Scheme for Deterministic Loading of Laser-Cooled Molecules into Optical Tweezers.

We propose to repeatedly load laser-cooled molecules into optical tweezers, and transfer them to storage states that are rotationally excited by two additional quanta. Collisional loss of molecules in these storage states is suppressed, and a dipolar blockade prevents the accumulation of more than one molecule. Applying three cycles loads tweezers with single molecules at an 80% success rate, limited by residual collisional loss.

Collisions between Ultracold Molecules and Atoms in a Magnetic Trap.

We prepare mixtures of ultracold CaF molecules and Rb atoms in a magnetic trap and study their inelastic collisions. When the atoms are prepared in the spin-stretched state and the molecules in the spin-stretched component of the first rotationally excited state, they collide inelastically with a rate coefficient k_{2}=(6.6±1.

Enhancing Dipolar Interactions between Molecules Using State-Dependent Optical Tweezer Traps.

We show how state-dependent optical potentials can be used to trap a pair of molecules in different internal states at a separation much smaller than the wavelength of the trapping light. This close spacing greatly enhances the dipole-dipole interaction and we show how it can be used to implement two-qubit gates between molecules that are 100 times faster than existing protocols and than rotational coherence times already demonstrated. We analyze complications due to hyperfine structure, tensor light shifts, photon scattering, and collisional loss, and conclude that none is a barrier to implementing the scheme.

Long Rotational Coherence Times of Molecules in a Magnetic Trap.

Polar molecules in superpositions of rotational states exhibit long-range dipolar interactions, but maintaining their coherence in a trapped sample is a challenge. We present calculations that show many laser-coolable molecules have convenient rotational transitions that are exceptionally insensitive to magnetic fields. We verify this experimentally for CaF where we find a transition with sensitivity below 5  Hz G^{-1} and use it to demonstrate a rotational coherence time of 6.

Deep Laser Cooling and Efficient Magnetic Compression of Molecules.

We introduce a scheme for deep laser cooling of molecules based on robust dark states at zero velocity. By simulating this scheme, we show it to be a widely applicable method that can reach the recoil limit or below. We demonstrate and characterize the method experimentally, reaching a temperature of 5.

Magnetic Trapping and Coherent Control of Laser-Cooled Molecules.

We demonstrate coherent microwave control of the rotational, hyperfine, and Zeeman states of ultracold CaF molecules, and the magnetic trapping of these molecules in a single, selectable quantum state. We trap about 5×10^{3} molecules for almost 2 s at a temperature of 70(8)  μK and a density of 1.2×10^{5}  cm^{-3}.

Laser Cooled YbF Molecules for Measuring the Electron's Electric Dipole Moment.

We demonstrate one-dimensional sub-Doppler laser cooling of a beam of YbF molecules to 100  μK. This is a key step towards a measurement of the electron's electric dipole moment using ultracold molecules. We compare the effectiveness of magnetically assisted and polarization-gradient sub-Doppler cooling mechanisms.

Blue-Detuned Magneto-Optical Trap.

We present the properties and advantages of a new magneto-optical trap (MOT) where blue-detuned light drives "type-II" transitions that have dark ground states. Using ^{87}Rb, we reach a radiation-pressure-limited density exceeding 10^{11}  cm^{-3} and a temperature below 30  μK. The phase-space density is higher than in normal atomic MOTs and a million times higher than comparable red-detuned type-II MOTs, making the blue-detuned MOT particularly attractive for molecular MOTs, which rely on type-II transitions.

Characterising molecules for fundamental physics: an accurate spectroscopic model of methyltrioxorhenium derived from new infrared and millimetre-wave measurements.

Precise spectroscopic analysis of polyatomic molecules enables many striking advances in physical chemistry and fundamental physics. We use several new high-resolution spectroscopic devices to improve our understanding of the rotational and rovibrational structure of methyltrioxorhenium (MTO), the achiral parent of a family of large oxorhenium compounds that are ideal candidate species for a planned measurement of parity violation in chiral molecules. Using millimetre-wave and infrared spectroscopy in a pulsed supersonic jet, a cryogenic buffer gas cell, and room temperature absorption cells, we probe the ground state and the Re[double bond, length as m-dash]O antisymmetric and symmetric stretching excited states of both CHReO and CHReO isotopologues in the gas phase with unprecedented precision.

Principles and Design of a Zeeman-Sisyphus Decelerator for Molecular Beams.

We explore a technique for decelerating molecules using a static magnetic field and optical pumping. Molecules travel through a spatially varying magnetic field and are repeatedly pumped into a weak-field seeking state as they move towards each strong field region, and into a strong-field seeking state as they move towards weak field. The method is time-independent and so is suitable for decelerating both pulsed and continuous molecular beams.

A versatile dual-species Zeeman slower for caesium and ytterbium.

