A pinhole discharge unit as well as a dielectric barrier discharge (DBD) head were developed for the Nijmegen pulsed valve (NPV) and the molecular beam properties accessible from each source were characterised and compared. The discharge conditions were optimised for maximum hydroxyl radical density. It was found that the DBD source yields colder OH radicals, whereas the pinhole discharge source provides a threefold larger radical density compared to the DBD discharge head. \n \nTranslationally cold packages of hydroxyl radicals (Ttrans > 1mK) were produced by means of Stark deceleration and a 124-stage Stark decelerator was set up in the laboratory. The decelerator was conditioned, characterised and optimised for operation at low final velocities (v < 40 m/s). The performance of the decelerator was assessed by determining the density of OH radicals available after the deceleration process. \n \nIn a final step, a translationally cold OH package was loaded into a cryogenic magnetic trap. The trap design, the coupling of the magnetic trap to the Stark decelerator and the loading efficiency were numerically optimised employing a direct search algorithm on Monte-Carlo trajectory simulations. The cryogenic environment efficiently prevents black-body radiation from pumping OH radicals out of trappable states and the background pressure improved significantly. Under cryogenic conditions the 1/e trap lifetime improved by a factor of 30 compared to room temperature. The magnetic trap forms part of a hybrid trapping scheme for neutral molecules and ionic species. This novel type of trap represents a versatile environment for investigating ion-neutral molecule reactions in the cold regime, while offering full control over the contributing quantum states.
A pinhole discharge unit as well as a dielectric barrier discharge (DBD) head were developed for the Nijmegen pulsed valve (NPV) and the molecular beam properties accessible from each source were characterised and compared. The discharge conditions were optimised for maximum hydroxyl radical density. It was found that the DBD source yields colder OH radicals, whereas the pinhole discharge source provides a threefold larger radical density compared to the DBD discharge head. \n \nTranslationally cold packages of hydroxyl radicals (Ttrans > 1mK) were produced by means of Stark deceleration and a 124-stage Stark decelerator was set up in the laboratory. The decelerator was conditioned, characterised and optimised for operation at low final velocities (v < 40 m/s). The performance of the decelerator was assessed by determining the density of OH radicals available after the deceleration process. \n \nIn a final step, a translationally cold OH package was loaded into a cryogenic magnetic trap. The trap design, the coupling of the magnetic trap to the Stark decelerator and the loading efficiency were numerically optimised employing a direct search algorithm on Monte-Carlo trajectory simulations. The cryogenic environment efficiently prevents black-body radiation from pumping OH radicals out of trappable states and the background pressure improved significantly. Under cryogenic conditions the 1/e trap lifetime improved by a factor of 30 compared to room temperature. The magnetic trap forms part of a hybrid trapping scheme for neutral molecules and ionic species. This novel type of trap represents a versatile environment for investigating ion-neutral molecule reactions in the cold regime, while offering full control over the contributing quantum states.
A hybrid trap was developed to confine neutral molecules and molecular ions. We demonstrated the long-term trapping of Stark-decelerated OH radicals in the X 2Pi3/2 (v = 0, J = 3/2, MJ = 3/2, f) state in a permanent magnetic trap. The trap environment was cryogenically cooled to a temperature of 17 K in order to efficiently suppress black-body-radiation-induced pumping of the molecules out of trappable quantum states and collisions with residual background gas molecules which usually limit the trap lifetimes. The cold molecules were kept confined on timescales approaching minutes, an improvement of up to two orders of magnitude compared to room-temperature experiments, at translational temperatures on the order of 25 mK. A cryogenic ion trap was built and laser cooled Ca+ ions were confined. This ion trap can be used to confine sympathetically cooled molecular ions such as N+2or H2O+. Furthermore, a mechanism to superimpose both trap centers by moving the permanent magnets from the magnetic trap over the ion trap was developed. Both traps were characterized and their functionality was proven. The challenges of lasercooling in the strong magnetic field gradients were discussed. The present results pave the way for investigations of cold collisions and reactions with very small reaction rates between molecular ions and neutral molecules, for new avenues for the production of ultracold molecules via sympathetic cooling and for the realization of new forms of hybrid matter with co-trapped atoms or ions.
Abstract Trapped cold molecules represent attractive systems for precision-spectroscopic studies and for investigations of cold collisions and chemical reactions. However, achieving their confinement for sufficiently long timescales remains a challenge. Here, we report the long-term trapping of Stark-decelerated OH radicals in their X2Π3/2 (ν = 0, J = 3/2, MJ = 3/2, f) state in a permanent magnetic trap. The trap environment is cryogenically cooled to a temperature of 17 K to suppress black-body-radiation-induced pumping of the molecules out of trappable quantum states and collisions with residual background gas molecules which usually limit the trap lifetime. The cold molecules are thus confined on timescales approaching minutes, an improvement of up to two orders of magnitude compared with room temperature experiments, at translational temperatures of ∼25 mK. The present results pave the way for new experiments using trapped cold molecules in precision spectroscopy, in studies of slow chemical processes at low energies and in the quantum technologies.
