Abstract Optically trapped laser-cooled polar molecules hold promise for new science and technology in quantum information and quantum simulation. Large numerical aperture optical access and long trap lifetimes are needed for many studies, but these requirements are challenging to achieve in a magneto-optical trap (MOT) vacuum chamber that is connected to a cryogenic buffer gas beam source, as is the case for all molecule laser cooling experiments so far. Long distance transport of molecules greatly eases fulfilling these requirements as molecules are placed into a region separate from the MOT chamber. We realize a fast transport method for ultracold molecules based on an electronically focus-tunable lens combined with an optical lattice. The high transport speed is achieved by the 1D red-detuned optical lattice, which is generated by interference of a focus-tunable laser beam and a focus-fixed laser beam. Efficiency of 48(8)% is realized in the transport of ultracold calcium monofluoride (CaF) molecules over 46 cm distance in 50 ms, with a moderate heating from 32(2) μK to 53(4) μK. Positional stability of the molecular cloud allows for stable loading of an optical tweezer array with single molecules.
Abstract Optically trapped laser-cooled polar molecules hold promise for new science and technology in quantum information and quantum simulation. Large numerical aperture optical access and long trap lifetimes are needed for many studies, but these requirements are challenging to achieve in a magneto-optical trap (MOT) vacuum chamber that is connected to a cryogenic buffer gas beam source, as is the case for all molecule laser cooling experiments so far. Long distance transport of molecules greatly eases fulfilling these requirements as molecules are placed into a region separate from the MOT chamber. We realize a fast transport method for ultracold molecules based on an electronically focus-tunable lens combined with an optical lattice. The high transport speed is achieved by the 1D red-detuned optical lattice, which is generated by interference of a focus-tunable laser beam and a focus-fixed laser beam. Efficiency of 48(8)% is realized in the transport of ultracold calcium monofluoride (CaF) molecules over 46 cm distance in 50 ms, with a moderate heating from 32(2) μK to 53(4) μK. Positional stability of the molecular cloud allows for stable loading of an optical tweezer array with single molecules.
Laser cooling and trapping in a magneto-optical trap (MOT) have been essential to the success of cold atom physics in the last decades. Recently, the application of the same techniques to molecules has begun. The complexity of even a simple diatomic molecule makes laser cooling difficult, but promises new applications in many areas of research. In this thesis I describe the development of the first three-dimensional MOT of calcium fluoride (CaF) molecules. First, a cryogenic buffer gas source was set up, producing a pulsed beam of 9.3*10^10 molecules per steradian per pulse with forward velocities around 170 m/s. A similar source for very large molecules was set up during a 5 month internship at the University of Vienna. Next, the molecular pulse was slowed down to the capture velocity of a MOT using chirped laser slowing, resulting in about 7*10^5 CaF molecules passing through the typical MOT volume of 1 cm^3 at velocities of 15+-5 m/s. A new deceleration method, called Zeeman-Sisyphus deceleration, was also investigated. In this method molecules move through a spatially varying magnetic field and are optically pumped between low- and high-field seeking states in such as a way that they are always losing kinetic energy. The method promises to deliver more slow molecules because the molecules are guided transversely as they are decelerated. A small prototype was built and the optical pumping step was tested successfully. Finally, 7.6*10^3 CaF molecules were trapped in a MOT and cooled to a temperature of 8.5 mK. The radial trap frequency is 2 pi*130 Hz and the damping constant is beta=9.5*10^2 s^-1. The lifetime is about 100 ms and depends strongly on the scattering rate. This MOT is an an ideal starting point for a wide range of new experiments with ultracold molecules.
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.
