ionization of the Rydberg gas. The step-scan method is used to acquire Stark maps, and these measurements verify a single-electron model for calculating dipole matrix-elements. From the matrix-elements, interaction strengths between strontium Rydberg atoms have been calculated for the first time. The presence of two valence electrons in an alkaline earth metal, such as strontium, offers a new angle on the study of Rydberg atoms. We create doubly excited ``autoionizing" states, the first such study in a cold gas. Autoionization is used as a high yield probe of Rydberg states, and enables a study of excitation dynamics with nanosecond time-resolution. We show that autoionization can quantitatively identify and elucidate state mixing in the Rydberg gas, and probe population transfer at the very onset of ultra-cold plasma formation.
Alkaline earth Rydberg atoms are very promising tools for quantum technologies. Their highly excited outer electron provides them with the remarkable properties of Rydberg atoms and, notably, with a huge coupling to external fields or to other Rydberg atoms while the ionic core retains an optically active electron. However, low angular-momentum Rydberg states suffer almost immediate autoionization when the core is excited. Here, we demonstrate that strontium circular Rydberg atoms with a core excited in a 4D metastable level are impervious to autoionization over more than a few millisecond time scale. This makes it possible to trap and laser-cool Rydberg atoms. Moreover, we observe singlet to triplet transitions due to the core optical manipulations, opening the way to a microwave to optical quantum interface.