This thesis describes an experiment to produce the first laser cooled mixtures of atoms and polar molecules in magneto-optical and magnetic quadrupole traps. Inelastic collision processes between CaF molecules and Rb atoms are studied in both trapping arrangements. When molecules occupy the first rotationally excited state it is found that loss from either trap occurs at near the universal rate due to collisions with co-trapped atoms. When the molecular sample is transferred to the ground rotational state the loss rate is suppressed by at least an order of magnitude. The experimental results are compared to a quantum scattering model based on quantum defect theory and the results seem to be encouraging for observing a high ratio of elastic to inelastic collision rates in this system. In addition, improvements to the experimental apparatus are presented which led to the first measurements of the elastic cross-section for collisions between CaF and Rb. Although at the currently attainable number densities no thermalization is observed, an upper bound on the value of the cross section is placed.
This thesis describes an experiment to produce the first laser cooled mixtures of atoms and polar molecules in magneto-optical and magnetic quadrupole traps. Inelastic collision processes between CaF molecules and Rb atoms are studied in both trapping arrangements. When molecules occupy the first rotationally excited state it is found that loss from either trap occurs at near the universal rate due to collisions with co-trapped atoms. When the molecular sample is transferred to the ground rotational state the loss rate is suppressed by at least an order of magnitude. The experimental results are compared to a quantum scattering model based on quantum defect theory and the results seem to be encouraging for observing a high ratio of elastic to inelastic collision rates in this system. In addition, improvements to the experimental apparatus are presented which led to the first measurements of the elastic cross-section for collisions between CaF and Rb. Although at the currently attainable number densities no thermalization is observed, an upper bound on the value of the cross section is placed.
We prepare mixtures of ultracold CaF molecules and Rb atoms in a magnetic trap and study their inelastic collisions. When the atoms are prepared in the spin-stretched state and the molecules in the spin-stretched component of the first rotationally excited state, they collide inelastically with a rate coefficient k_{2}=(6.6±1.5)×10^{-11} cm^{3}/s at temperatures near 100 μK. We attribute this to rotation-changing collisions. When the molecules are in the ground rotational state we see no inelastic loss and set an upper bound on the spin-relaxation rate coefficient of k_{2}<5.8×10^{-12} cm^{3}/s with 95% confidence. We compare these measurements to the results of a single-channel loss model based on quantum defect theory. The comparison suggests a short-range loss parameter close to unity for rotationally excited molecules, but below 0.04 for molecules in the rotational ground state.
Measurements of the temperature dependence of trap loss collisions of laser-cooled rubidium atoms are presented. A significant suppression of the rate of collisions between ground- and excited-state atoms is observed for temperatures below $\\sim$70 muK. In such inelastic collisions, the atomic excitation takes place at long range and must survive against spontaneous decay to short range. Our results are consistent with recent predictions for the low temperature suppression of these collisions due to reduced survival of atomic excitation at low collision velocities.^ We report on measurements of trap loss collisions between ultracold Rb atoms which are confined in a magneto-optical trap. Both isotopes sp85Rb and sp87Rb have been studied over wide range of trap laser intensities and detunings. The trap loss collision rates exhibit variations over 3 orders of magnitude. We observe significant differences between the isotopes. At large detunings the ability of the trap to recapture products of the hyperfine-changing collisions is significantly diminished. This finding is supported by our numerical simulations of the recapture process. The trap loss rates due to collisions with room temperature background gas have also been measured.^ Using laser light tuned to a repulsive molecular potential, we have been able to suppress inelastic ground-state hyperfine changing collisions between ultracold sp87Rb atoms. Adiabatic excitation to the repulsive curve alters the atomic trajectories and prevents the atoms from approaching close enough for the hyperfine change to occur. Experimental results show suppressions up to $\\sim$50% and are in reasonable agreement with a simple Landau-Zener model.^ Finally, we have observed a significant cooperative effect in ultracold trap loss collisions induced by two separate lasers. One laser, tuned close to the atomic resonance, excites the atom pair to an attractive potential at long range. The resulting acceleration and deflection give rise to an enhancement in the collisional flux of ground-state atoms reaching short range, as probed by a second laser. Enhancements up to a factor of $\\sim$3 have been observed. ^
Abstract We study inelastic collisions between CaF molecules and 87Rb atoms in a dual-species magneto-optical trap. The presence of atoms increases the loss rate of molecules from the trap. By measuring the loss rates and density distributions, we determine a collisional loss rate coefficient k 2 = (1.43 ± 0.29) × 10−10 cm3 s−1 at a temperature of 2.4 mK. We show that this is not substantially changed by light-induced collisions or by varying the populations of excited-state atoms and molecules. The observed loss rate is close to the universal rate expected in the presence of fast loss at short range, and can be explained by rotation-changing collisions in the ground electronic state.
Potential wide-ranging scientific applications, spanning fundamental physics to quantum engineering, has led to significant efforts in controlling molecules at the quantum level. The rich internal structure of molecules, that gives rise to these desirable properties also complicates the task of controlling such species. Over the past decade, our ability to produce, control, and detect molecules has advanced tremendously with direct laser-cooling and magneto-optical trapping of diatomic molecules realized by several groups around the world. In this thesis, we describe the creation of the first RF MOT of CaF, which at the time of the writing of this thesis, remains the largest and densest molecular MOT. New laser cooling techniques for molecules are demonstrated, allowing laser cooling of molecules to 4 uK, 50 times colder than the Doppler limit. Optical trapping of these molecules is also achieved, which, in combination with in-trap laser cooling increased the density of trapped molecules by five orders of magnitude compared to the density in the MOT. We developed methods to cool and detect single molecules with high fidelity, which aided us in the creation of an optical tweezer array of single, ultracold CaF molecules. The densities of molecules (10^12 cm^-3) attained inside the tweezer traps also enabled us to observe both light-assisted and ground state collisions of laser cooled molecules, for the first time. The phase space density within the merged tweezers reached 5x10^-4, 10 orders of magnitude larger than the initial MOT. We implemented internal quantum state control of the molecules and dynamical control of the tweezers to build a platform for exploring state-selective ultracold quantum chemistry.
Abstract Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes in the dark or to laser-free decay pathways. For atom–molecule mixtures, RbCs + Rb and RbCs + Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom–molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.
This thesis discusses a new technique for measuring collision cross sections, using a magnetooptical trap (MOT) or magnetic trap as well as theoretical predictions for the resulting measurements based on scattering theory. The initial discussion focuses on a theoretical overview of the principles involved in laser cooling and trapping, magnetic trapping, and scattering theory. Following this, a detailed overview of the experimental instruments and methods describing the vacuum system, laser light, magnetic coils, imaging and control systems will be presented. In addition to an experimental overview, the methods and mechanical formulation involved in predicting cross sections and loss rates based on scattering theory are discussed. Finally, an overview of both experimental and theoretical results including cross sections and loss rates for the case of trapped 87Rb and background argon or helium gas will be given. The results gathered in this thesis show a strong dependence of elastic collision cross section on trap depth, which indicates that the majority of elastic collisions between ultra-cold rubidium and room temperature argon impart energy below 1K. These results suggest that the magnetic trap may be a better tool for measuring total elastic collision cross sections.