We present a study of Sisyphus cooling of molecules: the scattering of a single-photon remove a substantial amount of the molecular kinetic energy and an optical pumping step allow to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperature. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using Kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase space density by a factor of 10^7 . Even in the case of molecules with both low Franck-Condon coefficients and a non-closed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperature in few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam
We present a study of Sisyphus cooling of molecules: the scattering of a single-photon remove a substantial amount of the molecular kinetic energy and an optical pumping step allow to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperature. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using Kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase space density by a factor of 10^7 . Even in the case of molecules with both low Franck-Condon coefficients and a non-closed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperature in few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam
We present a study of Sisyphus cooling of molecules: The scattering of a single photon removes a substantial amount of the molecular kinetic energy and an optical pumping step allows one to repeat the process. A review of the produced cold molecules so far indicates that the method can be implemented for most of them, making it a promising method able to produce a large sample of molecules at sub-mK temperatures. Considerations of the required experimental parameters, for instance the laser power and linewidth or the trap anisotropy and dimensionality, are given. Rate equations, as well as scattering and dipolar forces, are solved using kinetic Monte Carlo methods for several lasers and several levels. For NH molecules, such detailed simulation predicts a 1000-fold temperature reduction and an increase of the phase-space density by a factor of 107. Even in the case of molecules with both low Franck-Condon coefficients and a nonclosed pumping scheme, 60% of trapped molecules can be cooled from 100 mK to sub-mK temperatures in a few seconds. Additionally, these methods can be applied to continuously decelerate and cool a molecular beam.
Cold and ultracold molecules are highly desirable for a diverse range of applications in physics and chemistry such as precision measurements, tests of fundamental physics, quantum simulation and information processing, quantum chemistry, and the physics of strongly correlated quantum matter. Laser cooling is usually infeasible in molecules because their rotational and vibrational transitions make is difficult to come up with a closed scattering cycle. Recently, a narrow range of diatomic molecules, one of which is CaF, has been shown to possess a convenient electronic structure and a highly-diagonal Franck-Condon matrix and thus be amenable to laser cooling. This thesis describes experiments on laser cooling of CaF radicals produced in a supersonic source. We first investigate the increased fluorescence when multi-frequency resonant light excites the molecules from the four hyperfine levels of the ground X²∑+(N = 1, v = 0) state to the first excited A²π½ (J’ = 1=2; v’ = 0) state. The number of photons scattered per molecule increases significantly from one or two in the single frequency case to more than 50 before the molecules get pumped into the X²∑+(N = 1; v = 1) state. We demonstrate laser cooling and slowing of CaF using counter-propagating laser light which causes the molecules to scatter more than a thousand photons on the X (N = 1, v = 0, 1) <->A (J’ = 1=2; v’ = 0) transition. The effect of the laser cooling is to slow a group of molecules from 600 ms-1 to about 580 ms-1 and to narrow their velocity distribution from an initial temperature of 3 K down to 300 mK. In addition, chirping the frequency of the cooling light to keep it on resonance with the decelerating molecules doubles the deceleration and further compresses the velocity distribution. The effect of the laser cooling is limited by the optical pumping of molecules in the X (N = 1, v = 2) state.
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.
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
The ability to cool and trap atoms has revolutionized atomic and ultra-cold physics. Molecular physics is currently undergoing a similar transformation. This thesis aims to research a general cooling method that will be applicable to wide range of molecular and atomic species and other particles. We studied the dynamics of molecules in optical fields, focusing in particular on exploring the molecular self-organisation phenomena in optical cavities to cool molecular ensembles to sub-mK temperatures. Firstly, the general model of cavity cooling from atoms to molecules and the dynamics of a particle in a single cavity mode were discussed. We extended the existing cooling scheme for two-level atoms to an ensemble of multi-level molecules. Then we studied the spatial dynamics of molecules in the new parameter conditions, focusing in particular on exploring the molecular self-organisation phenomena in optical cavities to cool molecular ensembles to sub-mK temperatures. The scheme complements well with our present experimental work on the deceleration and focusing of cold molecules and can extend our present capability to simultaneously cool and trap a large cold molecular ensemble. For simulation of a large ensemble of molecules, we proposed a new statistical model based on the Boltzmann equation beside the traditional discrete model and studied two solution methods. The comparison of the theory and numerical simulations between discrete model and statistical model showed a good agreement, which validated this new model. We then explored the scaling laws with a view to the self-organization and cooling of a large ensemble of species. We studied the cooling of a CN molecular cloud of the density 10/cm, with an initial temperature at 10 mK in an optical cavity. We found that more than a third of the molecules are stably trapped by the intracavity field and the final temperature is below 1mK. We discussed the scaling laws in the case when a large ensemble of species is involved. Finally we argue that cavity cooling using a far
Ultracold molecular gases are promising as an avenue to rich many-body physics, quantum chemistry, quantum information, and precision measurements. This richness, which flows from the complex internal structure of molecules, makes the creation of ultracold molecular gases using traditional methods (laser plus evaporative cooling) a challenge, in particular due to the spontaneous decay of molecules into dark states. We propose a way to circumvent this key bottleneck using an all-optical method for decelerating molecules using stimulated absorption and emission with a single ultrafast laser. We further describe single-photon cooling of the decelerating molecules that exploits their high dark state pumping rates, turning the principal obstacle to molecular laser cooling into an advantage. Cooling and deceleration may be applied simultaneously and continuously to load molecules into a trap. We discuss implementation details including multilevel numerical simulations of strontium monohydride. These techniques are applicable to a large number of molecular species and atoms with the only requirement being an electric dipole transition that can be accessed with an ultrafast laser.