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Molecules with unstable isotopes often contain heavy and deformed nuclei andthus possess a high sensitivity to parity-violating effects, such as Schiffmoments. Currently the best limits on Schiff moments are set with diamagneticatoms. Polar molecules with quantum-enhanced sensing capabilities, however, canoffer better sensitivity. In this work, we consider the prototypical 223Fr107Agmolecule, as the octupole deformation of the unstable 223Fr francium nucleusamplifies the nuclear Schiff moment of the molecule by two orders of magnituderelative to that of spherical nuclei and as the silver atom has a largeelectronegativity. To develop a competitive experimental platform based onmolecular quantum systems, 223Fr atoms and 107Ag atoms have to be broughttogether at ultracold temperatures. That is, we explore the prospects offorming 223Fr107Ag from laser-cooled Fr and Ag atoms. We have performed fullyrelativistic electronic-structure calculations of ground and excited states ofFrAg that account for the strong spin-dependent relativistic effects of Fr andthe strong ionic bond to Ag. In addition, we predict the nearest-neighbordensities of magnetic-field Feshbach resonances in ultracold 223Fr+107Agcollisions with coupled-channel calculations. These resonances can be used formagneto-association into ultracold, weakly-bound FrAg. We also determine theconditions for creating 223Fr107Ag molecules in their absolute ground statefrom these weakly-bound dimers via stimulated Raman adiabatic passage using ourcalculations of the relativistic transition electronic dipole moments.

Prospects for assembling ultracold radioactive molecules from laser-cooled atoms