In this thesis I describe two non-evaporative cooling schemes for cooling Rb atoms. The first is a Sisyphus-like ultracold gas cooling scheme called Spatially-selecTive Optical Pumping (STOP) cooling. In principle, STOP cooling has wide applicability to both atoms and molecules. STOP cooling works by exploiting the fact that atoms or molecules in a confining potential can be optically pumped out of an otherwise dark state in a spatially-selective way. Selecting atoms or molecules for optical pumping out of a dark state in a region of high potential energy and then waiting a fixed time after the optical pumping allows for the creation of a group of high kinetic energy atoms or molecules moving in a known direction. These can then be slowed using external fields (such as the scattering force from a resonant laser beam) and optically pumped back into the dark state, cooling the gas and closing the cooling cycle. I present theoretical modeling of the STOP cooling technique, including predictions of achievable cooling rates. I have conducted an experimental study of the cooling technique for a single cooling cycle, observing one dimensional cooling rates in excess of 100 micro-K per second in an ultracold gas of 87Rb atoms. I will also comment on the prospects for improving the cooling performance beyond that presented in this work. The second cooling scheme I investigated is called Two-Isotope Collision Assisted Zeeman (2-CAZ) cooling. Through a combination of spin-exchange collisions in a magnetic field and optical pumping, it is possible to cool a gas of atoms without requiring the loss of atoms from the gas. I investigated 2-CAZ cooling using 85Rb and 87Rb. I was able to experimentally confirm that the measured 2-CAZ cooling rate agreed with a cooling rate predicted though a simple analytic model. As part of the measured cooling rate, I quantitatively characterized the heating rates associated with our actual implementation of this cooling technique and found hyperfine-changing collisions to be a significant limitation for the 85/87Rb gas mixture. Possible improvements to this experiment will be discussed as well as the prospects for improved cooling performance using an atom without hyperfine structure as the optically pumped atom.
In this thesis I describe two non-evaporative cooling schemes for cooling Rb atoms. The first is a Sisyphus-like ultracold gas cooling scheme called Spatially-selecTive Optical Pumping (STOP) cooling. In principle, STOP cooling has wide applicability to both atoms and molecules. STOP cooling works by exploiting the fact that atoms or molecules in a confining potential can be optically pumped out of an otherwise dark state in a spatially-selective way. Selecting atoms or molecules for optical pumping out of a dark state in a region of high potential energy and then waiting a fixed time after the optical pumping allows for the creation of a group of high kinetic energy atoms or molecules moving in a known direction. These can then be slowed using external fields (such as the scattering force from a resonant laser beam) and optically pumped back into the dark state, cooling the gas and closing the cooling cycle. I present theoretical modeling of the STOP cooling technique, including predictions of achievable cooling rates. I have conducted an experimental study of the cooling technique for a single cooling cycle, observing one dimensional cooling rates in excess of 100 micro-K per second in an ultracold gas of 87Rb atoms. I will also comment on the prospects for improving the cooling performance beyond that presented in this work. The second cooling scheme I investigated is called Two-Isotope Collision Assisted Zeeman (2-CAZ) cooling. Through a combination of spin-exchange collisions in a magnetic field and optical pumping, it is possible to cool a gas of atoms without requiring the loss of atoms from the gas. I investigated 2-CAZ cooling using 85Rb and 87Rb. I was able to experimentally confirm that the measured 2-CAZ cooling rate agreed with a cooling rate predicted though a simple analytic model. As part of the measured cooling rate, I quantitatively characterized the heating rates associated with our actual implementation of this cooling technique and found hyperfine-changing collisions to be a significant limitation for the 85/87Rb gas mixture. Possible improvements to this experiment will be discussed as well as the prospects for improved cooling performance using an atom without hyperfine structure as the optically pumped atom.
Through a combination of spin-exchange collisions in a magnetic field and optical pumping, it is possible to cool a gas of atoms without requiring the loss of atoms from the gas. We investigated this technique, Collision Assisted Zeeman Cooling, using 85Rb and 87Rb. We experimentally confirmed that our measured two isotope CAZ cooling rate agreed with a cooling rate predicted though a simple analytic model. As part of the measured cooling rate, we quantitatively characterized the heating rates associated with our actual implementation of this cooling technique and found hyperfine-changing collisions to be a significant limitation for the 85/87Rb gas mixture. We comment on the prospects for improving the cooling performance beyond that presented in this work.
