We use (1+1$$) resonance-enhanced multiphoton photodissociation (REMPD) to detect the population in individual rovibronic states of trapped HfF$^+$ with a single-shot absolute efficiency of 18%, which is over 200 times better than that obtained with
fluorescence detection. The first photon excites a specific rotational level to an intermediate vibronic band at 35,000-36,500 cm$^{-1}$, and the second photon, at 37,594 cm$^{-1}$ (266 nm), dissociates HfF$^+$ into Hf$^+$ and F. Mass-resolved time-of-flight ion detection then yields the number of state-selectively dissociated ions. Using this method, we observe rotational-state heating of trapped HfF$^+$ ions from collisions with neutral Ar atoms. Furthermore, we measure the lifetime of the $^3Delta_1$ $v=0,, J=1$ state to be 2.1(2) s. This state will be used for a search for a permanent electric dipole moment of the electron.
Polar molecules are desirable systems for quantum simulations and cold chemistry. Molecular ions are easily trapped, but a bias electric field applied to polarize them tends to accelerate them out of the trap. We present a general solution to this is
sue by rotating the bias field slowly enough for the molecular polarization axis to follow but rapidly enough for the ions to stay trapped. We demonstrate Ramsey spectroscopy between Stark-Zeeman sublevels in 180Hf19F+ with a coherence time of 100 ms. Frequency shifts arising from well-controlled topological (Berry) phases are used to determine magnetic g-factors. The rotating-bias-field technique may enable using trapped polar molecules for precision measurement and quantum information science, including the search for an electron electric dipole moment.
The molecular ion HfF$^+$ is the chosen species for a JILA experiment to measure the electron electric dipole moment (eEDM). Detailed knowledge of the spectrum of HfF is crucial to prepare HfF$^+$ in a state suitable for performing an eEDM measuremen
tcite{Leanhardt}. We investigated the near-infrared electronic spectrum of HfF using laser-induced fluorescence (LIF) of a supersonic molecular beam. We discovered eight unreported bands, and assign each of them unambiguously, four to vibrational bands belonging to the transition $[13.8]0.5 leftarrow X1.5$, and four to vibrational bands belonging to the transition $[14.2]1.5 leftarrow X1.5$. Additionally, we report an improved measurement of vibrational spacing of the ground state, as well as anharmonicity $omega_e x_e$.
Autoionization of Rydberg states of HfF, prepared using the optical-optical double resonance (OODR) technique, holds promise to create HfF+ in a particular Zeeman level of a rovibronic state for an electron electric dipole moment (eEDM) search. We ch
aracterize 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 (LIF) 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.
