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.
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.
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.
A new technique for buffer gas loading is described. This technique greatly extends the range of atoms and molecules that may be magnetically trapped at low temperature. The advance is made possible by the rapid removal of the buffer gas on a time scale one hundred times greater than in previous buffer gas loading experiments. A new cryogenic valve is developed and employed. The following benchmarks were attained in our first experimental run; approximately 10 atoms with effective magnetic moments μeff & 3μB were trapped and thermally isolated with near unit efficiency, ~ 10 μeff = 2μB atoms were trapped and thermally isolated, and ~ 10 μeff = 1μB atoms were trapped, but without thermal isolation. For comparison, all previous buffer gas loading experiments that achieved thermal isolation after trapping were done with atoms having a magnetic moment of at least 6μB. In our second run of the experiment, better temperature management allowed us to increase the number of trapped and thermally isolated μeff = 2μB atoms to ~10 and trapped μeff = 1μB atoms to ~ 10. The performance of the present apparatus is limited by the presence of a desorbing helium film that compromises the vacuum in the cell after the bulk of the buffer gas is removed. Future improvements to address this problem are suggested that will likely allow for efficient trapping and thermal isolation of atoms and molecules with magnetic moments as low as 1μB. Analysis of the trapping and pumping dynamics is presented.
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.
We have extended buffer gas cooling to trap atoms with small effective magnetic moments μ eff . For μ eff ⩾ 3μ B , 10 12 atoms were buffer gas cooled, trapped, and thermally isolated in ultra high vacuum with roughly unit efficiency. For μ eff < 3μ B , the fraction of atoms remaining after full thermal isolation was limited by two processes: wind from the rapid removal of the buffer gas and desorbing helium films. In our current apparatus we trap atoms with μ eff ⩾ 1μ B , and thermally isolate atoms with μ eff ⩾ 1.8μ B . This triples the number of atomic species which can be buffer gas cooled and trapped in thermal isolation. Extrapolation of our results and simulations of the loss processes indicate that it is possible to trap and evaporatively cool 1μ B atoms using buffer gas cooling.
Ultracold and cold molecules have enormous potential for yielding a wealth of new physics and new technologies. Molecules possess several features that greatly increase the possibilities for new interactions, collective quantum states and effects, collisional processes, fundamental symmetry tests and chemical processes. This is due to 1) the strong interactions between the dipole moments of polar molecules, 2) the rotational and vibrational internal structure of all molecules, and 3) the easily orientable internal electric field of many molecules. The promise of cold and ultracold molecules will only be realized when samples can be prepared with at least the same ease in which we now prepare atomic samples. Several approaches towards trapping of molecules, the key first step toward studying ultracold molecules at high density, have already succeeded: direct cooling of molecules via a buffer gas, mechanical slowing of a pulsed molecular beam with electric fields and photoassociation of alkali atoms. In the ICAP 2002 session on molecules I described some of the current theoretical results and predictions about ultracold molecular systems. Profs. Meijer and Heinzen described results on pulsed beam slowing and photoassociation. This contribution describes some of the key results on buffer-gas loading of molecules. A.
Quantum gases of diatomic molecules are many body systems that offer unprecedented control over their intrinsic long and short range interactions. This is due to the unique nature of the interactions between molecules, which can be much stronger than those in magnetic atoms and which can be tuned independently through external electromagnetic fields. As a result, diatomic molecules enable both the exploration of novel supersolid states and the creation of dipole dominated and self assembled quantum solids. The molecular properties and internal structure of calcium monofluoride (CaF) make it a promising candidate molecule for the realization of several kinds of strongly correlated quantum systems, such as strongly dipolar Bose Einstein condensates, quantum crystals and arrays of molecules in optical tweezers. This dissertation summarizes the first steps towards the realization of such systems using directly laser cooled CaF molecules. The two major experimental steps which are summarized in this thesis are cryogenic buffer gas cooling and transversal laser cooling of CaF molecules. For the first achievement, cryogenic buffer gas cooling, it is important to observe that CaF molecules are radicals and therefore do not exist in a stable gas phase. As a result, the production of a beam of molecules requires a cryogenic buffer gas cell setup, in which the molecules are produced via laser ablation of a solid precursor target. Two different kinds of ablation target are used to produce a molecular beam. The first is a pellet of a mixture of CaF2/BaF2. The second is a calcium metal target in addition to sulfurhexafluoride gas, which acts as a fluorine donor. The metal target is found to be the much more stable molecule production method, and the buffer gas cooling setup produces a bright and slow beam of molecules with a flux of around 1011 - 1013sr-1 molecules in the ground state of the laser cooling cycle. The second achievement is a significant improvement of the techniques for laser cooling of the resulting molecular beam. Notably, trapped cold gases of directly laser cooled molecules have not reached the quantum degenerate regime yet, but this milestone is within reach. In our experiment we aim to improve the loading of the magneto optical trap from the laser slowed beam, as this has been the most inefficient step in previous experiments with CaF. Our approach is to collimate the molecular beam through transversal laser cooling on the 𝑋 - 𝐴 transition. Due to the angular momentum structure of the type-II cooling transition, Doppler cooling forces in molecules are typically accompanied by sub Doppler Sisyphus heating forces and vice versa. This has made the collimation of molecular beams difficult in previous experiments, because efficient Doppler cooling over a large velocity range is perturbed by the appearance of sub Doppler heating forces at low transversal velocities. Here, we present a new way to address the hyperfine structure in the molecules using carefully chosen laser sidebands, which overcomes this limitation. The sideband spectrum of the cooling laser consists of one strong sideband with ≈ 80% of the laser power addressing a single hyperfine state and several weaker sidebands which repump population from the other hyperfine states. Depending on the detuning of the cooling laser, the strong sideband generates sub Doppler cooling forces on the 𝑋2Σ+(𝐹 = 2) - 𝐴2Π1/2 (𝐹 = 1) or the 𝑋2Σ+(𝐹 = 1+) - 𝐴2Π1/2 (𝐹 = 0) transition. The measured transversal density profiles of the molecular beam suggest that, for certain detunings of the cooling laser, both mechanisms lead to forces that counteract the molecular motion, leading to the simultaneous appearance of Doppler and sub Doppler cooling. This result is contrary to the conventional tendency of type II systems, where sub Doppler cooling forces are usually opposed by Doppler heating forces. The observed behavior is supported by numerical simulations of the laser cooling forces and molecular trajectories based on the optical Bloch equations. Overall, the results highlight the importance of a well tailored cooling laser sideband structure for molecular laser cooling to control the interplay between both cooling mechanisms. Through the collimation of the molecular motion towards the capture region of a magneto-optical trap, the transversal cooling of the molecular beam with simultaneous Doppler and sub-Doppler cooling forces should enable a more efficient trap loading. The experimental results presented here therefore form the basis for future experiments on laser slowing, magneto optical trapping and evaporative cooling towards Bose Einstein condensation or the loading of large optical tweezer arrays of cold CaF molecules.