Received 28th October 2008, Accepted 5th February 2009First published as an Advance Article on the web 28th May 2009DOI: 10.1039/b819079hWe propose a general scheme for sympathetic cooling of molecules to mKtemperatures on a timescale of seconds. Experimental parameters have beenestimated from theory, which indicate the viability of the scheme. This method,which is particularly suited to optical Stark deceleration, utilises ultracold, lasercooled metastable rare gas atoms quenched to their ground state as collisionpartnerstoco-trappedmolecular species within adeepopticaltrap(150mK). Wealso describe the measurement of the role of laser-induced molecular alignmenton the dipole force in optical Stark deceleration and outline progress towards therealisation of chirped optical Stark deceleration for producing slow molecularbeams with mK energy spreads.
Received 28th October 2008, Accepted 5th February 2009First published as an Advance Article on the web 28th May 2009DOI: 10.1039/b819079hWe propose a general scheme for sympathetic cooling of molecules to mKtemperatures on a timescale of seconds. Experimental parameters have beenestimated from theory, which indicate the viability of the scheme. This method,which is particularly suited to optical Stark deceleration, utilises ultracold, lasercooled metastable rare gas atoms quenched to their ground state as collisionpartnerstoco-trappedmolecular species within adeepopticaltrap(150mK). Wealso describe the measurement of the role of laser-induced molecular alignmenton the dipole force in optical Stark deceleration and outline progress towards therealisation of chirped optical Stark deceleration for producing slow molecularbeams with mK energy spreads.
We propose a general scheme for sympathetic cooling of molecules to microK temperatures on a timescale of seconds. Experimental parameters have been estimated from theory, which indicate the viability of the scheme. This method, which is particularly suited to optical Stark deceleration, utilises ultracold, laser cooled metastable rare gas atoms quenched to their ground state as collision partners to co-trapped molecular species within a deep optical trap (150 mK). We also describe the measurement of the role of laser-induced molecular alignment on the dipole force in optical Stark deceleration and outline progress towards the realisation of chirped optical Stark deceleration for producing slow molecular beams with mK energy spreads.
Ultracold matter offers a unique capability to reach the best high-precision spectroscopy measurements and leads to exciting perspectives in many different areas of science and technology. Molecules, thanks to their complex spectra, couple with a broader range of photons compared to atoms, so they are extremely attractive for fundamental science or to design new quantum technologies. However, to date, only a few molecular species have been brought to temperatures of the order of the microkelvin. This was done by laser cooling, a process that has been demonstrated only for species featuring an unpaired electron that does not participate to the chemical bond. \n \nA different approach, which is indifferent to the molecule electronic structure and thus potentially universal, is sympathetic cooling, where neutral molecules are cooled in a bath of ultracold atoms. However, inelastic collisions between molecules and the coolant is a major obstacle that has hindered the advances of this method thus far. Trapping the molecules in their absolute ground state would circumvent this problem or at least greatly simplify it. In this thesis we simulate the feasibility of an experiment in which metastable CO molecules are first slowed down to a few m/s with a microstructured Stark decelerator, then they are stopped by a strong DC electrical barrier and finally they are transferred irreversibly to their absolute ground state and captured in an optical trap. \nUnfortunately, the results of the simulations indicate that the total number of molecules that can be accumulated in the optical trap is rather low, far behind the observation threshold. Therefore, we concluded that other approaches to produce ultracold molecules must to be searched.
Research of cold and ultracold molecules is currently a burgeoning field in experimental and theoretical physics. New experimental techniques, involving an increasingly large set of molecule types under high levels of control, are currently opening up new avenues of research with a vast array of potential applications. From understanding the role of quantum mechanics in molecular scattering and cold chemistry, to testing the fundamental symmetries of nature and realizing quantum computing with dipolar molecular qubits, experiments are accessing regimes not dreamed of even a few years ago. Theoretical interest and computing capabilities are also at an all time high, spurred on by the possibility of creating ultracold dipolar gases as tunable realizations of strongly interacting quantum Hamiltonians, creating exotic phases of matter, and the investigation of controlling molecular interactions with applied electromagnetic fields.\nLess than a decade ago, cold molecule experiments had seemingly reached a technological plateau, being capable of creating moderate densities of 106-107 molecules/cm3 at temperatures of 10-100 mK. With many applications requiring colder temperatures and higher densities, the field was ripe for new advances. Today, via a plethora of methods such as direct molecular laser cooling, electro-optical cooling, magneto- and photo-association, and new molecular beam deceleration techniques, the field is just beginning to have the tools capable of producing truly interesting systems for study.\nThis work will discuss a couple of major steps taken in the direction of achieving scientific goals using cold molecules. The first experimental advancement discussed will be the development of a co-trap environment for studying interactions and collisions between ultracold atoms and Stark decelerated cold polar molecules. In this experiment, rubidium atoms are trapped using magnetic fields, and ammonia atoms are decelerated and trapped using electric fields. The two traps are spatially overlapped in order to investigate inter-species interactions. The co-trap environment provides exceedingly long interaction times, many orders of magnitude longer than typical beam-based interaction studies. As a result, it provides extremely high sensitivity to weak interaction mechanisms. The second experimental advancement discussed will be the development and construction of a new style of Stark decelerator, capable of producing much larger densities of cold molecules. This apparatus has the potential to expand the realm of possible experiments with chemically interesting species, and provide an unprecedented amount of control over molecular beams and traps. The gains haven't come easily though, as a new class of custom high-voltage amplifiers have needed to be developed. This part of the experiment alone took approximately two years of consistent effort to bring to fruition. After many years of development, this experiment is poised to come online, finally fulfilling its potential.
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
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.
This thesis describes the construction and characterisation of a unique cold argon atom source for sympathetic cooling of molecules. Argon atoms were laser cooled from their lowest lying metastable state using the 4s[3/2]2 → 4p[5/2]3 transition at 811.5 nm. A magneto-optical trap (MOT) was used to cool the metastable argon (Ar*) atoms to 73.2 ± 0.4 μK and trap them at a density of 3.93 × 10^9 cm-3. Cooling was facilitated using an external-cavity diode laser which was frequency-stabilised to the cooling transition using a magnetic dichroism technique. This was the first application of this technique to a plasma operated at our pressures where the applied magnetic field affected the gas behaviour. The Ar* atoms in the MOT were used to demonstrate chirped optical Stark acceleration for the first time. Atoms were accelerated up to velocities of 191 ± 1 ms-1 while maintaining narrow energy spreads in the accelerated ensemble (30-100 mK). The acceleration occurred over tens of nanoseconds and on micrometre length scales. Control over the number of particles accelerated was achieved by tailoring the depth of the optical lattice potential. Monte Carlo numerical simulations of acceleration were used to fit experimental results and study the dynamics of particles over the acceleration duration. Trapping of Ar* atoms in a quasi-electrostatic trap (QUEST) has also been demonstrated. The QUEST was formed at the focus of a 100 W laser beam with a wavelength of 10.6 μm. A trap lifetime of 18.3 ± 0.3 ms was measured.