In this thesis, I study optical pumping as a powerful cooling tool for trapped ultra-cold atoms in a highly collisional regime. First application of optical pumping is a continuous loading scheme used to transfer atoms from a guided beam into a hybrid trap. Further, I introduce a Sisyphus cooling scheme based on radio-frequency transitions and optical pumping, operating simultaneously to the accumulation of atoms in the trap. The combined scheme of continuous loading and Sisyphus cooling is demonstrated for a large range of initial conditions of the guided atoms. Thereby, I show that collisional thermalization occurs in a steady-state for almost arbitrary initial conditions, provided that the first dissipative step is able to prevent the atom from leaving the trap during its first passage. On the one hand, this scheme could be applied to a wide range of atomic or molecular beams. On the other hand, phase-space density of 4*10^-4 is reached in a continuous operation mode with chromium atoms. In the second part, I investigate demagnetization cooling based on dipolar relaxation collisions driving the thermalization of the internal (spin) and the external (motional) degrees of freedom. In the case of a gas, one has the advantage that the spin degree of freedom can be cooled very efficiently using optical pumping. It is shown, that demagnetization cooling of a gas is more efficient than evaporation cooling in terms of phase-space density gain versus loss of atoms. This allows reaching a temperature of 6uK at a phase-space density of 0.03. It is observed, that both, continuous Sisyphus cooling and demagnetization cooling are limited by a density dependent loss mechanism. I present circumstantial evidence for excited-state collisions as the dominant limiting process. Finally, I discuss possible extensions to the current experimental procedures, possibly allowing reaching quantum degeneracy by optical means only.
Abstract We present both the theoretical description and experimental implementation of a novel cooling technique for ultracold atoms trapped in a confining potential. We call the technique ‘spatially truncated optical pumping cooling.’ By using the fact that the internal states of atoms can be manipulated by laser light focused on only part of a confined ultracold gas, high energy atoms can be preferentially selected and then slowed to achieve cooling without requiring the loss of any atoms. This technique uses cooling photons more efficiently on a per photon basis than Doppler or polarization gradient cooling, while having approximately the same degree of difficulty with regard to experimental implementation.
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.
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.
Slowing down atoms using laser cooling, together with techniques like magnetic trapping and evaporative cooling, has led to numerous exciting results over the last decade [1], with the realization of Bose-Einstein condensation as the most spectacular achievement [2]. Laser-cooling schemes are applicable to atoms since closed multilevel systems can be realized and many consecutive absorptionemission cycles can be induced. This leads to a significant momentum transfer from the photons of the laser to the atom, resulting in a change of the velocity of the atom. There currently is a great interest in producing cold molecules for the study of cold molecule-molecule collisions, molecular quantum collective effects, Doppler-free spectroscopy, frequency standards, as well as many other applications already realized for atoms [3]. Slowing down of neutral molecules, a prerequisite for being able to trap them, has proven to be considerably more difficult to be achieved, however. The above-mentioned laser-cooling scheme cannot be applied to slow down molecules as no simple closed-level systems can be found; the unavoidable off-resonant radiative decay of molecules from the excited state to other vibrational levels in the electronic ground state hampers efficient momentum transfer [4]. Once molecules are present at sufficiently low kinetic energies, below a fraction of a cm21, they can be trapped in various ways. Trapping of neutral molecules in inhomogeneous magnetic [3] and electric fields [5] and trapping based on the use of evanescent fields close to the dielectricvacuum interface have been proposed [6]. It has also been suggested that extremely high laser powers might be used to induce a dipole moment in polarizable molecules, leading to trapping of these molecules in the laser beam [7]. Other methods to produce slow molecules have been put forward and have recently been successfully applied to produce the first samples of trapped molecules. By injecting molecules in a cold buffer gas, sufficiently low kinetic energies of the injected molecules can be obtained after thermalization that they can subsequently be trapped in an inhomogeneous magnetic field. This has recently been demonstrated for CaH injected in 3He buffer gas at temperatures of around 0.3 K [8]. Associative collisions between ultracold trapped atoms [9] have proven to be