Dilute ion-neutral gas mixtures are an interesting system to study due to the rich variety and enormous strength of their scattering interactions, especially in the cold and ultracold regimes. Ion-neutral collisions are dominated by long-range polarization potentials that lead to cross sections several orders of magnitude larger than typical neutral-neutral van der Waals interactions. These large ion-neutral interactions can play an important role in atomic and molecular optical physics, astrophysics, and quantum chemistry. Thanks to advances in theoretical modeling of ion-neutral scattering and the development of new ion-neutral hybrid trapping and cooling technology, interest in this previously unexplored area of cold atomic and molecular physics has surged over the past decade.\nThe ion-neutral hybrid trap, composed of a magneto-optical trap concentric within a linear Paul trap, offers the ideal playground for studying and manipulating ion-neutral interactions over a wide energy range (~ 1 μK - 104 K). This dissertation discusses the development of UConn's hybrid trap, compares experimental measurements of the Na+ - Na system and Ca+ - Na system's low-energy collision rates with previously reported theory, and reports on experimental and simulation results of the sympathetic cooling of Na+ ions by laser cooled Na atoms.
A hybrid ion-neutral trap provides an ideal system to study collisional dynamics between ions and neutral atoms. This system provides a general cooling method that can be applied to species that do not have optically accessible transitions and can also potentially cool internal degrees of freedom. The long-range polarization potentials ($V\ensuremath{\propto}\ensuremath{-}\ensuremath{\alpha}/{r}^{4}$) between ions and neutrals result in large scattering cross sections at cold temperatures, making the hybrid trap a favorable system for efficient sympathetic cooling of ions by collisions with neutral atoms. We present experimental evidence of sympathetic cooling of trapped Na
+ ions, which are closed shell and therefore do not have a laser-induced atomic transition from the ground state, by equal-mass cold Na atoms in a magneto-optical trap.
Long-range polarization forces between ions and neutral atoms result in large elastic scattering cross sections (e.g., $\ensuremath{\sim}\phantom{\rule{-0.16em}{0ex}}\phantom{\rule{-0.16em}{0ex}}{10}^{6}\phantom{\rule{0.28em}{0ex}}\mathrm{a}.\mathrm{u}.$ for
Na-
Na+ or
Na-
Ca+ at cold and ultracold temperatures). This suggests that a hybrid ion-neutral trap should offer a general means for significant sympathetic cooling of atomic or molecular ions. We present simion 7.0 simulation results concerning the advantages and limitations of sympathetic cooling within a hybrid trap apparatus consisting of a linear rf Paul trap concentric with a
Na magneto-optical trap (MOT). This paper explores the impact of various heating mechanisms on the hybrid system and how parameters related to the MOT, Paul trap, number of ions, and ion species affect the efficiency of the sympathetic cooling.
Interactions between neutral and ionized atoms are medium-range, and the spiraling nature of these collisions can lead to long interaction times and large cross-sections. The field of ion-neutral interactions is bolstered by methods from atomic physics, which allow us to accurately control and determine the quantum-states of the reactants. Trapping techniques allow us to study these interactions over a large range of energies, in order to observe interesting effects from the ultracold to hot temperature regimes. This control allows us to analyze and determine specific channels for the reaction, allowing for theoretical verification.\nThe hybrid-trap enables the concentric trapping of a sample of cold atoms and ions. This work discusses our exploration into the controlled reactions in the
textNa−textCa+ system, including measurements of sympathetic cooling and charge-exchange rates which change as a function of energy and molecular state. The quantum-state distributions of Na in our magneto-optical trap is also explored, as well as its agreement and subsequent deviation based on a predictive model. The measurements of reaction rate reveal that there are reaction-energy thresholds in two separate reaction pathways, which can be attributed to either an endothermic reaction pathway or an activation barrier due to quantum-mechanical interactions.
