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Springer eBooks

Cold Chemical Reactions Between Molecular Ions and Neutral Atoms

Jesús Pérez‐Ríos

Published Jan 1, 2020• 1 citation
Publisher
DOI
10.1007/978-3-030-55936-6_11

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The study of chemical reactions between ions and neutral species at very low energies reveals precise informations about the dynamics of collisions and fine details of intermolecular interactions. Here, we report progress towards the development of next- generation experiments for the investigation of cold ion-neutral reactions. First, we present a new ''dynamic" hybrid ion-atom trap which enables the study of collisions with a superior energy resolution accessing a regime in which quantum scattering resonances may become observable. Second, we discuss and numerically characterize the concept and properties of a hybrid trap for cold neutral molecules and molecular ions which paves the way for the study of ion-molecule reactions in the millikelvin regime.
Using a laser-cooled ion trapping apparatus, we have investigated laser-induced chemical reactions between cold trapped Ba+{\mathrm{Ba}}^{+}Ba+ ions and several neutral molecular gases at room temperature, O2{\mathrm{O}}_{2}O2​, CO2\mathrm{C}{\mathrm{O}}_{2}CO2​, and N2O{\mathrm{N}}_{2}\mathrm{O}N2​O, leading to the production of cold trapped $(\ensuremath{\approx}20\phantom{\rule{0.3em}{0ex}}\mathrm{mK})$ BaO+\mathrm{Ba}{\mathrm{O}}^{+}BaO+ ions. The BaO+\mathrm{Ba}{\mathrm{O}}^{+}BaO+ ions were converted back to Ba+{\mathrm{Ba}}^{+}Ba+ ions via reaction with room-temperature CO. Reaction rates were determined by employing molecular dynamics simulations. The cold mixed-species ion ensembles produced were used for studying the efficiency of sympathetic cooling, by variation of the ratio of laser-cooled to sympathetically cooled ion numbers. In one extreme case, 20 laser-cooled 138Ba+^{138}\mathrm{Ba}^{+}138Ba+ ions were capable of maintaining the translational temperature of 120 sympathetically cooled barium isotopes (135−−137Ba+)(^{135--137}\mathrm{Ba}^{+})(135−−137Ba+) and 430 138Ba16O+^{138}\mathrm{Ba}^{16}{\mathrm{O}}^{+}138Ba16O+ molecules at approximately 25mK25\phantom{\rule{0.3em}{0ex}}\mathrm{mK}25mK.
The recent development of a range of techniques for producing cold atoms and molecules at very low translational temperatures T < or = 1 K has provided the opportunity to investigate collisional processes in a new physical regime. We have recently presented a new experimental method to study low-temperature reactive collisions between translationally cold ions and neutral molecules (S. Willitsch et al., Phys. Rev. Lett. 2008, 100, 043203). Our technique relies on the combination of a quadrupole-guide velocity selector for the generation of translationally cold neutral molecules with a facility to produce ordered structures of cold ions (Coulomb crystals) by laser cooling in a linear quadrupole ion trap. The strong localisation of the ions in the trap in combination with the high sensitivity of laser-induced-fluorescence detection enabled us to study chemical reactions on the single-particle level, down to temperatures of T approximately 1 K. In the current paper, we present a detailed characterisation of the scope and limitations of this method based on our study of the reaction between laser-cooled Ca+ ions and velocity-selected CH3F molecules. The properties of our cold-neutrals source and the dependence of the measured rate constant on the shape of the Coulomb crystals, trapping and laser-cooling parameters are discussed. An extension of our technique for the study of low-temperature reactions with sympathetically cooled molecular ions (translational temperature T > 10 mK) is presented and first results on the charge-transfer reaction between OCS+ and ND3 are discussed. Finally, perspectives for further developments of our method are explored.