We have measured the reaction rates of trapped, buffer gas cooled Th$^{3+}$ and various gases and have analyzed the reaction products using trapped ion mass spectrometry techniques. Ion trap lifetimes are usually limited by reactions with background molecules, and the high electron affinity of multiply charged ions such as Th$^{3+}$ make them more prone to loss. Our results show that reactions of Th$^{3+}$ with carbon dioxide, methane, and oxygen all occur near the classical Langevin rate, while reaction rates with argon, hydrogen, and nitrogen are orders of magnitude lower. Reactions of Th$^{3+}$ with oxygen and methane proceed primarily via charge exchange, while simultaneous charge exchange and chemical reaction occurs between Th$^{3+}$ and carbon dioxide. Loss rates of Th$^{3+}$ in helium are consistent with reaction with impurities in the gas. Reaction rates of Th$^{3+}$ with nitrogen and argon depend on the internal electronic configuration of the Th$^{3+}$.
We measure chemical reactions between a single trapped $^{174}$Yb$^+$ ion immersed in an ultracold bath of $^6$Li atoms containing trace amounts of Li$_2$ dimers. This produces LiYb$^+$ molecular ions that we detect via mass spectrometry. We explain the reaction rates by modelling the dimer density as a function of the magnetic field and obtain excellent agreement when we assume the reaction to follow the Langevin rate. Our results present a novel approach towards the creation of cold molecular ions and point to the exploration of ultracold chemistry in ion molecule collisions. What is more, w…
A recent expansion of cold and ultracold molecule applications has led to renewed focus on molecular species preparation under ultrahigh vacuum conditions. Meanwhile, molecular beams have been used to study gas phase chemical reactions for decades. In this manuscript, we describe an apparatus that uses pulsed molecular beam technology to achieve high local gas densities, leading to faster reaction rates with cold trapped ions. We characterize the beam's spatial profile using the trapped ions themselves. This apparatus could be used for preparation of molecular species by reactions requiring ex…
The gas-phase reaction of CCl+ with acetonitrile (CH3CN) is studied using a linear Paul ion trap coupled to a time-of-flight mass spectrometer. This work builds on a previous study of the reaction of CCl+ with acetylene and further explores the reactivity of CCl+ with organic neutral molecules. Both of the reactant species are relevant in observations and models of chemistry in the interstellar medium (ISM). Nitriles, in particular, are noted for their relevance in prebiotic chemistry, such as is found in the atmosphere of Titan, one of Saturn's moons. This work represents one of the first stu…
The two most widely used ion cooling methods are laser cooling and sympathetic cooling by elastic collisions (ECs). Here we demonstrate another method of cooling ions that is based on resonant charge exchange (RCE) between the trapped ion and the ultracold parent atom. Specifically, trapped Cs$^{+}$ ions are cooled by collisions with co-trapped, ultracold Cs atoms and, separately, by collisions with co-trapped, ultracold Rb atoms. We observe that the cooling of Cs$^{+}$ ions by Cs atoms is more efficient than cooling of Cs$^{+}$ ions by Rb atoms. This signals the presence of a cooling mechanis…
We investigate theoretically the possibility for robust and fast cooling of a trapped atomic ion by transient interaction with a pre-cooled ion. The transient coupling is achieved through dynamical control of the ions' equilibrium positions. To achieve short cooling times we make use of shortcuts to adiabaticity by applying invariant-based engineering. We design these to take account of imperfections such as stray fields, and trap frequency offsets. For settings appropriate to a currently operational trap in our laboratory, we find that robust performance could be achieved down to $6.3$ motion…
We have developed a novel scheme to measure the secular motion of trapped ions. Employing pulsed excitation and analysis of the fluorescence of laser cooled ions, we have measured the centre-of-mass mode frequency of single as well as entire ion crystals with a frequency precision better than 5e-4 within an interrogation time on the order of seconds, limited only by the fluorescence collection efficiency and the background noise. We have used this method to measure the mass of ions and observed charge exchange collisions between trapped calcium isotopes.
The tunneling reaction H$_2$ + D$^-$ $\rightarrow$ HD + H$^-$ was studied in a recent experimental work at low temperatures (10, 19, and 23~K) by Endres {\it et al.}, Phys. Rev. A {\bf 95}, 022706 (2017). An upper limit of the rate coefficient was found to be about 10$^{-18}$ cm$^3$/s. In the present study, reaction probabilities are determined using the ABC program developed by Skouteris {\it et al.}, Comput. Phys. Commun. {\bf 133}, 128 (2000). The probabilities for ortho-H$_2$ and para-H$_2$ in their ground rovibrational states are obtained numerically at collision energies above 50~meV wit…
The loss of ultracold trapped atoms in the vicinity of a Feshbach resonance is treated as a two-stage reaction, using the Breit-Wigner theory. The first stage is the formation of a resonant diatomic molecule, and the second one is its deactivation by inelastic collisions with other atoms. This model is applied to the analysis of recent experiments on $^{87}$Rb, leading to an estimated value of $7\times 10^{-11}$ cm$^{3}/$s for the deactivation rate coefficient.
