Cold gases of atoms and molecules provide a system for the exploration of a diverse set of physical phenomena. For example, cold gasses of magnetically and electrically polar atoms and molecules are ideal systems for quantum simulation and quantum computation experiments, and cold gasses of large polar molecules allow for novel spectroscopic techniques. Buffer-gas cooling is a robust and widely applicable method for cooling atoms and molecules to temperatures of approximately 1 Kelvin. In this thesis, I present novel applications of buffer-gas cooling to obtaining gases of trapped, ultracold atoms and diatomic molecules, as well as the study of the cooling of large organic molecules. In the first experiment of this thesis, a buffer-gas beam source of atoms is used to directly load a magneto-optical trap. Due to the versatility of the buffer-gas beam source, we obtain trapped, sub-milliKelvin gases of four different lanthanide species using the same experimental apparatus. In the second experiment of this thesis, a buffer-gas beam is used as the initial stage of an experiment to directly laser cool and magneto-optically trap the diatomic molecule CaF. In the third experiment of this thesis, buffer-gas cooling is used to study the cooling of the conformational state of large organic molecules. We directly observe conformational relaxation of gas-phase 1,2-propanediol due to cold collisions with helium gas. Lastly, I present preliminary results on a variety of novel applications of buffer-gas cooling, such as mixture analysis, separation of chiral mixtures, the measurement of parity-violation in chiral molecules, and the cooling and spectroscopy of highly unstable reaction intermediates.
Cold gases of atoms and molecules provide a system for the exploration of a diverse set of physical phenomena. For example, cold gasses of magnetically and electrically polar atoms and molecules are ideal systems for quantum simulation and quantum computation experiments, and cold gasses of large polar molecules allow for novel spectroscopic techniques. Buffer-gas cooling is a robust and widely applicable method for cooling atoms and molecules to temperatures of approximately 1 Kelvin. In this thesis, I present novel applications of buffer-gas cooling to obtaining gases of trapped, ultracold atoms and diatomic molecules, as well as the study of the cooling of large organic molecules. In the first experiment of this thesis, a buffer-gas beam source of atoms is used to directly load a magneto-optical trap. Due to the versatility of the buffer-gas beam source, we obtain trapped, sub-milliKelvin gases of four different lanthanide species using the same experimental apparatus. In the second experiment of this thesis, a buffer-gas beam is used as the initial stage of an experiment to directly laser cool and magneto-optically trap the diatomic molecule CaF. In the third experiment of this thesis, buffer-gas cooling is used to study the cooling of the conformational state of large organic molecules. We directly observe conformational relaxation of gas-phase 1,2-propanediol due to cold collisions with helium gas. Lastly, I present preliminary results on a variety of novel applications of buffer-gas cooling, such as mixture analysis, separation of chiral mixtures, the measurement of parity-violation in chiral molecules, and the cooling and spectroscopy of highly unstable reaction intermediates.
Achieving precise control over an array of ultracold molecules would provide a unique tool-set for carrying out quantum simulations and quantum computations, as a result of the molecules' rich internal structure. To realise this aim, the molecules have to be cooled and trapped. This is much more difficult for molecules than for atoms due to their complex internal structure. This thesis presents preliminary work towards realising a versatile, permanent magnet trap for buffer gas cooled molecules. Atoms are used throughout to test the feasibility of the trap, as they are easier to produce and detect. Two novel methods for trapping buffer gas cooled atoms in a permanent magnet trap are investigated. The first of these involves trapping the atoms directly from a cryogenic buffer gas cooled ablation plume. Dy atoms, with a magnetic moment of 10µB, are trapped with a lifetime of 800±30 μs, thought to be limited by collisions with a high density of background buffer gas atoms remaining in the trap region. Information gained from the direct trapping experiments motivated the design of a second trapping set-up. Here, a beam of Dy atoms is first extracted from a cryogenic buffer gas source, and when this beam reaches the trapping region, a fraction of the atoms are stopped through collisions with cold helium gas present in the trapping region. This second method reduces the density of buffer gas required in the trap region. The trap lifetime achieved in this arrangement of 810±40 μs is no longer than in the direct trapping experiments, but this arrangement is much more stable and repeatable. The lifetime here is also thought to be limited by collisions with background buffer gas atoms.