A dual hybrid ion–neutral trap has been built to study collisions between a cloud of ultracold atoms and small numbers of co-trapped atomic or molecular ions, in a common volume. Ultracold Na atoms are trapped in a vapour-cell magneto-optical trap (MOT), via a single-mode frequency-stabilized ring-dye laser, with repumping. A linear rf quadrupole Paul ion trap, centred on the MOT, co-traps selected atomic or molecular ions, for example Ca+. Control of the initial ion temperature involves laser cooling Ca+ ions via the resonant Fraunhofer K line at 397 nm. We showed the rf ion trap can operate simultaneously with the MOT without destroying the ultracold atom cloud. The goal is to investigate the physics of ion–neutral sympathetic cooling, the cooling by neutrals of translationally cold and vibrorotationally hot molecular ions (e.g. Na2 +(v*, J*)), and the observation of other ion–neutral processes near 0 K, of potential interest in astrophysics.
Closed shell ions like Na+, as well as many molecular ions, cannot be easily laser cooled, for spectroscopy, quantum gates, and near zero-K reaction studies. We report on experiments studying collisions between trapped ions and trapped cold atoms. The ion-atom interaction is dominated by long-range polarization forces, principally a term V $\sim -\alpha $ /R
4, $\alpha $ being the dipole polarizability of the neutral. The Hybrid trap consists of a linear Paul ion trap, set to trap Na+ ions, centered on a sodium magneto-optical trap (MOT). We investigate the sympathetic cooling of the (equal atomic mass) Na+ ion cloud concentric with the MOT, using either the 3s F=2$\to
3pF^{\prime}
=3orthe3sF=2\to
3pF^{\prime}$= 2 MOT transitions. The lifetime of the ions in the Paul trap is observed to be detectably longer when they are sympathetically cooled by the cold neutral MOT atoms, consistent with simulations via SIMION.
This Dissertation details the development of state-of-the-art hybrid atom-ion trapping architecture and technique towards increasing the quantum control of matter and the detection of chemical processes at cold temperatures. Experimental work discussed herein is performed primarily using the second-generation of the MOTion trap, a hybrid atom-ion trap consisting of a co-located magneto-optical trap (MOT) and a linear quadrupole trap (LQT), with which
40Ca and a variety of atomic and molecular ions (Yb
+, Ba
+, BaCl
+, and others) can be co-trapped and cooled. Such a device enables the immersion of laser-cooled, ionic Coulomb crystals in diffuse gases of laser-cooled, highly-polarizable neutral atoms, allowing for studies in sympathetic cooling, cold atom-ion chemistry, and nonequilbrium collisional dynamics.In the first of these studies, I discuss our method of sympathetic cooling in which we use a laser-cooled gas of Ca atoms to sympathetically cool BaCl
+ ions confined in the LQT. Because of the large polarizability of Ca, this method is found to be extremely efficient at cooling the notoriously difficult vibrational degree of freedom. This technique opens the door to research with general, ultracold, highly-localized molecular ions in the quantum ground-state which are not able to be produced using the more traditional methods of Doppler-cooling or photoassociation.In the study of cold chemistry in the hybrid trap, I characterize a fundamental reaction, known as charge exchange, at the single-particle level in which an electron is transferred from a neutral atom to an atomic ion during an inelastic collision. This low-temperature process is thought to be foundational to the chemistry leading to the formation of stars, planets and interstellar clouds in our universe. Herein I discuss how improved experimental architecture has enabled the determination of reaction rate constants for individual electronic states of the reactants.Our theoretical study of the collisional processes in hybrid atom-ion traps has led to the discovery of surprising nonequilibrium physics which exists in the hybrid trap environment. Herein I outline the collisional dynamics between neutral atoms and atomic ions in the presence of a time-dependent confining potential and describe how these dynamics manifest themselves in the emergence of nonequilbrium phenomena as indicated by bifurcations in steady-state energies of trapped ions. I show how the these dynamics can potentially limit the efficiency and overall viability of using neutral buffer gases to sympathetically cool the translational motion of trapped ions to ultracold temperatures.In addition to these experimental studies, the development of architecture is discussed with focus given to the implementation of a novel time-of-flight mass spectrometer (TOF-MS) for use with hybrid atom-ion traps as well as standard LQTs. This simple, modular device couples radially with the LQT and enables the straightforward mass analysis of trapped species without complications derived from typical experimental difficulties, engineering constraints, and financial concerns. With this robust device we precisely characterize chemical processes which can take place in these hybrid atom-ion traps. Additionally, I describe how this new architecture is used to perform the action spectroscopy of several previously unstudied molecular ions in order to further establish the field of cold molecular ion research and the widespread use of hybrid atom-ion traps.