Engineering Rydberg-pair interactions in divalent atoms with hyperfine-split ionization thresholds

Quantum information processing with neutral atoms relies on Rydberg excitation for entanglement generation. While the use of heavy divalent or open-shell elements, such as strontium or ytterbium, has benefits due to their optically active core and a variety of possible qubit encodings, their Rydberg structure is generally complex. For some isotopes in particular, hyperfine interactions are relevant even for highly excited electronic states. We employ multi-channel quantum defect theory to infer the Rydberg structure of isotopes with non-zero nuclear spin and perform non-perturbative Rydberg-pair interaction calculations. We find that due to the high level density and sensitivities to external fields, experimental parameters must be precisely controlled. Specifically in {}⁸⁷Sr, we study an intrinsic Förster resonance, unique to divalent atoms with hyperfine-split thresholds, which simultaneously provides line stability with respect to external field fluctuations and enhanced long-range interactions. Additionally, we provide parameters for pair states that can be effectively described by single-channel Rydberg series. The explored pair states provide exciting opportunities for applications in the blockade regime as well as for more exotic long-range interactions such as largely flat, distance-independent potentials.