Cryogenic buffer gas cooled beams and cells can be used to study many species, from atoms and polar molecules to biomolecules. We report on recent applications of this technique to improve the limit on the electron electric dipole moment [1], load polar molecules into a magnetic trap through optical pumping [2], perform chirally sensitive microwave spectroscopy on polyatomic molecules [3], progress towards magneto-optical trapping of polar molecules [4], and studies of atom-molecule sticking [5]. [1] The ACME Collaboration: J. Baron et al., Science 343, p. 269 (2014) [2] B. Hemmerling et al., arXiv:1310.2669, to appear in Phys. Rev. Lett. [3] D. Patterson, M. Schnell, \& J. M. Doyle, Nature 497, p. 475 (2013) [4] H. Lu et al., arXiv:1310.3239, to appear in New. J. Phys. [5] J. Piskorski et al., under preparation
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.
While cold molecule experiments are rapidly moving towards their promised benefits of precision spectroscopy, controllable chemistry, and novel condensed phases, heretofore the field has been greatly limited by a lack of methods to cool and compress chemically diverse species to temperatures below ten millikelvin. While in atomic physics these needs are fulfilled by laser cooling, magneto-optical trapping, and evaporative cooling, until now none of these techniques have been applicable to molecules. In this thesis, two major breakthroughs are reported. The first is the observation of evaporative cooling in magnetically trapped hydroxyl (OH) radicals, which potentially opens a path all the way to Bose-Einstein condensation of dipolar radicals, as well as allowing cold- and ultracold-chemistry studies of fundamental reaction mechanisms. Through the combination of an extremely high gradient magnetic quadrupole trap and the use of the OH Λ-doublet transition to enable highly selective forced evaporation, cooling by an order of magnitude in temperature was achieved and yielded a final temperature no higher than 5mK. The second breakthrough is the successful application of laser cooling and magneto-optical trapping to molecules. Motivated by a proposal in this thesis, laser cooling of molecules is now known to be technically feasible in a select but substantial pool of diatomic molecules. The demonstration of not only Doppler cooling but also two-dimensional magneto-optical trapping in yttrium (II) oxide, YO, is expected to enable rapid growth in the availability of ultracold molecules--just as the invention of the atomic magneto-optical trap stimulated atomic physics twenty-five years ago.
Different from atoms, molecules have unique properties, and play an important role in the research of atomic, molecular and optical physics. Cold molecules have important applications in science and have been studied for more than 20 years. But traditional methods, such as the Stark decelerator, have hit a bottleneck: it is hard to increase the phase space density of molecules. Extending the direct laser-cooling technique to new molecular species has recently been a hot topic and also a big challenge. In this review paper, on one hand, we make a brief review to recent progresses on the direct laser cooling of polar molecules. On the other hand, a demonstration on the feasibility of laser cooling BaF molecule has been experimentally illustrated, including the analysis on the molecular energy levels, measurements of the high-resolution spectroscopy, efficient pre-cooling and state preparation via buffer-gas cooling and detailed investigations on the molcule-light interactions. All these results not only pave the way for future laser-cooling and -trapping experiments, but also serve as a reference for the laser-cooling explorations on new molecular species.
Cold molecules are an invaluable tool for modern physics. Cold atoms have already revolutionized precision metrology, allowed for spectacular findings in quantum physics and opened the door for the creation and observation of novel states of matter. Cold molecules bring with them additional degrees of freedom which give rise to unique properties that enable new kinds of experiments. For these experiments it is of vital importance to start with a sufficiently large number of cold molecules. There are multiple paths for the slowing and cooling of atoms and most of the slowing techniques utilizing lasers for direct cooling have been transferred to the molecular case with its specific requirements. The Zeeman slowing technique is advantageous for loading a trap with cold particles but had not yet been transferred from atoms to the molecular case. In this thesis I will show the first realization of the Zeeman slowing technique for diatomic molecules. This thesis will discuss several preparatory steps: Our group has had some ideas to collimate the molecular beam with a conical nozzle outlet at the buffer gas cell which I investigated on potassium atoms generated by the ablation of 39K35Cl inside the buffer gas cell. I also realized a fluorescence spectroscopy of the |XΣ1/2, N = 1, v = 0⟩ → |AΠ1/2, N = 0, v = 0⟩ transition in magnetic fields up to 300 G and confirmed simulations regarding our two laser cycling scheme in the Paschen-Back regime by measuring the scattering rate of light on one molecule. Finally, I created pre-cooled 40Ca19F with a forward velocity of around 150 m s−1 from a 40Ca19F2 target with laser ablation inside a cryogenic buffer gas cell. With the Zeeman slowing technique I slowed the molecules down to 25 m s−1, a velocity where trapping can be possible. I have also shown the characteristic compression into specific velocity classes for not yet trappable velocities. Together these two findings demonstrate that molecular Zeeman slowing is possible and a real promising tool for future experiments.