Chin-Wen Chou

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.

Spectroscopy is a powerful tool for studying molecules and is commonly performed on large thermal molecular ensembles that are perturbed by motional shifts and interactions with the environment and one another, resulting in convoluted spectra and limited resolution. Here, we use generally applicable quantum-logic techniques to prepare a trapped molecular ion in a single quantum state, drive terahertz rotational transitions with an optical frequency comb, and read out the final state non-destructively, leaving the molecule ready for further manipulation. We resolve rotational transitions to 11 significant digits and derive the rotational constant of CaH+ to be B_R = 142501777.9(1.7) kHz. Our approach suits a wide range of molecular ions, including polyatomics and species relevant for tests of fundamental physics, chemistry, and astrophysics.

Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in molecules could also lead to profound developments such as controlled chemical reactions and sensitive probes of fundamental theories, but the vibrational and rotational degrees of freedom in molecules pose a formidable challenge for controlling their quantum mechanical states. Here, we use quantum-logic spectroscopy (QLS) for preparation and nondestructive detection of quantum mechanical states in molecular ions. We develop a general technique to enable optical pumping and preparation of the molecule into a pure initial state. This allows for the observation of high-resolution spectra in a single ion (here CaH+) and coherent phenomena such as Rabi flopping and Ramsey fringes. The protocol requires a single, far-off resonant laser, which is not specific to the molecule, so that many other molecular ions, including polyatomic species, could be treated with the same methods in the same apparatus by changing the molecular source. Combined with long interrogation times afforded by ion traps, a broad range of molecular ions could be studied with unprecedented control and precision, representing a critical step towards proposed applications, such as precision molecular spectroscopy, stringent tests of fundamental physics, quantum computing, and precision control of molecular dynamics.

One of the outstanding challenges for ion trap quantum information processing is to accurately detect the states of many ions in a scalable fashion. In the particular case of surface traps, geometric constraints make imaging perpendicular to the surface appealing for light collection at multiple locations with minimal cross-talk. In this report we describe an experiment integrating Diffractive Optic Elements (DOE's) with surface electrode traps, connected through in-vacuum multi-mode fibers. The square DOE's reported here were all designed with solid angle collection efficiencies of 3.58%; with all losses included a detection efficiency of 0.388% (1.02% excluding the PMT loss) was measured with a single Ca+ ion. The presence of the DOE had minimal effect on the stability of the ion, both in temporal variation of stray electric fields and in motional heating rates.