Rotational spectroscopy of a single molecular ion at sub part-per-trillion resolution

We use quantum-logic spectroscopy (QLS) and interrogate rotational transitions of a single CaH+ ion with a highly coherent frequency comb, achieving a fractional statistical uncertainty for a transition line center of 4 x 10^-13. We also improve the resolution in measurement of the Stark effect due to the radio-frequency (rf) electric field experienced by a molecular ion in an rf Paul trap, which we characterize and model. This allows us to determine the electric dipole moment of CaH+ by systematically displacing the ion to sample different known rf electric fields and measuring the resultant shifts in transition frequency.