Autoionization of Rydberg states of HfF, prepared using the optical-optical double resonance technique, holds promise to create HfF+ in a particular Zeeman level of a rovibronic state for an electron electric dipole moment search. We characterize a vibronic band of Rydberg HfF at 54 cm−1 above the lowest ionization threshold and directly probe the state of the ions formed from this vibronic band by performing laser-induced fluorescence on the ions. The Rydberg HfF molecules show a propensity to decay into only a few ion rotational states of a given parity and are found to preserve their orientation qualitatively upon autoionization. We show empirically that we can create 30% of the total ion yield in a particular |J+, M+〉 state and present a simplified model describing autoionization from a given Rydberg state that assumes no angular dynamics.
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