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arXiv:2005.09552 · Physical Review A

Isolated core excitation of high-orbital-quantum-number Rydberg states of ytterbium

Henri Lehec, Xin Hua, P. Pillet, Patrick Cheinet

Published Feb 9, 2021• 16 citations
arXivHTMLPDF

Abstract

We study isolated core excitation of ultracold ytterbium Rydberg atoms of high orbital angular momentum quantum number $\ensuremath{\ell}$. Measurements were performed on the $6{s}_{1/2}40\ensuremath{\ell}\ensuremath{\rightarrow}6{p}_{1/2}40\ensuremath{\ell}$ transition with $\ensuremath{\ell}=5--9$. The extracted energy shifts and autoionization rates are in good agreement with a model based on independent electrons, taking interactions into account in a perturbative approach. We reveal a slow decrease in the autoionization rates with $\ensuremath{\ell}$, explained by the strong coupling of the $6{p}_{1/2}n\ensuremath{\ell}$ autoionizing state with the $5{d}_{3/2}\ensuremath{\epsilon}{\ensuremath{\ell}}^{\ensuremath{'}}$ continua compared to previously studied divalent atoms.

DOI
10.1103/physreva.103.022806

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This paper is devoted to the autoionization process of large-angular-momentum Rydberg states. After a brief account of autoionization formalism in nonrelativistic theory and single-configuration approximation, we apply it to atomic states with one electron of large angular momentum. The dominant contribution is the direct one and the exchange contribution is ignored. In this framework, the autoionization width varies with the principal quantum number as ${n}^{\mathrm{\ensuremath{-}}3}$ and exponentially with the angular momentum. When two excited electrons interact with a spherically symmetric core, it is demonstrated that the interaction between the Rydberg electron and the core polarized by the valence electron is proportional to the interaction between the two active electrons. Using newly derived radial matrix elements, we obtain a generally good agreement between our results and experiments on barium and strontium. Large-l Rydberg states are shown to be stable versus autoionization as soon as l is about 7. Possible refinements of our method are reviewed.
Divalent atoms have emerged as powerful alternatives to alkalis in ultracold atom platforms, offering unique advantages arising from their two-electron structure. Among these species, ytterbium (Yb) is especially promising, yet its anionic properties and its Rydberg spectrum remain comparatively unexplored. In this work, we perform a first and comprehensive experimental and theoretical investigation of ultralong-range Rydberg molecules (ULRMs) of 174^{174}174Yb in 6sns 1S06sns\,^1S_06sns1S0​ Rydberg states across nearly two decades in principal quantum number nnn and three orders of magnitude in molecular binding energy. Using the Coulomb Green's function formalism, we compute Born-Oppenheimer molecular potentials describing the Rydberg atom in the presence of a ground-state perturber and achieve quantitative agreement with high-resolution molecular spectra. This enables the extraction of low-energy electron-Yb scattering phase shifts, including the zero-energy sss-wave scattering length and the positions of two spin-orbit split ppp-wave shape resonances. Our results provide strong evidence that the Yb−^{-}− anion exists only as a metastable resonance.% We additionally show the sensitivity of ULRM spectra to the atomic quantum defects, using this to determine the quantum defect of the 6s23f 1F36s23f\, ^1F_36s23f1F3​ state. Together, these findings establish Yb ULRMs as a powerful probe of electron-Yb interactions and lay essential groundwork for future Rydberg experiments with divalent atoms.
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.
In the study of Yb atomic Rydberg states, new members of 6sns 1 S 0 series for n=23, 24, 66-116 and 6snd 1 D 2 series for n=81-114 were observed. The data are in excellent agreement with the MQDT analysing results. The autoionizing Rydberg series 6p 1 2 /n's ( 1/2 , 1/2 ) 1 0 were investigated by three-step laser excitation. The ICE model was used to explain the experimental spectrum, and it has been proved to be suitable for describing the excitation of the autoionizing Rydberg states with a weakly-excited core.
We study, using a combination of experiment and theory, the excitation and decay of very-high-$n\phantom{\rule{4pt}{0ex}}(n\ensuremath{\sim}280\text{--}430)$ strontium autoionizing Rydberg states formed by near-resonant driving of the $5s\phantom{\rule{0.16em}{0ex}}^{2}S_{1/2}\ensuremath{\rightarrow}5p\phantom{\rule{0.16em}{0ex}}^{2}P_{1/2}$ core-ion transition. The branching ratio between decay through radiative transitions and through autoionization is explored. Autoionization rates are measured as a function of both the nnn and $\ensuremath{\ell}$ quantum numbers of the Rydberg electron. The nonstationary decay dynamics is studied by creating and manipulating Rydberg wave packets and by varying the laser pulse that drives the core excitation.