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 (180)Hf(19)F(+) with a coherence time of 100 milliseconds. 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.
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 (180)Hf(19)F(+) with a coherence time of 100 milliseconds. 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.
Heavy polar molecules can be used to measure the electric dipole moment of the electron, which is a sensitive probe of physics beyond the Standard Model. The value is determined by measuring the precession of the molecule’s spin in a plane perpendicular to an applied electric field. The longer this precession evolves coherently, the higher the precision of the measurement. For molecules in a trap, this coherence time could be very long indeed. We evaluate the sensitivity of an experiment where neutral molecules are trapped electrically, and compare this to an equivalent measurement in a molecular beam. We consider the use of a Stark decelerator to load the trap from a supersonic source, and calculate the deceleration efficiency for YbF molecules in both strong-field seeking and weak-field seeking states. With a 1 s holding time in the trap, the statistical sensitivity could be ten times higher than it is in the beam experiment, and this could improve by a further factor of five if the trap can be loaded from a source of larger emittance. We study some effects due to field inhomogeneity in the trap and find that rotation of the electric field direction, leading to an inhomogeneous geometric phase shift, is the primary obstacle to a sensitive trap-based measurement. 1
The search for a permanent electron electric dipole moment (eEDM) serves as a test of fundamental symmetry violations and of physics beyond the Standard Model. Trapped molecular ions in the 3Δ1 metastable electronic state are suitable candidates for an eEDM search due to their large effective electric fields and long electron spin coherence times. This thesis presents the quantum state manipulation and coherent spectroscopy of trapped HfF+ molecular ions in rotating bias fields for an eEDM search. The quantum state manipulation, which involves preparation of a large fraction of molecular ions in a single desired quantum state as well as rotational-state-resolved detection, is complicated by the lack of HfF+ spectroscopic information prior to the start of this thesis. We performed state preparation by first state-selectively autoionizing neutral HfF such that 35% of the HfF+ are formed in a single rovibrational level of the electronic ground state 1Σ+, and then transferring those ions into the desired Stark levels of a single hyperfine-rovibrational manifold of the 3Δ1 state. Rotational-state-resolved detection is accomplished by both laser-induced fluorescence and resonance-enhanced multi-photon photodissociation, where the latter is preferred as the state detection method of choice because its efficiency is two orders of magnitude higher compared to fluorescence. With the quantum state manipulation techniques developed, we performed Ramsey spectroscopy of the trapped HfF+ ions in the presence of rotating bias electric and magnetic fields, demonstrating electron spin coherence times as long as 150 ms. Finally, we present a preliminary measurement of the eEDM at the |de| < 10-25 e cm level.
Heavy polar molecules can be used to measure the electric dipole moment of the electron, which is a sensitive probe of physics beyond the Standard Model. The value is determined by measuring the precession of the molecule's spin in a plane perpendicular to an applied electric field. The longer this precession evolves coherently, the higher the precision of the measurement. For molecules in a trap, this coherence time could be very long indeed. We evaluate the sensitivity of an experiment where neutral molecules are trapped electrically, and compare this to an equivalent measurement in a molecular beam. We consider the use of a Stark decelerator to load the trap from a supersonic source, and calculate the deceleration efficiency for YbF molecules in both strong-field seeking and weak-field seeking states. With a 1 s holding time in the trap, the statistical sensitivity could be ten times higher than it is in the beam experiment, and this could improve by a further factor of five if the trap can be loaded from a source of larger emittance. We study some effects due to field inhomogeneity in the trap and find that rotation of the electric field direction, leading to an inhomogeneous geometric phase shift, is the primary obstacle to a sensitive trap-based measurement.
Today's most sensitive experiments for detecting CP-violating permanent electric dipole moments (EDM) rely on molecular spectroscopy. The high sensitivity arises from large internal electric fields that interact with the constituents of the molecule. For molecular ions it has long been assumed that experiments with static polarization from dc electric fields are infeasible, as the ion's charge would either shift it to a field free region or eject it from the trap. This constraint appears to make single ion quantum-logic clocks, among the most precise measurement devices available, incompatible with EDM measurements. Here, we demonstrate that, under typical trapping conditions, heavy molecular ions with small Ω/Λ-doubling can be polarized by a static electric field while remaining confined in the Paul trap. This effect arises from a cancellation between the electrostatic force and the trap's ponderomotive force, resulting in an equilibrium position where the ion experiences a dc electric field component. Dynamic decoupling allows to implement co-magnetometry schemes in a single molecule and provides long interrogation times. This will allow the operation of a quantum-logic molecular radio-frequency clock in static electric fields, providing sensitivity to EDMs. Working with only a few ions and non-destructive detection techniques opens the door to the use of highly sensitive, rare, and radioactive molecular species as well as quantum-enhanced metrology schemes to achieve unprecedented levels of accuracy and precision.
Cold and ultracold polar molecules with nonzero electronic angular momenta are of great interest for studies in quantum chemistry and control, investigations of novel quantum systems, and precision measurement. However, in mixed electric and magnetic fields, these molecules are generically subject to a large set of avoided crossings among their Zeeman sublevels; in magnetic traps, these crossings lead to distorted potentials and trap loss from electric bias fields. We have characterized these crossings in OH by microwave-transferring trapped OH molecules from the upper $|f;\phantom{\rule{0.16em}{0ex}}M=+\frac{3}{2}\ensuremath{\rangle}$ parity state to the lower $|e;\phantom{\rule{0.16em}{0ex}}+\frac{3}{2}\ensuremath{\rangle}$ state and observing their trap dynamics under an applied electric bias field. Our observations are very well fit by a simple Landau-Zener model, yielding insight to the rich spectra and dynamics of polar radicals in mixed external fields.
Experimental advances in the production of cold molecules in the last years have triggered a flurry of theoretical work in fields as diverse as precision spectroscopy, controlled chemistry, fundamental physics, or quantum computation and simulation [1,2]. Progress on these lines naturally demands an increasing level of precision in the measurement and control of molecular states and properties. In this talk, I will present two of our recent contributions to this end. First, I will review some ideas and tools of cold atomic physics and quantum information that underlie our work. Then, I will introduce a quantum spectroscopy protocol for molecular ions based on their interaction with trapped atomic ions and phase gates [3]. After this, I will show how these ideas can be generalized to enable the measurement of a polar molecule's electric dipole moment [4]. Finally, I will discuss some of our ongoing work to use cold polar molecules for quantum simulation and quantum metrology.