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We report the spectroscopy of the 14 lowest excited electronic states in theradioactive molecule radium monofluoride (RaF). The observed excitationenergies are compared with fully relativistic state-of-the-art Fock-spacecoupled cluster (FS-RCC) calculations, which achieve an agreement of >=99.64%(within ~12 meV) with experiment for all states. Guided by theory, a firmassignment of the angular momentum and term symbol is made for 10 states and atentative assignment for 4 states. The role of high-order electron correlationand quantum electrodynamics effects in the excitation energy of excited statesis studied, found to be important for all states. Establishing the simultaneousaccuracy and precision of calculations is an important step for research at theintersection of particle, nuclear, and chemical physics, including searches ofphysics beyond the Standard Model, for which RaF is a promising probe.

Pinning down electron correlations in RaF via spectroscopy of excited states and high-accuracy relativistic quantum chemistry