Edmund R. Meyer

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 issue 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.

Trapped diatomic molecular ions could prove to be a sensitive probe for a permanent electron electric dipole moment (eEDM). We propose to use a ground or metastable $^3Δ_1$ level, due to its high polarizability and large EDM enhancement factor. Ions allow for simple trapping and long interrogation times, but require a time-varying electric bias field in order to probe the eEDM. We discuss experimental design as well as challenges in performing a precision spectroscopic measurement in rapidly time-varying electric fields.

This paper is a theoretical work in support of a newly proposed experiment (R. Stutz and E. Cornell, Bull. Am. Soc. Phys. 89, 76 2004) that promises greater sensitivity to measurements of the electron's electric dipole moment (EDM) based on the trapping of molecular ions. Such an experiment requires the choice of a suitable molecule that is both experimentally feasible and possesses an expectation of a reasonable EDM signal. We find that the molecular ions PtH+, HfH+, and HfF+ are suitable candidates in their low-lying triplet Delta states. In particular, we anticipate that the effective electric fields generated inside these molecules are approximately of 73 GV/cm, -17 GV/cm, and -18 GV/cm respectively. As a byproduct of this discussion, we also explain how to make estimates of the size of the effective electric field acting in a molecule, using commercially available, nonrelativistic molecular structure software.