Abstract We simulated the motion of BaH + molecular ions which are sympathetically cooled by laser-cooled Ba + ions in linear quadrupole and octupole radiofrequency (RF) ion traps. By varying the trap voltages, we studied the velocity distribution of hydrogen atoms that would be produced upon threshold photodissociation of the BaH + . We found that hydrogen with a kinetic energy below 30 mK × k B can be produced in both traps, making the scheme suitable for loading hybrid ion–atom traps such as those used to synthesize and trap antihydrogen or study ultracold atom–ion collisions. We discuss how the dynamics of RF traps could be exploited to produce hydrogen below this limit by either driving the photodissociation transition with a small laser beam aligned along the axis of the trap, or by pulsing the laser during the micromotion turning points.
Abstract We simulated the motion of BaH + molecular ions which are sympathetically cooled by laser-cooled Ba + ions in linear quadrupole and octupole radiofrequency (RF) ion traps. By varying the trap voltages, we studied the velocity distribution of hydrogen atoms that would be produced upon threshold photodissociation of the BaH + . We found that hydrogen with a kinetic energy below 30 mK × k B can be produced in both traps, making the scheme suitable for loading hybrid ion–atom traps such as those used to synthesize and trap antihydrogen or study ultracold atom–ion collisions. We discuss how the dynamics of RF traps could be exploited to produce hydrogen below this limit by either driving the photodissociation transition with a small laser beam aligned along the axis of the trap, or by pulsing the laser during the micromotion turning points.
Abstract I present a novel scheme for producing cold (magnetically trappable) atomic hydrogen, based on threshold photodissociation of the BaH+ molecular ion. BaH+ can be sympathetically cooled using laser cooled Ba+ in an ion trap, before it is photodissociated on the single photon A1Σ+ ← X1Σ+ transition. The small mass ratio between Ba+ and BaH+ ensures a strong overlap within the ion trap for sympathetic cooling, while the large mass ratio between BaH+ and H means that the released hydrogen can be up to 139 times colder than the parent molecular ions. I examine the hydrogen production rate, and describe how the trap dynamics and photodissociation laser detuning influence the achievable energies. The low infrastructure costs and the ion trap nature of the scheme make it suitable for loading hydrogen into an antihydrogen experiment. This would support a direct matter–antimatter comparison, which could provide important clues as to why our Universe contains so little antimatter.
This dissertation details of the construction of and experiments performed in a hybrid system consisting of a cold neutral atomic magneto-optical trap (MOT) contained within a linear radio-frequency quadrupole ion trap (LQT). The combination of these two workhorses of atomic physics facilitates a variety of developing science such as the controlled investigation of ion-neutral quantum chemistry and the production of ground-state molecular ions. While the primary focus of this work is the production of ultracold molecular ions via sympathetic cooling, there has been investigation of cold (T ~ mK) ion-neutral charge exchange processes in two different ion-neutral pair systems. In addition, a possible method of producing ultracold homonuclear molecular ions via a photo-associative ionization (PAI) pathway is studied in the MOT. The LQT traps ions in spatial overlap with a 40Ca MOT constituting an ultracold buffer gas purposed to sympathetically cool molecular ions.An effective, general method of producing ground-state molecular ions would open a field of physics allowing, for example, precise measurements of molecular transitions which are uniquely sensitive to parity violation, or the possible variation of fundamental constants. Another promising application of cold molecular ions is an implementation of a quantum computing architecture by coupling micro-fabricated strip-line resonators to the microwave rotational transition found in many diatomic molecular ions. The molecular ion BaCl+ is chosen to be used in proof-of-principle sympathetic cooling experiments. Ultimately, a vibrational internal state thermometry experiment shows that the Ca MOT performs very efficiently at quenching the vibrational motion of the BaCl+ molecular ion.As a product of overcoming experimental challenges, this thesis discusses several experiments to characterize trapping and reaction dynamics in the hybrid system. For example, charge transfer measurements are performed with two different laser-cooled atomic ion species, Yb+ and Ba+, which are allowed and disallowed ground-state reaction, respectively. Controlled measurements of these inelastic processes test the cutting edge of quantum theory of ion-neutral interaction in both the ground-state and under optical excitation.
Abstract Reaching ultracold temperatures within hybrid atom–ion systems is a major limiting factor for control and exploration of the atom–ion interaction in the quantum regime. In this work, we present results on numerical simulations of trapped ion buffer gas cooling using an ultracold atomic gas in a large number of experimentally realistic scenarios. We explore the suppression of micromotion-induced heating effects through optimization of trap parameters for various radio-frequency (rf) traps and rf driving schemes including linear and octupole traps, digital Paul traps, rotating traps and hybrid optical/rf traps. We find that very similar ion energies can be reached in all of them even when considering experimental imperfections that cause so-called excess micromotion. Moreover we look into a quantum description of the system and show that quantum mechanics cannot save the ion from micromotion-induced heating in an atom–ion collision. The results suggest that buffer gas cooling can be used to reach close to the ion’s groundstate of motion and is even competitive when compared to some sub-Doppler cooling techniques such as Sisyphus cooling. Thus, buffer gas cooling is a viable alternative for ions that are not amenable to laser cooling, a result that may be of interest for studies into cold controlled quantum chemistry and charged impurity physics.
Over the past few decades, radiofrequency ion traps have become an attractive platform for studying chemical reactions as they enable a high degree of control over ion-molecule dynamics. In this review, we summarize techniques for the trapping and cooling of atomic and molecular ions in radiofrequency traps, including Doppler and resolved-sideband laser cooling, sympathetic cooling, and cryogenic buffer-gas methods. We discuss strategies for controlling key reaction parameters: the preparation of specific internal quantum states by internal cooling, optical pumping, state-selective photoionization and quantum logic spectroscopy; the manipulation of collision energies through micromotion control, dynamic trapping, and combination with molecular beams; and the selection of molecular structure via isotopic substitution, conformational separation, and isomer-specific ion generation. We illustrate applications of these approaches by discussing studies on quantum-state-dependent kinetics, quantum resonance effects, and structure-sensitive reactivity in ion-neutral collisions. We conclude by outlining future challenges, including full state-to-state reaction mapping, reaching the ultracold quantum regime free of micromotion, and the exploration of complex and chiral systems.
We have measured the ro-vibrational infrared transition (v = 0, J = 2) → (v = 4, J = 1) in ultracold HD+ molecular ions embedded inside Be+ Coulomb crystals, by 1+1 REMPI spectroscopy. The molecular ions, trapped in a linear radiofrequency trap, were cooled to temperatures of few tens of mK, via sympathetic cooling using laser-cooled Be+ ions. For detection, we have used secular excitation of the HD+ ions to monitor their loss rate. The transition frequency agrees with a theoretical prediction.
We report a method of efficiently generating ultracold hydrogen molecular ions HD+ in a segmented linear ion trap. HD+ ions are created by [2+1′] resonance-enhanced multiphoton ionization (REMPI) of an HD supersonic molecular beam, and sympathetically cooled by laser-cooled Be+ ions. The HD+ ions are generated species-selectively using 201 nm and 395 nm pulse lasers with energies of 0.08 mJ (5.1 × 106 W/cm2) and 1.5 mJ (9.5 × 107 W/cm2) respectively. The average loading rate of 4.3(2) HD+ ions per second in the ion trap is determined by comparing the experimental images with the simulated images of Be+-HD+ bi-component Coulomb crystals. This method paves a way to produce the state-selected HD+ ions, which can improve the signal strengths of the selected rovibrational transitions of HD+ ions.