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arXiv:1608.07043 · Physical Review A

Characterization of charge-exchange collisions between ultracold Li6 atoms and Ca40+ ions

Ryoichi Saito, Shinsuke Haze, Mizuki Sasakawa, R. Nakai, Maurice Raoult, Humberto da Silva, Olivier Dulieu, Takashi Mukaiyama

Published Mar 31, 2017• 48 citations
arXivHTMLPDF

Abstract

We investigate the energy dependence and the internal-state dependence of the charge-exchange collision cross sections in a mixture of $^{6}\mathrm{Li}$ atoms and ${^{40}\mathrm{Ca}}^{+}$ ions. Deliberately excited ion micromotion is used to control collision energy of atoms and ions. The energy dependence of the charge-exchange collision cross section obeys the Langevin model in the temperature range of the current experiment, and the measured magnitude of the cross section is correlated to the internal state of the ${^{40}\mathrm{Ca}}^{+}$ ions. Revealing the relationship between the charge-exchange collision cross sections and the interaction potentials is an important step toward the realization of the full quantum control of the chemical reactions at an ultralow-temperature regime.

DOI
10.1103/physreva.95.032709

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We investigate the energy dependence and the internal-state dependence of the charge-exchange collision cross sections in a mixture of 6Li^{6}\mathrm{Li}6Li atoms and 40Ca+{^{40}\mathrm{Ca}}^{+}40Ca+ ions. Deliberately excited ion micromotion is used to control collision energy of atoms and ions. The energy dependence of the charge-exchange collision cross section obeys the Langevin model in the temperature range of the current experiment, and the measured magnitude of the cross section is correlated to the internal state of the 40Ca+{^{40}\mathrm{Ca}}^{+}40Ca+ ions. Revealing the relationship between the charge-exchange collision cross sections and the interaction potentials is an important step toward the realization of the full quantum control of the chemical reactions at an ultralow-temperature regime.
Charge-exchange collisions between ultracold fermionic 6Li^{6}\mathrm{Li}6Li atoms and 40Ca+^{40}\mathrm{Ca}^{+}40Ca+ ions are observed in the millikelvin temperature range. The reaction product of the charge-exchange collision is identified via mass spectrometry during which the motion of the ions is excited parametrically. The cross sections of the charge-exchange collisions between 6Li^{6}\mathrm{Li}6Li atoms in the ground state and 40Ca+^{40}\mathrm{Ca}^{+}40Ca+ ions in the ground and metastable excited states are determined. Investigation of the inelastic collision characteristics in the atom-ion mixture is an important step toward ultracold chemistry based on ultracold atoms and ions.
Abstract Hybrid atom-ion systems are a rich and powerful platform for studying chemical reactions, as they feature both excellent control over the electronic state preparation and readout as well as a versatile tunability over the scattering energy, ranging from the few-partial wave regime to the quantum regime. In this work, we make use of these excellent control knobs, and present a joint experimental and theoretical study of the collisions of a single 138Ba+ ion prepared in the 5 d 2 D 3 / 2 , 5 / 2 metastable states with a ground state 6Li gas near quantum degeneracy. We show that in contrast to previously reported atom-ion mixtures, several non-radiative processes, including charge exchange, excitation exchange and quenching, compete with each other due to the inherent complexity of the ion-atom molecular structure. We present a full quantum model based on high-level electronic structure calculations involving spin-orbit couplings. Results are in excellent agreement with observations, highlighting the strong coupling between the internal angular momenta and the mechanical rotation of the colliding pair, which is relevant in any other hybrid system composed of an alkali-metal atom and an alkaline-earth ion.
We study cold heteronuclear atom-ion collisions by immersing a trapped single ion into an ultracold atomic cloud. Using ultracold atoms as reaction targets, our measurement is sensitive to elastic collisions with extremely small energy transfer. The observed energy-dependent elastic atom-ion scattering rate deviates significantly from the prediction of Langevin but is in full agreement with the quantum mechanical cross section. Additionally, we characterize inelastic collisions leading to chemical reactions at the single particle level and measure the energy-dependent reaction rate constants. The reaction products are identified by in-trap mass spectrometry, revealing the branching ratio between radiative and nonradiative charge exchange processes.
Studies of charge transfer and total cross sections in elastic collisions of atom-ion alkali metals at ultralow temperatures are reported. Calculations for Na+Na+\mathrm{Na}+{\mathrm{Na}}^{+}Na+Na+ have been carried out with the best available ${}^{2}{\ensuremath{\Sigma}}_{g}^{+}$ and ${}^{2}{\ensuremath{\Sigma}}_{u}^{+}$ potential curves. As functions of energy, the cross sections show considerable structure and are large in the limit of low temperature. The scattering lengths were also computed, and the effective range expansion verified. For higher temperatures, we compare quantal and semiclassical results, and investigate the range of applicability of the Langevin formula. Even at temperatures of a few degrees kelvin, the charge-transfer cross sections are large, and could provide an efficient way to produce cold ions.
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+\\text{Na}-\\text{Ca}^+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.
Cold chemical reactions between laser-cooled Ca^+ ions and Rb atoms were studied in an ion-atom hybrid trap. Reaction rate constants were determined in the range of collision energies /k_B = 20 mK-20 K. The lowest energies were achieved in experiments using single localized Ca^+ ions. Product branching ratios were studied using resonant-excitation mass spectrometry. The dynamics of the reactive processes in this system (non-radiative and radiative charge transfer as well as radiative association leading to the formation of CaRb^+ molecular ions) have been analyzed using high-level quantum-chemical calculations of the potential energy curves of CaRb^+ and quantum-scattering calculations for the radiative channels. For the present low-energy scattering experiments, it is shown that the energy dependence of the reaction rate constants is governed by long-range interactions in line with the classical Langevin model, but their magnitude is determined by short-range non-adiabatic and radiative couplings which only weakly depend on the asymptotic energy. The quantum character of the collisions is predicted to manifest itself in the occurrence of narrow shape resonances at well-defined collision energies. The present results highlight both universal and system-specific phenomena in cold ion-neutral reactive collisions.