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. By using guiding magnets at each weak field region, the beam can be simultaneously guided and decelerated. By tapering the magnetic field strength in the strong field regions, and exploiting the Doppler shift, the velocity distribution can be compressed during deceleration. We develop the principles of this deceleration technique, provide a realistic design, use numerical simulations to evaluate its performance for a beam of CaF, and compare this performance to other deceleration methods.
Escher meets Sisyphus: A deceleration technique for molecular beams is explored that relies on repeated optical pumping in a static, spatially varying, magnetic field. Molecules are pumped between weak‐ and strong‐field seeking states so that they are always climbing potential hills (see picture). The principles of this technique are developed, a design based on permanent magnets presented, and trajectory simulations used to study its performance for slowing a beam of CaF.
Magneto-optical trapping and sub-Doppler cooling have been essential to most experiments with quantum degenerate gases, optical lattices, atomic fountains and many other applications. A broad set of ...new applications await ultracold molecules, and the extension of laser cooling to molecules has begun. A magneto-optical trap (MOT) has been demonstrated for a single molecular species, SrF, but the sub-Doppler temperatures required for many applications have not yet been reached. Here we demonstrate a MOT of a second species, CaF, and we show how to cool these molecules to 50 μK, well below the Doppler limit, using a three-dimensional optical molasses. These ultracold molecules could be loaded into optical tweezers to trap arbitrary arrays for quantum simulation, launched into a molecular fountain for testing fundamental physics, and used to study collisions and chemistry between atoms and molecules at ultracold temperatures.
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±1.5)×10^{-11} cm^{3}/s at temperatures near 100 μK. We attribute this to rotation-changing collisions. When the molecules are in the ground rotational state we see no inelastic loss and set an upper bound on the spin-relaxation rate coefficient of k_{2}<5.8×10^{-12} cm^{3}/s with 95% confidence. We compare these measurements to the results of a single-channel loss model based on quantum defect theory. The comparison suggests a short-range loss parameter close to unity for rotationally excited molecules, but below 0.04 for molecules in the rotational ground state.
We present the properties of a magneto-optical trap (MOT) of CaF molecules. We study the process of loading the MOT from a decelerated buffer-gas-cooled beam, and how best to slow this molecular beam ...in order to capture the most molecules. We determine how the number of molecules, the photon scattering rate, the oscillation frequency, damping constant, temperature, cloud size and lifetime depend on the key parameters of the MOT, especially the intensity and detuning of the main cooling laser. We compare our results to analytical and numerical models, to the properties of standard atomic MOTs, and to MOTs of SrF molecules. We load up to 2 × 10 4 molecules, and measure a maximum scattering rate of 2.5 × 10 6 s−1 per molecule, a maximum oscillation frequency of 100 Hz, a maximum damping constant of 500 s−1, and a minimum MOT rms radius of 1.5 mm. A minimum temperature of 730 K is obtained by ramping down the laser intensity to low values. The lifetime, typically about 100 ms, is consistent with a leak out of the cooling cycle with a branching ratio of about 6 × 10 − 6 . The MOT has a capture velocity of about 11 m s−1.
Using frequency-chirped radiation pressure slowing, we precisely control the velocity of a pulsed CaF molecular beam down to a few m s-1, compressing its velocity spread by a factor of 10 while ...retaining high intensity: at a velocity of 15 m s-1 the flux, measured 1.3 m from the source, is 7 × 105 molecules per cm2 per shot in a single rovibrational state. The beam is suitable for loading a magneto-optical trap or, when combined with transverse laser cooling, improving the precision of spectroscopic measurements that test fundamental physics. We compare the frequency-chirped slowing method with the more commonly used frequency-broadened slowing method.
The electric dipole moment of the electron (eEDM) can be measured with high precision using heavy polar molecules. In this paper, we report on a series of new techniques that have improved the ...statistical sensitivity of the YbF eEDM experiment. We increase the number of molecules participating in the experiment by an order of magnitude using a carefully designed optical pumping scheme. We also increase the detection efficiency of these molecules by another order of magnitude using an optical cycling scheme. In addition, we show how to destabilise dark states and reduce backgrounds that otherwise limit the efficiency of these techniques. Together, these improvements allow us to demonstrate a statistical sensitivity of 1.8 × 10−28 e cm after one day of measurement, which is 1.2 times the shot-noise limit. The techniques presented here are applicable to other high-precision measurements using molecules.
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 6.4(8) ms in a magnetic trap. Simulations suggest it is feasible to extend this to more than 1 s using a smaller cloud in a biased magnetic trap.
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 5.4(7) μK. We solve a general problem of measuring low temperatures for large clouds by rotating the phase-space distribution and then directly imaging the complete velocity distribution. Using the same phase-space rotation method, we rapidly compress the cloud. Applying the cooling method a second time, we compress both the position and velocity distributions.
We propose an experiment to measure the electric dipole moment (EDM) of the electron using ultracold YbF molecules. The molecules are produced as a thermal beam by a cryogenic buffer gas source, and ...brought to rest in an optical molasses that cools them to the Doppler limit or below. The molecular cloud is then thrown upward to form a fountain in which the EDM of the electron is measured. A non-zero result would be unambiguous proof of new elementary particle interactions, beyond the standard model.
Sideband cooling is a popular method for cooling atoms to the ground state of an optical trap. Applying the same method to molecules requires a number of challenges to be overcome. Strong tensor ...Stark shifts in molecules cause the optical trapping potential, and corresponding trap frequency, to depend strongly on rotational, hyperfine, and Zeeman states. Consequently, transition frequencies depend on the motional quantum number and there are additional heating mechanisms, either of which can be fatal for an effective sideband cooling scheme. We develop the theory of sideband cooling in state-dependent potentials, and derive an expression for the heating due to photon scattering. We calculate the ac Stark shifts of molecular states in the presence of a magnetic field, and for any polarization. We show that the complexity of sideband cooling can be greatly reduced by applying a large magnetic field to eliminate electron- and nuclear-spin degrees of freedom from the problem. We consider how large the magnetic field needs to be, show that heating can be managed sufficiently well, and present a simple recipe for cooling to the ground state of motion.
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