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We report spectroscopic and time-resolved experimental observations to characterize the $\left[\mathrm{Xe}\right]4f^{13}\left({}^{2}F_{5/2}^o\right)5d6s\left({}^{1}D\right){}^1{[5/2]}_{5/2}^o$state in ${}^{172}\mathrm{Yb}^{+}$ ions. We access this state from the metastable $4f^{14}5d\left({}^{2}D_{3/2,5/2}\right)$manifold and observe an unexpectedly long lifetime of $\tau =37.9\left(9\right)\mu \mathrm{s}$ that allows visible Rabi oscillations and resolved-sideband spectroscopy. Using a combination of coherent population dynamics, high-fidelity detection and heralded state preparation, and optical pumping methods, we measure the branching ratios to the ${}^{2}D_{3/2}, {}^{2}D_{5/2}$, and ${}^{2}S_{1/2}$states to be $0.359\left(2\right)$, 0.639(2), and $0.0023\left(16\right)$, respectively. The branching ratio to the $4f^{13}6s^2\left({{}^{2}F}_{7/2}\right)$is compatible with zero within our experimental resolution. We also report measurements of Landé $g$-factor of the ${}^1{[5/2]}_{5/2}^o$state. Further, the branching ratio of the ${}^{2}D_{5/2}$to ${}^{2}S_{1/2}$decay in ${}^{172}\mathrm{Yb}^{+}$ was measured to be 0.188(3), improving its relative uncertainty by an order of magnitude. Our measurements provide experimental benchmarks for better understanding the atomic structure of ${\mathrm{Yb}}^{+}$ ions, which still lacks accurate numerical descriptions, and the use of high-lying excited states for partial detection and qubit manipulation in the architecture. 

Electron transfer is at the heart of many fundamental physical, chemical, and biochemical processes essential for life. The exact simulation of these reactions is often hindered by the large number of degrees of freedom and by the essential role of quantum effects. Here, we experimentally simulate a paradigmatic model of molecular electron transfer using a multispecies trapped-ion crystal, where the donor-acceptor gap, the electronic and vibronic couplings, and the bath relaxation dynamics can all be controlled independently. By manipulating both the ground-state and optical qubits, we observe the real-time dynamics of the spin excitation, measuring the transfer rate in several regimes of adiabaticity and relaxation dynamics. Our results provide a testing ground for increasingly rich models of molecular excitation transfer processes that are relevant for molecular electronics and light-harvesting systems.