We describe the design, construction, and operation of a versatile dual-species Zeeman slower for both Cs and Yb, which is easily adaptable for use with other alkali metals and alkaline earths. With the aid of analytic models and numerical simulation of decelerator action, we highlight several real-world problems affecting the performance of a slower and discuss effective solutions. To capture Yb into a magneto-optical trap (MOT), we use the broad (1)S0 to (1)P1 transition at 399 nm for the slower and the narrow (1)S0 to (3)P1 intercombination line at 556 nm for the MOT.

Production and characterization of a dual species magneto-optical trap of cesium and ytterbium.

We describe an apparatus designed to trap and cool a Yb and Cs mixture. The apparatus consists of a dual species effusive oven source, dual species Zeeman slower, magneto-optical traps in a single ultra-high vacuum science chamber, and the associated laser systems. The dual species Zeeman slower is used to load sequentially the two species into their respective traps.

Submillikelvin Dipolar Molecules in a Radio-Frequency Magneto-Optical Trap.

We demonstrate a scheme for magneto-optically trapping strontium monofluoride (SrF) molecules at temperatures one order of magnitude lower and phase space densities 3 orders of magnitude higher than obtained previously with laser-cooled molecules. In our trap, optical dark states are destabilized by rapidly and synchronously reversing the trapping laser polarizations and the applied magnetic field gradient. The number of molecules and trap lifetime are also significantly improved from previous work by loading the trap with high laser power and then reducing the power for long-term trapping.

A search for varying fundamental constants using hertz-level frequency measurements of cold CH molecules.

Many modern theories predict that the fundamental constants depend on time, position or the local density of matter. Here we develop a spectroscopic method for pulsed beams of cold molecules, and use it to measure the frequencies of microwave transitions in CH with accuracy down to 3 Hz. By comparing these frequencies with those measured from sources of CH in the Milky Way, we test the hypothesis that fundamental constants may differ between the high- and low-density environments of the Earth and the interstellar medium.

Characterization of a cryogenic beam source for atoms and molecules.

We present a combined experimental and theoretical study of beam formation from a cryogenic buffer gas cell. Atoms and molecules are loaded into the cell by laser ablation of a target, and are cooled and swept out of the cell by a flow of cold helium. We study the thermalization and flow dynamics inside the cell and measure how the speed, temperature, divergence and extraction efficiency of the beam are influenced by the helium flow.

Stark deceleration of CaF molecules in strong- and weak-field seeking states.

We report the Stark deceleration of CaF molecules in the strong-field seeking ground state and in a weak-field seeking component of a rotationally-excited state. We use two types of decelerator, a conventional Stark decelerator for the weak-field seekers and an alternating gradient decelerator for the strong-field seekers, and we compare their relative merits. We also consider the application of laser cooling to increase the phase-space density of decelerated molecules.

Improved measurement of the shape of the electron.

The electron is predicted to be slightly aspheric, with a distortion characterized by the electric dipole moment (EDM), d(e). No experiment has ever detected this deviation. The standard model of particle physics predicts that d(e) is far too small to detect, being some eleven orders of magnitude smaller than the current experimental sensitivity.

Prospects for measuring the electric dipole moment of the electron using electrically trapped polar molecules.

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.

A robust floating nanoammeter.

A circuit capable of measuring nanoampere currents while floating at voltages up to at least 25kV is described. The circuit relays its output to ground potential via an optical fiber. We particularly emphasize the design and construction techniques, which allow robust operation in the presence of high voltage spikes and discharges.

A supersonic beam of cold lithium hydride molecules.

We have developed a source of cold LiH molecules for Stark deceleration and trapping experiments. Lithium metal is ablated from a solid target into a supersonically expanding carrier gas. The translational, rotational, and vibrational temperatures are 0.

Stark shift of the A2Pi(1/2) state in 174YbF.

We have measured the Stark shift of the A2Pi(1/2)-X2Sigma+ transition in YbF. We use a molecular beam triple resonance method, with two laser transitions acting as pump and probe, assisted by an rf transition that tags a single hyperfine transition of the X state. After subtracting the known ground state Stark shift, we obtain a value of 70.

Slowing heavy, ground-state molecules using an alternating gradient decelerator.

We have decelerated a supersonic beam of 174YbF molecules using a switched sequence of electrostatic field gradients. These molecules are 7 times heavier than any previously decelerated. An alternating gradient structure allows us to decelerate and focus the molecules in their ground state.

Measurement of the electron electric dipole moment using YbF molecules.

The most sensitive measurements of the electron electric dipole moment d(e) have previously been made using heavy atoms. Heavy polar molecules offer a greater sensitivity to d(e) because the interaction energy to be measured is typically 10(3) times larger than in a heavy atom. We have used YbF to make the first measurement of this kind.