Electric-field noise from the surfaces of ion-trap electrodes couples to the ion's charge causing heating of the ion's motional modes. This heating limits the fidelity of quantum gates implemented in quantum information processing experiments. The exact mechanism that gives rise to electric-field noise from surfaces is not well-understood and remains an active area of research. In this work, we detail experiments intended to measure ion motional heating rates with exchangeable surfaces positioned in close proximity to the ion, as a sensor to electric-field noise. We have prepared samples with …
We present measurements of the charge-exchange reaction rate between neutral sodium (Na) and ionized calcium (\ce{Ca+}) in a hybrid atom-ion trap, which is comprised of a Na magneto-optical trap concentric with a linear Paul trap. Once the Na and \ce{Ca+} are co-trapped, the reaction rate is measured by continuously quenching the reaction product \ce{Na+} from the ion trap, and then destructively measuring the decay of the remaining ion population. The reactants' electronic state and temperature are experimentally controlled, allowing us to determine the four individual reaction-rates between …
We present a method for generating cold neutral atoms via charge exchange reactions between trapped ions and Rydberg positronium. The high charge exchange reaction cross section leads to efficient neutralisation of the ions and since the positronium-ion mass ratio is small, the neutrals do not gain appreciable kinetic energy in the process. When the original ions are cold the reaction produces neutrals that can be trapped or further manipulated with electromagnetic fields. Because a wide range of species can be targeted we envisage that our scheme may enable experiments at low temperature that…
The rate constants for recombination and exchange reactions are calculated using the flux correlation approach with a general form of the Boltzmannized flux operator, which can simultaneously describe the Kubo and traditional half-split forms. First, we consider an exactly solvable model, i.e., the free particle case, in terms of a new scaling function. Next, as a non-trivial case, we study the recombination and exchange reactions at very high pressure. Since the rate constant is calculated by Laplace transform of the flux correlation function, the result depends on how the Boltzmannized flux …
Ultracold molecules offer remarkable opportunities to study chemical reactions at nearly zero temperature. Although significant progresses have been achieved in exploring ultracold bimolecular reactions, the investigations are usually limited to measurements of the overall loss rates of the reactants. Detection of the reaction products will shed new light on understanding the reaction mechanism and provide a unique opportunity to study the state-to-state reaction dynamics. Here we report on the direct observation of an exoergic atom-exchange reaction in an ultracold atom-dimer mixture. Both th…
Trapped Be+ ions are a leading platform for quantum information science [1], but reactions with background gas species, such as H2 and H2O, result in qubit loss. Our experiment reveals that the BeOH+ ion is the final trapped ion species when both H2 and H2O exist in a vacuum system with cold, trapped Be+. To understand the loss mechanism, low-temperature reactions between sympathetically cooled BeD+ ions and H2O molecules have been investigated using an integrated, laser-cooled Be+ ion trap and high-resolution Time-of-Flight (TOF) mass spectrometer (MS) [2]. Among all the possible products,BeH…
The control of chemical reactions is a recurring theme in physics and chemistry. Traditionally, chemical reactions have been investigated by tuning thermodynamic parameters, such as temperature or pressure. More recently, physical methods such as laser or magnetic field control have emerged to provide completely new experimental possibilities, in particular in the realm of cold collisions. The control of reaction pathways is also a critical component to implement molecular quantum information processing. For these undertakings, single particles provide a clean and well-controlled experimental …
We show that isotope-exchange reactions between ground-state alkali-metal, alkaline-earth-metal, and lanthanide heteronuclear dimers consisting of two isotopes of the same atom are exothermic with an energy change in the range of 1-8000$\,$MHz thus resulting in cold or ultracold products. For these chemical reactions there are only one rovibrational and at most several hyperfine possible product states. The number and energetics of open and closed reactive channels can be controlled by the laser and magnetic fields. We suggest a laser-induced isotope- and state-selective Stark shift control to…
Trapping molecular ions that have been sympathetically cooled with laser-cooled atomic ions is a useful platform for exploring cold ion chemistry. We designed and characterized a new experimental apparatus for probing chemical reaction dynamics between molecular cations and neutral radicals at temperatures below 1 K. The ions are trapped in a linear quadrupole radio-frequency trap and sympathetically cooled by co-trapped, laser-cooled, atomic ions. The ion trap is coupled to a time-of-flight mass spectrometer to readily identify product ion species, as well as to accurately determine trapped i…
Microscopic control over polar molecules with tunable interactions would enable realization of novel quantum phenomena. Using an applied electric field gradient, we demonstrate layer-resolved state preparation and imaging of ultracold potassium-rubidium molecules confined to two-dimensional planes in an optical lattice. The coherence time of rotational superpositions in individual layers is maximized by rotating the electric field relative to the optical trap polarization to achieve state-insensitive trapping. Molecules in adjacent layers interact via dipolar exchange of rotational angular mom…
We theoretically study trapped ions that are immersed in an ultracold gas of Rydberg-dressed atoms. By off-resonant coupling on a dipole-forbidden transition, the adiabatic atom-ion potential can be made repulsive. We study the energy exchange between the atoms and a single trapped ion and find that Langevin collisions are inhibited in the ultracold regime for these repulsive interactions. Therefore, the proposed system avoids recently observed ion heating in hybrid atom-ion systems caused by coupling to the ion's radio frequency trapping field and retains ultracold temperatures even in the pr…
The interaction between the electric dipole moment of a trapped molecular ion and the configuration of the confined Coulomb crystal couples the orientation of the molecule to its motion. We consider the practical feasibility of harnessing this interaction to initialize, process, and read out quantum information encoded in molecular ion qubits without optically illuminating the molecules. We present two schemes wherein a molecular ion can be entangled with a co-trapped atomic ion qubit, providing, among other things, a means for molecular state preparation and measurement. We also show that vir…
The velocity dependence of the stopping power of swift protons and deuterons in low energy collisions is investigated. At low projectile energies the stopping is mainly due to nuclear stopping and charge exchange of the electron. The second mechanism dominates after Ep >=200 eV. A dynamical treatment of the charge exchange mechanism based on two-center electronic wavefunctions yields very transparent results for the exchange probability. We predict that the stopping cross sections vary approximately as v to the 1.35 power for projectile protons on hydrogen targets in the 1 keV energy region.