Cold, neutral hydroxyl radicals are Stark decelerated and efficiently loaded into a permanent magnetic trap. The OH molecules are trapped in the rovibrational ground state at a density of $\ensuremath{\sim}{10}^{6}\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}3}$ and temperature of 70 mK. Collision studies between the trapped OH sample and supersonic beams of atomic He and molecular D2 determine absolute collision cross sections. The He-OH and ${\mathrm{D}}_{2}\mathrm{\text{\ensuremath{-}}}\mathrm{OH}$ center-of-mass collision energies are tuned from $60\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}1}$ to $230\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}1}$ and $145\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}1}$ to $510\text{ }\text{ }{\mathrm{cm}}^{\ensuremath{-}1}$, respectively, yielding evidence of quantum threshold scattering and resonant energy transfer between colliding particles.
The motion of polar molecules can be controlled by time-varying inhomogeneous electric fields. In a Stark decelerator, this is exploited to accelerate, transport, or decelerate a fraction of a molecular beam. When combined with a trap, the decelerator provides a means to store the molecules for times up to seconds. Here, we review our efforts to produce cold molecules via this technique. In particular, we present a new generation Stark decelerator and electrostatic trap that selects a significant part of a molecular beam pulse that can be loaded into the trap. Deceleration and trapping experiments using a beam of OH radicals are discussed.
Molecular physics has experienced groundbreaking progress in the fields of precision spectroscopy, chemical reaction kinetics, quantum state engineering and many-body physics. In order to better observe these phenomena, there is an insatiable pursuit of larger trapped molecular densities and longer lifetime. In this thesis, several key milestones that we have recently achieved towards these goals for hydroxyl radicals (OH) are reported. First, we discovered an enhanced spin-flip behavior of dipolar molecules due to the existence of dual (electric and magnetic) dipole moments and obtained a better understanding of complex spin-dynamics for both Hund's case (a) and (b) molecules in mixed electric and magnetic fields. Second, we demonstrated that the skimmer cooling technique can be applied to radicals and the production of OH can be enhanced by factor of 30 due to both clogging mitigation and more favorable skimmer-valve distance. Finally, we showed some preliminary results that it is possible to use a newly built Stark decelerator to study electric field controlled sub-kelvin collisions in an intra-beam.
Generating a controllable and pure source of molecular free-radicals or open-shell atoms has been one of the primary barriers hindering the detailed study of radical processes in the laboratory. In this thesis, a novel source of state-selected radicals -- composed of a Zeeman decelerator interfaced with a newly-designed magnetic guide -- is introduced. This tuneable source generates a pure beam of velocity-selected hydrogen atoms that will enable the study of radical interactions with exceptional control over the properties of the radical species. In Zeeman deceleration, time-varying spatially inhomogeneous magnetic fields are used to create packets of translationally cold, quantum-state-selected paramagnetic particles with a tuneable forward velocity, which are ideal for cold reaction dynamics studies. In a proof-of-principle experiment, the Zeeman deceleration of nitrogen atoms in the metastable 2D5/2 state from 460 to 410 m/s is demonstrated for the first time. The covariance matrix adaptation evolutionary strategy (CMA-ES) is adopted in order to optimise deceleration switching sequences for the operation of a 12-stage Zeeman decelerator. Using the optimised sequences, a 40% increase in the number of decelerated H(2S1/2) atoms is observed compared to standard sequences for the same final velocity, imposing the same experimental boundary conditions. Furthermore, up to 98% of the initial kinetic energy of particles in the incoming beam is removed by the optimised sequences, compared to the removal of a maximum of 83% of kinetic energy with standard sequences. Three-dimensional particle-trajectory simulations show that the optimal solution uncovered by the evolutionary algorithm is not merely a local optimisation of the experimental parameters -- it is a new mode of operation that goes beyond the standard periodic phase stability approach typically adopted. A novel magnetic guide is designed and constructed to purify the post-deceleration beam. Only radicals with a selected velocity are transmitted through the guide; all other components of the incoming beam (radical species travelling at other velocities, precursor molecules and seed gases) are removed. The guide is composed of four Halbach arrays -- hexapolar focusing elements -- and two skimming blades. The relative positions of these components can be adjusted to tune the properties of the resulting beam and to optimise transmission for a given velocity. Experimental measurements of Zeeman-decelerated H atoms transmitted through the guide, combined with extensive simulations, show that the magnetic guide successfully removes 99% of H atoms travelling outside the narrow target velocity range.