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Molecules containing heavy, radioactive nuclei are predicted to be extremely sensitive to violations of the fundamental symmetries of nature. Radium monofluoride molecules are of particular interest, as the nuclear octupole deformation of certain radium isotopes massively boosts their sensitivity to symmetry-violating nuclear properties. Moreover, they are predicted to be laser coolable, opening up a wide range of opportunities for precision studies. Here, we present measurements of the rovibronic structure of these molecules, which allow an unambiguous determination of their laser cooling scheme. We demonstrate an improvement in resolution of more than two orders of magnitude compared to previous studies. Our developments allowed measurements of minuscule amounts of hot molecules, with only a few hundred per second produced in a particular rotational state. The combined precision and sensitivity achieved in this work offer new opportunities for studies of radioactive molecules of interest in fundamental physics, chemistry and astrophysics.

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Highly‐charged UF3+, established by Helmut Schwarz and colleagues as the first thermodynamically stable diatomic trication, is investigated theoretically as a messenger for violations of fundamental symmetries, complementing the neutral, isoelectronic ThO, which experimentally gave one of the tightest bounds on violation of parity and time‐reversal symmetry. Electronic levels of UF3+ are analysed in comparison to the isoelectronic ions PaF2+ and ThF+. Non‐relativistic complete active space self‐consistent field calculations with scalar‐relativistic effective core potentials and a state‐optimized all‐electron two‐component complex Generalized Hartree‐Fock approach are employed to determine electronic states and properties relevant for tests of fundamental physics with these systems.

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