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arXiv:2501.17530 · Physical Review A

Ion-kinetic-energy sampling in a 22-pole trap using ring-electrode evaporation

Miguel Jiménez-Redondo, D. Gerlich, P. Caselli, Pavol Jusko

Published Jan 28, 2025• 1 citation
arXivHTMLPDF

Abstract

We present an experimental method for the characterization of the kinetic energies of ions confined in a 22-pole radio frequency trap by inducing a small potential barrier using the surrounding ring electrodes, allowing the selective extraction of ions. Energy sampling experiments have been performed on buffer-gas thermalized He + ions at trap temperatures between 10 and 180 K, resulting in distinct extraction curves as a function of the potential barrier, and a differentiated behavior depending on the escape time from the trap. The experiments are complemented by Monte Carlo simulations of the ion trajectories inside the calculated trap potential and allow us to investigate the properties of the sampling method, the role of ion motion coupling, and the impact of residual buffer-gas collisions on the observed results. The technique has also been successfully applied to identify energetic H 3 + ions produced in an exothermic reaction inside the trap. Upon calibration, this method can provide relative kinetic energy distributions or be used to filter the maximum desired kinetic energy of the ions inside the trap.

DOI
10.1103/physreva.111.013120

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We present an experimental method for the characterization of the kinetic energies of ions confined in a 22-pole radio frequency trap by inducing a small potential barrier using the surrounding ring electrodes, allowing the selective extraction of ions. Energy sampling experiments have been performed on buffer-gas thermalized He + ions at trap temperatures between 10 and 180 K, resulting in distinct extraction curves as a function of the potential barrier, and a differentiated behavior depending on the escape time from the trap. The experiments are complemented by Monte Carlo simulations of the ion trajectories inside the calculated trap potential and allow us to investigate the properties of the sampling method, the role of ion motion coupling, and the impact of residual buffer-gas collisions on the observed results. The technique has also been successfully applied to identify energetic H 3 + ions produced in an exothermic reaction inside the trap. Upon calibration, this method can provide relative kinetic energy distributions or be used to filter the maximum desired kinetic energy of the ions inside the trap.
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The immersion of a single ion confined by a radiofrequency (RF) trap in an ultracold atomic gas extends the concept of buffer gas cooling to a new temperature regime. The steady-state energy distribution of the ion is determined by its kinetics in the RF field rather than the temperature of the buffer gas. Moreover, the finite size of the ultracold gas facilitates the observation of back-action of the ion onto the buffer gas. We numerically investigate the system's properties depending on atom–ion mass ratio, trap geometry, differential cross-section and non-uniform neutral atom density distribution. Experimental results are well reproduced by our model considering only elastic collisions. We identify excess micromotion to set the typical scale for the ion energy statistics and explore the applicability of the mobility collision cross-section to the ultracold regime.
The kinetic energy distribution of a cloud of ions stored in a RF trap has been investigated by use of two methods based on phase-stopped ejection. The oscillation of the RF voltage is stopped at a phase corresponding to zero field Value inside the trap. After their subsequent ejection from the trap, the ions are detected by an electron multiplier. The instantaneous ion cloud temperature value corresponding to the phase-stopping time can be deduced from the recorded profile of the ion signal. An alternative method consists in submitting the ejected ions to a repulsive field, applied before the detector, which allows us to discriminate the velocity classes. In both cases, the experiments are interpreted thanks to a simple theoretical description of a cloud of ions at thermal equilibrium in a RF trap and to a precise calculation of the ejection process. Both methods are compared, for the various trap working points. In all cases, the ion cloud average temperature is of the order of a tenth of the potential well depth.
An ion in a radiofrequency (rf) trap sympathetically cooled by a simultaneously trapped neutral buffer gas exhibits deviations from thermal statistics caused by collision-induced coupling of the rf field to the ion motion. For a uniform density distribution of the buffer gas, the energy distribution of the ion can be described by Tsallis statistics. Moreover, runaway heating of the ion occurs if the buffer gas particles are sufficiently heavy relative to the ion. In typical experiments, however, ultracold buffer gases are confined in traps resulting in localised, non-uniform density distributions. Using a superstatistical approach, we develop an analytical model for an ion interacting with a localised buffer gas. We demonstrate theoretically that limiting collisions to the centre of the ion trap enables cooling at far greater mass ratios than achievable using a uniform buffer gas, but that an upper limit to the usable mass ratio exists even in this case. Furthermore, we analytically derive the functional form of the energy distribution for an ion interacting with a buffer gas held in a harmonic potential. The analytical distribution obtained is found to be in excellent agreement with the results of numerical simulations.
Cooling all degrees of freedom of a molecule, a cluster, or even a nanoparticle which is suspended in a vacuum, is an experimental challenge. Without suitable schemes, cold or ultracold chemical reactions are not feasible. Methods such as laser based preparation of very slow atoms, decelerating molecules to low velocities with electric fields or freezing molecular ions into Coulomb crystals, are generally not suitable to cool the vibrational or rotational motion of molecules. This contribution describes a new method in which a beam of slow atoms or molecules (H, He, H2, or D2) is used for cooling charged particles confined in a multi-electrode rf trap. For reaching sub-K temperatures, the fast part of a cold effusive beam is removed with a shutter before the slow remaining neutrals interact with the ion cloud. The development of a pulsed cold beam source is discussed as well as suitable methods for determining the ion temperature. A challenging application is to prepare internally cold CH5+ for spectroscopy or chemistry. New experimental results for hydrogen abstraction in collisions with slow H atoms are reported at energies of a few meV. For evaluating these measurements and for predicting effective rate coefficients at lower energies, the kinematic conditions of the slow neutral beam-ion trap arrangement have been analyzed in detail. The potential of cooling ions such as protonated methane or H3+ with slow energy selected H atoms is briefly mentioned. An interesting process is the formation of weakly bound ions such as H4+ or CH6+ via radiative or ternary association. Such ions are ideal candidates for preparing the corresponding collision complexes very close (microeV) to the dissociation continuum using infrared transitions.