We present experimental results from a new scheme for magneto–optically trapping strontium monofluoride (SrF) molecules, which provides increased confinement compared to our original work. The improved trap employs a new approach to magneto–optical trapping presented by Tarbutt (2015 New J. Phys. 17 015007 ), which provided insight for the first time into the source of the restoring force in magneto–optical traps (MOTs) where the cycling transition includes dark Zeeman sublevels (known as type-II MOTs). We measure a radial spring constant greater than in our original work with SrF, comparable to the spring constants reported in atomic type-II MOTs. We achieve a trap lifetime ms, over longer than originally reported for SrF. Finally, we demonstrate further cooling of the trapped molecules by briefly increasing the trapping lasers' detunings. Our trapping scheme remains a straightforward extension of atomic techniques and marks a step towards the direct production of large, dense, ultracold molecular gases via laser cooling.
We present experimental results from a new scheme for magneto–optically trapping strontium monofluoride (SrF) molecules, which provides increased confinement compared to our original work. The improved trap employs a new approach to magneto–optical trapping presented by Tarbutt (2015 New J. Phys. 17 015007 ), which provided insight for the first time into the source of the restoring force in magneto–optical traps (MOTs) where the cycling transition includes dark Zeeman sublevels (known as type-II MOTs). We measure a radial spring constant greater than in our original work with SrF, comparable to the spring constants reported in atomic type-II MOTs. We achieve a trap lifetime ms, over longer than originally reported for SrF. Finally, we demonstrate further cooling of the trapped molecules by briefly increasing the trapping lasers' detunings. Our trapping scheme remains a straightforward extension of atomic techniques and marks a step towards the direct production of large, dense, ultracold molecular gases via laser cooling.
Laser cooling and trapping are central to modern atomic physics. It has been roughly three decades since laser cooling techniques produced ultracold atoms, leading to rapid advances in a vast array of fields and a number of Nobel prizes. Prior to the work presented in this thesis, laser cooling had not yet been extended to molecules because of their complex internal structure. However, this complexity makes molecules potentially useful for a wide range of applications. The first direct laser cooling of a molecule and further results we present here provide a new route to ultracold temperatures for molecules. In particular, these methods bridge the gap between ultracold temperatures and the approximately 1 kelvin temperatures attainable with directly cooled molecules (e.g. with cryogenic buffer gas cooling or decelerated supersonic beams). Using the carefully chosen molecule strontium monofluoride (SrF), decays to unwanted vibrational states are suppressed. Driving a transition with rotational quantum number R=1 to an excited state with R'=0 eliminates decays to unwanted rotational states. The dark ground-state Zeeman sublevels present in this specific scheme are remixed via a static magnetic field. Using three lasers for this scheme, a given molecule should undergo an average of approximately 100,000 photon absorption/emission cycles before being lost via unwanted decays. This number of cycles should be sufficient to load a magneto-optical trap (MOT) of molecules. In this thesis, we demonstrate transverse cooling of an SrF beam, in both Doppler and a Sisyphus-type cooling regimes. We also realize longitudinal slowing of an SrF beam. Finally, we detail current progress towards trapping SrF in a MOT. Ultimately, this technique should enable the production of large samples of molecules at ultracold temperatures for molecules chemically distinct from competing methods.
Abstract We report the production of ultracold, trapped strontium monofluoride (SrF) molecules with number density and phase‐space density significantly higher than previously achieved. These improvements are enabled by three distinct changes to our recently‐demonstrated scheme for radio‐frequency magneto‐optical trapping of SrF: modification of the slowing laser beam geometry, addition of an optical pumping laser, and incorporation of a compression stage to the magneto‐optical trap. With these improvements, we observe a trapped sample of SrF molecules at density 2.5×105 cm−3 and phase‐space density 6×10−14, each a factor of 4 greater than in previous work. Under different experimental conditions, we observe trapping of up to 104 molecules, a factor of 5 greater than in previous work. Finally, by reducing the intensity of the applied trapping light, we observe molecular temperatures as low as 250 μK.
Abstract 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.
Ultracold polar molecules have emerged as promising platforms for quantum simulation, quantum information science, precision measurements of fundamental symmetry violations, and quantum chemistry. Over the past decade, rapid progress in direct laser cooling of molecules has enabled new capabilities such as magneto-optical traps (MOTs), sub-Doppler cooling, and optical dipole traps (ODTs), expanding the quantum toolbox with ultracold molecules of complex internal structures and strong dipolar interactions. This thesis presents the design, construction, and operation of an experiment on ultracold strontium monofluoride (88Sr19F) molecules, demonstrating state-of-the-art techniques for molecular laser cooling and trapping. The apparatus integrates a broad range of technical sub-systems, including cryogenics, ultra-high vacuum, optics, electronics, and automated laboratory control software. SrF molecules produced in a slowed cryogenic buffer gas beam are captured into a dual-frequency MOT. Subsequent Λ-enhanced gray molasses cooling reduces the molecule temperature to as low as 5 μK. A novel blue-detuned MOT is also implemented to further compress the molecular cloud, increasing the density by a factor of ∼ 400. At this high density, SrF molecules are efficiently loaded into an ODT, a tight, conservative trap with long lifetimes. Population transfer between different rotational levels is achieved via optical pumping and coherent microwave control, yielding ∼ 0.8 ms coherence time in Rabi oscillation and ∼ 90 % transfer efficiency. This thesis also describes the development of an ultracold rubidium (87Rb) atom experiment, in which a loading rate of ∼ 10^10 atoms/s into a radio-frequency (RF) MOT is demonstrated. A modular two-dimensional MOT serves as the Rb source and can be seamlessly integrated into the SrF apparatus, opening the possibility for future studies of co-trapping and sympathetic cooling of SrF molecules with atoms. The results presented in this thesis establish an experimental foundation for exploring new frontiers in ultracold molecular physics.
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. With this procedure, temperatures as low as 400 μK are achieved.
Abstract The Fast Track Communication by Petzold et al (2018 New J. Phys. 20 042001) demonstrates the first Zeeman slowing scheme for species with type-II optical cycling transitions. This new approach is directly applicable to those 2 Σ molecules that have recently been captured and cooled in molecular magneto-optical traps (MOTs) and has the potential to efficiently and continuously load these traps for the first time. This advance could produce molecular MOTs with populations comparable to their atomic counterparts and realize an ideal platform for a wide range of studies using large, dense samples of ultracold molecules.