Abstract Achieving high-density samples of laser-cooled molecules is a critical step toward advancing applications in precision measurements, ultracold chemistry and quantum science. We report the experimental realization of a high-density conveyor-belt magneto-optical trap for calcium monofluoride (CaF) molecules. The obtained highly-compressed cloud has a mean radius of 64(5) μ m and a peak number density of 3.6(5) x 10 10 cm -3 , a 600-fold increase over the conventional red-detuned MOTs of CaF, and the densest molecular MOT observed to date. Subsequent loading of these molecules into an optical dipole trap yields up to 2.6 x 10 4 trapped molecules at a temperature of 14(2) μ K with a peak phase-space density of ~2.4 x 10 -6 . This opens new possibilities for a range of applications utilizing high-density, optically trapped ultracold molecules.
Ultracold molecules can be used for a diverse set of exciting applications including controlled quantum chemistry, probes of physics beyond the standard model, simulation of many-body quantum systems and quantum information processing. However their rich internal structure makes the required control of their motional and internal states difficult. In the last decade, the field has made rapid progress on developing techniques for producing, cooling and trapping molecules and, whilst challenges remain, many of these applications are now being realised. This thesis presents my work on laser cooling and coherent control of calcium monofluoride (CaF) molecules. We load molecules into a three-dimensional magneto-optical trap (MOT), the first such trap for CaF and the second for any molecule. The MOT contains around 2×10⁴ molecules with an initial temperature of 12 mK. Lowering the laser intensity brings the temperature of the MOT down to 960 μK. To further cool the molecules we load them into a blue-detuned optical molasses, cooling them to 5.4(7) μK. This temperature is ~40 times below the Doppler limit and corresponds to a typical molecule moving at only a few times the single-photon recoil velocity. We optically pump the molecules into a single Zeeman sub-level and coherently transfer them between rotational states using microwave radiation. We load the molecules into a magnetic trap where they remain confined for about 5 s, the lifetime being limited by vibrational excitation due to room-temperature blackbody radiation. We show how to prepare the trapped molecules in a coherent superposition of two rotational states, and how to maintain this coherence for long periods, up to 6.4(8) ms. Detailed simulations of the remaining decoherence mechanisms suggest that it is possible to extend this to more than a second by compressing the sample to a smaller size, and using a magnetic trap geometry where the direction of the field is nearly uniform across the trapping volume. Finally we explore theoretically how Raman sideband cooling can be applied to molecules in optical tweezer traps, potentially providing a route to full quantum control.
We present a novel method for transporting ultracold atoms in a focused optical lattice over macroscopic distances of many Rayleigh ranges. With this method ultracold atoms were transported over 5 cm in 250 ms without significant atom loss or heating. By translating the interference pattern together with the beam geometry, the trap parameters are maintained over the full transport range. Thus, the presented method is well suited for tightly focused optical lattices that have sufficient trap depth only close to the focus. Tight focusing is usually required for far-detuned optical traps or traps that require high laser intensity for other reasons. The transport time is short and thus compatible with the operation of an optical lattice clock in which atoms are probed in a well-designed environment spatially separated from the preparation and detection region.
A key method to produce trapped and laser-cooled molecules is the magneto-optical trap (MOT), which is conventionally created using light red detuned from an optical transition. In this work, we report a MOT for CaF molecules created using blue-detuned light. The blue-detuned MOT (BDM) achieves temperatures well below the Doppler limit and provides the highest densities and phase-space densities reported to date in CaF MOTs. Our results suggest that BDMs are likely achievable in many relatively light molecules including polyatomic ones, but our measurements suggest that BDMs will be challenging to realize in substantially heavier molecules due to sub-mK trap depths. In addition to record temperatures and densities, we find that the BDM substantially simplifies and enhances the loading of molecules into optical tweezer arrays, which are a promising platform for quantum simulation and quantum information processing. Notably, the BDM reduces molecular number requirements ninefold compared to a conventional red-detuned MOT, while not requiring additional hardware. Our work therefore substantially simplifies preparing large-scale molecular tweezer arrays, which are a novel platform for simulation of quantum many-body dynamics and quantum information processing with molecular qubits.