Towards Collinear Laser Spectroscopy of Radioactive Molecules Utilizing In-trap Produced Molecular Ion Beam

Molecules containing short-lived isotopes, namely radioactive molecules, are among the most promising candidates for probing new physics beyond the Standard Model, although their production and spectroscopic measurements remain technically challenging. Here, we demonstrate an integrated methodology that combines formation of molecular ion beams in a radiofrequency quadrupole cooler-buncher with collinear laser spectroscopy. As a proof-of-principle experiment, we successfully produce molecular ions such as $\rm BaF^+$ and $\rm YbF^+$ via in-trap ion-molecule reactions and perform high-resolution laser spectroscopy of the target molecule $\rm ^{138}BaF$. Vibrational and rotational structures of $\rm ^{138}BaF$ across different electronic states are obtained using resonance-enhanced multiphoton ionization schemes, confirming the feasibility of the proposed methodology. This work establishes a practical route for future formation and spectroscopic studies of short-lived radioactive molecules, such as those containing $\rm ^{225}Ra$, at radioactive ion beam facilities.