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We theoretically investigate the laser cooling of fermionic barium monofluoride ( 137 BaF) molecules, which are promising candidates for precision studies of weak parity violation and nuclear anapole moments. This molecular species features two nuclear spins, resulting in a hyperfine structure that is considerably more complicated than the one found in the usual laser-cooled diatomics. We use optical Bloch equations and rate equations to show that optical cycling, sub-Doppler cooling and bichromatic forces can all be realized under realistically achievable experimental conditions.

Recent experiments have demonstrated direct cooling and trapping of diatomic and triatomic molecules in magneto-optical traps (MOTs). However, even the best molecular MOTs to date still have density 10 −5 times smaller than in typical atomic MOTs. The main limiting factors are: (i) inefficiencies in slowing molecules to velocities low enough to be captured by the MOT, (ii) low MOT capture velocities, and (iii) limits on density within the MOT resulting from sub-Doppler heating (Devlin and Tarbutt 2018 Phys. Rev. A 90 063415). All of these are consequences of the need to drive ‘Type-II’ optical cycling transitions, where dark states appear in Zeeman sublevels, in order to avoid rotational branching. We present simulations demonstrating ways to mitigate each of these limitations. This should pave the way toward loading molecules into conservative traps with sufficiently high density and number to evaporatively cool them to quantum degeneracy.

Aluminium monofluoride (AlF) is a promising candidate for laser cooling and trapping at high densities. We show efficient production of AlF in a bright, pulsed cryogenic buffer gas beam, and demonstrate rapid optical cycling on the Q rotational lines of the A 1 Π ↔ X 1 Σ + transition. We measure the brightness of the molecular beam to be >10 12 molecules per steradian per pulse in a single rotational state and present a new method to determine its velocity distribution in a single shot. The photon scattering rate of the optical cycling scheme is measured using three different methods, and is compared to theoretical predictions of the optical Bloch equations and a simplified rate equation model. Despite the large number of Zeeman sublevels (up to 216 for the Q(4) transition) involved, a high scattering rate of at least 17(2) × 10 6  s −1 can be sustained using a single, fixed-frequency laser without the need to modulate the polarisation. We deflect the molecu-lar beam using the radiation pressure force and measure an acceleration of 8.7(1.5) × 10 5 m s −2 . Losses from the optical cycle due to vibrational branching to X 1 Σ + , v ″ = 1 are addressed efficiently with a single repump laser. Further, we investigate two other loss channels, parity mixing by stray electric fields and photo-ionisation. The upper bounds for these effects are sufficiently low to allow loading into a magneto‐optical trap.

We have recently demonstrated a general and sensitive method to study low energy collisions that exploits the unique properties of a molecular synchrotron (Van der Poel et al., Phys Rev Lett 120:033402, 2018). In that work, the total cross section for ND3 + Ar collisions was determined from the rate at which ammonia molecules were lost from the synchrotron due to collisions with argon atoms in supersonic beams. This paper provides further details on the experiment. In particular, we derive the model that was used to extract the relative cross section from the loss rate, and present measurements to characterize the spatial and velocity distributions of the stored ammonia molecules and the supersonic argon beams.

We use narrow-band laser excitation of Yb atoms to substantially enhance the brightness of a cold beam of YbOH, a polyatomic molecule with high sensitivity to physics beyond the standard model (BSM). By exciting atomic Yb to the metastable 3P1 state in a cryogenic environment, we significantly increase the chemical reaction cross-section for collisions of Yb with reactants. We characterize the dependence of the enhancement on the properties of the laser light, and study the final state distribution of the YbOH products. The resulting bright, cold YbOH beam can be used to increase the statistical sensitivity in searches for new physics utilizing YbOH, such as electron electric dipole moment and nuclear magnetic quadrupole moment experiments. We also perform new quantum chemical calculations that confirm the enhanced reactivity observed in our experiment and compare reaction pathways of Yb(3P) with the reactants H2O and H2O2. More generally, our work presents a broad approach for improving experiments that use cryogenic molecular beams for laser cooling and precision measurement searches of BSM physics.

