Achieving a Large Density of Hydroxyl Radicals for Cold Collisions

Hao Wu

Published Jan 1, 2019• 0 citations

Abstract

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.

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OpenAlex

Abstract

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Samples of cold and ultracold polar molecules have the potential to revolutionize physical chemistry, precision measurement, and few-body quantum physics. This thesis describes experimental results for the production of cold samples of OH radicals by Stark deceleration of a supersonic beam. Since Stark deceleration cannot increase the phase space density of the sample, the initial production stage of the OH molecule is critical. The first set of experiments describes a general methodology for the production of OH beams with maximal phase space density, as well as the subsequent coupling to a Stark decelerator. Additionally, we describe the redesign of our electrostatic trap, optimized for future collision experiments of OH with co-trapped ultracold Rb atoms. The new design resulted in a 15-fold increase in total number of trapped molecules over the previous design when tested with ND3 molecules. The second set of experiments focuses on laser-based detection of OH molecules at the exit of the decelerator based on laser induced fluorescence (LIF) and resonance enhanced multiphoton ionizaton (REMPI). The latter method uses vacuum-ultraviolet light at 118nm produced by third-harmonic generation in Xe/Ar gas mixtures as the ionizing step. The sensitivity of this latter technique is limited by the attainable photon flux of the ionizing radiation at 118nm. We present detailed measurements of the conversion efficiencies as well as absolute photon fluxes. Strategies to overcome these limitations as well as prospects for detection of OH molecules in a trap are discussed.Samples of cold and ultracold polar molecules have the potential to revolutionize physical chemistry, precision measurement, and few-body quantum physics. This thesis describes experimental results for the production of cold samples of OH radicals by Stark deceleration of a supersonic beam. Since Stark deceleration cannot increase the phase space density of the sample, the initial production stage of the OH molecule is critical. The first set of experiments describes a general methodology for the production of OH beams with maximal phase space density, as well as the subsequent coupling to a Stark decelerator. Additionally, we describe the redesign of our electrostatic trap, optimized for future collision experiments of OH with co-trapped ultracold Rb atoms. The new design resulted in a 15-fold increase in total number of trapped molecules over the previous design when tested with ND3 molecules. The second set of experiments focuses on laser-based detection of OH molecules at the exit of the decelerator based on laser induced fluorescence (LIF) and resonance enhanced multiphoton ionizaton (REMPI). The latter method uses vacuum-ultraviolet light at 118nm produced by third-harmonic generation in Xe/Ar gas mixtures as the ionizing step. The sensitivity of this latter technique is limited by the attainable photon flux of the ionizing radiation at 118nm. We present detailed measurements of the conversion efficiencies as well as absolute photon fluxes. Strategies to overcome these limitations as well as prospects for detection of OH molecules in a trap are discussed.

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The interplay between hyperfine and dipolar resonances in mixed-species Cr-Cr and Rb-Cr collisions is studied. In Rb-Cr, it is found that the molecule has broken symmetry and therefore contains a large permanent electric dipole moment in the ground state. A recent collisional experiment at JILA of a supersonic helium beam with a magnetically trapped OH radical found the onset of a quantum threshold in the total OH loss rate. Using ab initio BO energy surfaces, I calculated the spin-changing collisions which removed OH from the trap. Only after including the effect of the trapping potential on the collision dynamics, some agreement with observation was found. ^In this dissertation, I present ab initio theoretical results on cold and ultra-cold collision of atomic and molecular systems with magnetic and electric dipole moments. The collisions of different isotopes of maximally spin-polarized chromium atoms (52Cr and 53Cr), alkali-metal atom (Rb) - chromium atom, and magnetically trapped hydroxide (OH) with cold supersonic helium beam are considered in this thesis. Spin-changing cross sections and rate constants in Cr-Cr isotopic collision in the presence of a magnetic field are calculated by propagating a set of multichannel equations in the field. The coupling between dipole-dipole allowed and hyperfine channels are included. The short range electrostatic interactions between atoms and atom-molecule are represented with highly-accurate Born-Oppenheimer (BO) potential energy curves. Due to the large spin multiplicity in Cr-Cr and Rb-Cr interactions, more than the usual singlet and triplet channels are obtained. 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Jan 1, 20111 citation

{\mathrm{D}}_{2}

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.