Revealing Electron-Ytterbium Interactions through Rydberg Molecular Spectroscopy

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Abstract
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 comprehensive experimental and theoretical investigation of ultralong-range Rydberg molecules (ULRMs) of Yb 174 in 6 s n s S 1 0 Rydberg states across nearly two decades in principal quantum number n and 3 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 s -wave scattering length and the positions of two spin-orbit split p -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 6 s 23 f F 1 3 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.
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Funding Information
  • European Research Council (101071882)
  • Deutsche Forschungsgemeinschaft (277625399)

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