We present the first experimental demonstration of radiation pressure force deflection and direct laser cooling for barium monohydride (BaH) molecules resulting from multiple photon scattering. Despite a small recoil velocity (2.7 mm s−1) and a long excited state lifetime (137 ns), we use 1060 nm laser light exciting the X → A electronic transition of BaH to deflect a cryogenic buffer-gas beam and reduce its transverse velocity spread. Multiple experimental methods are employed to characterize the optical cycling dynamics and benchmark theoretical estimates based on rate equation models as well as solutions of the Lindblad master equation for the complete multilevel system. Broader implications for laser cooling and magneto-optical trapping of heavy-metal-containing molecules with narrow transition linewidths are presented. Our results pave the way for producing a new class of ultracold molecules-alkaline earth monohydrides-via direct laser cooling and trapping, opening the door to realizing a new method for delivering ultracold hydrogen atoms (Lane 2015 Phys. Rev. A 92, 022511).

The Stark deceleration technique can produce molecular beams with very low velocities. In order to maximize the density of decelerated molecules, experimental parameters such as the velocity, the velocity spread and the spatial spread of the initial molecular beam as well as the operation characteristics of the decelerator have to be chosen appropriately. In this tutorial review, we describe procedures for the optimization of the density of Stark decelerated radicals for low-velocity applications which are of interest in, e.g., molecule trapping and cold-collision studies.

We theoretically investigate the damping and trapping forces in a three-dimensional magneto-optical trap (MOT), by numerically solving the optical Bloch equations. We focus on the case where there are dark states because the atom is driven on a 'type-II' system where the angular momentum of the excited state, F ′ , is less than or equal to that of the ground state, F. For these systems we find that the force in a three-dimensional light field has very different behaviour to its one dimensional counterpart. This differs from the more commonly used 'type-I' systems ( F ′ = F + 1 ) where the 1D and 3D behaviours are similar. Unlike type-I systems where, for red-detuned light, both Doppler and sub-Doppler forces damp the atomic motion towards zero velocity, in type-II systems in 3D, the Doppler force and polarization gradient force have opposite signs. As a result, the atom is driven towards a non-zero equilibrium velocity, v0, where the two forces cancel. We find that v 0 2 scales linearly with the intensity of the light and is fairly insensitive to the detuning from resonance. We also discover a new magneto-optical force that alters the normal MOT force at low magnetic fields and whose influence is greatest in the type-II systems. We discuss the implications of these findings for the laser cooling and magneto-optical trapping of molecules where type-II transitions are unavoidable in realising closed optical cycling transitions.

Direct laser cooling of molecules has made significant progress in recent years. However, the selective cooling and manipulation of generic molecular samples based on their isotopic composition, which is ubiquitous in atomic laser cooling, has not yet been achieved. Here, we demonstrate such isotopologue-selective laser cooling and near-arbitrary control over the isotopic composition of a molecular beam, using barium monofluoride (BaF) as an example. The manipulation of the rare and previously uncooled 136 BaF is achieved in the presence of several isotopologues of significantly higher natural abundance. Our results enable intense molecular beams, high fidelity detection and manipulation of select low-abundance isotopologues or isotopic mixtures. Such beams are a first step towards isotopologue-selective molecular trapping and will be useful for applications in trace gas analysis, cold collisions and precision tests of fundamental symmetries.

In this paper we report on the production and characterization of a cold beam of BaOH molecules using a cryogenic buffer-gas beam source. BaOH is a highly suitable molecule for studies of the violation of fundamental symmetries, such as the search for the electron’s electric dipole moment. BaOH molecules are synthesized inside the cold source through laser ablation of a barium metal target while water vapor is seeded into the neon buffer gas. The BaOH flux is significantly enhanced (∼11 times) when laser-exciting the barium atoms inside the buffer-gas cell on the 1 S 0 – 3 P 1 transition. A similar enhancement has been reported for other alkaline-earth(-like) monohydroxides. For typical source conditions, the molecular beam has an average velocity of ≈ 180 m s −1 and an intensity of ∼ 10 9 molecules s −1 in N = 1, which is comparable to that of cryogenic BaF beams.