We study the occurrence of long-lived metastable states in the $4f^{13}5d6s$ electron configuration of ${\mathrm{Yb}}^{+}$. By optical pumping of a single trapped ion on the ${}^2{F}_{7/2}^{\text{o}}\to {(7/2,0)}_{7/2}$ transition at 377.5 nm, we prepare a wide range of metastable electronic states. We use a cotrapped control ion to sympathetically cool the spectroscopy ion, allowing us to accurately time its subsequent decay. We record a strong decay signal corresponding to a lifetime of 0.92(8) s and a weaker decay signal with a lifetime of 9.8($+2.9,-2.0$) s and find evidence of a much longer lifetime, $>30$ s. We identify the metastable states with these lifetimes qualitatively and corroborate our results with atomic structure calculations that support the observed lifetimes and decay paths. These long-lived states provide opportunities in qubit- and qudit-state detection and optical clocks.

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• Electron correlation calculations for atoms & ions
• Electronic structure of atoms & molecules
• Lifetimes & widths