“…Individual atoms that possess two (or more) valence cycling electrons, such as AEL atoms, give rise to electronic states with metastable lifetimes, 54,55 ultranarrow optical transitions, [56][57][58] perturbation-free ''magic'' trapping conditions, [59][60][61] efficient autoionization pathways, [62][63][64] and fully tunable couplings to internal spins. 65 Leveraging these features in multi-electron atoms has been a principal factor enabling record-setting optical lattice [66][67][68][69] and tweezer clocks, 70,71 analog many-body simulators of highdimensional and multiorbital Hamiltonians, [72][73][74][75][76][77] advanced atom interferometers, 78 high-fidelity entangling gates, 64,79,80 and telecom-compatible quantum transducers and memories. [81][82][83][84][85] In this paper, we assess the feasibility of using generalized, ''multivalent'' electronic structure for photon cycling and optical control of polyatomic molecules.…”