The complex Rydberg structure of ytterbium atoms is shaped by multiple low-lying ion-core-excited states and strong channel interactions, which presents both opportunities and challenges for quantum information processing and precision metrology. In this work, we extend high-resolution microwave spectroscopy and multichannel quantum defect theory (MQDT) modeling of singly excited $6sn\ell$ Rydberg states in ${}^{174}\mathrm{Yb}$ and ${}^{171}\mathrm{Yb}$ to include the $\ell =3$ ($f$) and $\ell =4$ ($g$) series. Our measurements reveal $p\text{−}f$ mixing in odd-parity Rydberg states of ${}^{171}\mathrm{Yb}$, which we incorporate by combined MQDT models for $6snp$ and $6snf$ series. Additionally, we observe that for $\ell =4$ the spin-orbit interaction dominates over the exchange interaction, such that the $6sng$ states are more accurately described in a $jj$-coupled basis. We validate our models by comparing the predicted Landé $g$ factors and static dipole polarizabilities with experimental measurements, finding excellent agreement. These results provide important input for designing high-fidelity entangling gates with ytterbium atoms.

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• Atomic spectra
• Electronic structure of atoms & molecules
• Fine & hyperfine structure
• Long-range interactions
• van der Waals interaction
• Qubits
• Rydberg atoms & molecules
• Atomic Properties