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Physical Review Letters

Measurement of a Large Chemical Reaction Rate between Ultracold Closed-Shell Ca40 Atoms and Open-Shell Yb+174 Ions Held in a Hybrid Atom-Ion Trap

Wade G. Rellergert, Scott T. Sullivan, Svetlana Kotochigova, Alexander N. Petrov, Kuang Chen, Steven J. Schowalter, Eric R. Hudson

Published Dec 7, 2011• 139 citations
Publisher

Abstract

Ultracold 174Yb+ ions and 40Ca atoms are confined in a hybrid trap. The charge exchange chemical reaction rate constant between these two species is measured and found to be 4 orders of magnitude larger than recent measurements in other heteronuclear systems. The structure of the CaYb+ molecule is determined and used in a calculation that explains the fast chemical reaction as a consequence of strong radiative charge transfer. A possible explanation is offered for the apparent contradiction between typical theoretical predictions and measurements of the radiative association process in this and other recent experiments.

DOI
10.1103/physrevlett.107.243201

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We estimate the radiative quenching rate of the $^{40}$Ca - $^{174}$Yb$^{+}$ molecular ion and find that it under-estimates the value reported in recent experiments by about 5 orders of magnitude. We comment on possible explanations for this large discrepancy.

arXiv:1211.5079•Nov 21, 2012•0 citations

Chemical Reaction of Ultracold Atoms and Ions in a Hybrid Trap

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We will present measurements and theoretical calculations of a surprisingly fast chemical reaction observed between ultracold 174Yb+ ions and 40Ca atoms held in a hybrid MOTION trap, which was constructed to produce ultracold molecular ions.

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Ion-neutral chemistry at ultralow energies: dynamics of reactive collisions between laser-cooled Ca+ ions and Rb atoms in an ion-atom hybrid trap

Felix H. J. Hall, Pascal Eberle, Gregor Hegi +4 more

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 ⟨E coll⟩/k B=20 mK-20 K. The lowest energies were achieved in experiments using single localised 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 analysed 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.

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Ion-neutral chemistry at ultralow energies: Dynamics of reactive collisions between laser-cooled Ca^+ ions and Rb atoms in an ion-atom hybrid trap

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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.

•Feb 19, 2013•0 citations

Charge Exchange Dynamics in Cold Collisions of 40CaH+ and 39K

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Abstract We report the observation of charge-exchange collisions between trapped calcium monohydride molecular ions (40CaH+) and ultracold potassium atoms (39K) in a hybrid ion-atom trap. The measured charge-exchange rate coefficient is significantly suppressed relative to the Langevin rate constant for the system. We use ab initio quantum-chemical calculations to model the (CaH-K)+ complex in the ground and excited electronic states and to identify possible charge-exchange mechanisms. Our calculations rule out a direct nonradiative charge-exchange reaction and instead point to a radiative mechanism, but do not quantitatively reproduce the measured rate, highlighting the need for a full-dimensional quantum dynamics treatment that includes vibrational motion and intermediate complex formation. Our work demonstrates that cold hybrid ion-atom platforms with molecular ions enable access to richer chemical complexity and collisional dynamics inaccessible in purely atomic systems.

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Cold Heteronuclear Atom-Ion Collisions

Christoph Zipkes, Stefan Palzer, Lothar Ratschbacher +2 more

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.

arXiv:1005.3846•Physical Review Letters•Sep 23, 2010•120 citations
Ultracold 174Yb+ ions and 40Ca atoms are confined in a hybrid trap. The charge exchange chemical reaction rate constant between these two species is measured and found to be 4 orders of magnitude larger than recent measurements in other heteronuclear systems. The structure of the CaYb+ molecule is determined and used in a calculation that explains the fast chemical reaction as a consequence of strong radiative charge transfer. A possible explanation is offered for the apparent contradiction between typical theoretical predictions and measurements of the radiative association process in this and other recent experiments.
We estimate the radiative quenching rate of the 40^{40}40Ca - 174^{174}174Yb+^{+}+ molecular ion and find that it under-estimates the value reported in recent experiments by about 5 orders of magnitude. We comment on possible explanations for this large discrepancy.
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 ⟨E coll⟩/k B=20 mK-20 K. The lowest energies were achieved in experiments using single localised 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 analysed 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.
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.
Abstract We report the observation of charge-exchange collisions between trapped calcium monohydride molecular ions (40CaH+) and ultracold potassium atoms (39K) in a hybrid ion-atom trap. The measured charge-exchange rate coefficient is significantly suppressed relative to the Langevin rate constant for the system. We use ab initio quantum-chemical calculations to model the (CaH-K)+ complex in the ground and excited electronic states and to identify possible charge-exchange mechanisms. Our calculations rule out a direct nonradiative charge-exchange reaction and instead point to a radiative mechanism, but do not quantitatively reproduce the measured rate, highlighting the need for a full-dimensional quantum dynamics treatment that includes vibrational motion and intermediate complex formation. Our work demonstrates that cold hybrid ion-atom platforms with molecular ions enable access to richer chemical complexity and collisional dynamics inaccessible in purely atomic systems.
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.