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Physical Chemistry Chemical Physics

Chemical applications of laser- and sympathetically-cooled ions in ion traps

Stefan Willitsch, Martin T. Bell, Alexander D. Gingell, T. P. Softley

Published Jan 1, 2008• 146 citations
Publisher

Abstract

Ensembles of cold atomic and molecular ions in ion traps prepared at millikelvin temperatures by laser and sympathetic cooling have recently found considerable interest in both physics and chemistry. At very low temperatures the ions form ordered structures in the trap also known as "Coulomb crystals". Ion Coulomb crystals exhibit a range of intriguing properties which render them attractive systems for novel experiments in chemical dynamics, ultrahigh-resolution spectroscopy and quantum-information processing. In this article we review the methods used to prepare atomic and molecular ion Coulomb crystals and discuss some recent studies in mass spectrometry, low-temperature chemistry and precision spectroscopy to illustrate their scientific potential for chemical applications. Finally, we conclude with an outlook on outstanding challenges and prospective further developments in the field.

DOI
10.1039/b813408c

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Ensembles of cold atomic and molecular ions in ion traps prepared at millikelvin temperatures by laser and sympathetic cooling have recently found considerable interest in both physics and chemistry. At very low temperatures the ions form ordered structures in the trap also known as "Coulomb crystals". Ion Coulomb crystals exhibit a range of intriguing properties which render them attractive systems for novel experiments in chemical dynamics, ultrahigh-resolution spectroscopy and quantum-information processing. In this article we review the methods used to prepare atomic and molecular ion Coulomb crystals and discuss some recent studies in mass spectrometry, low-temperature chemistry and precision spectroscopy to illustrate their scientific potential for chemical applications. Finally, we conclude with an outlook on outstanding challenges and prospective further developments in the field.
Translationally cold, spatially localised molecular ions prepared by sympathetic cooling with laser-cooled atomic ions in ion traps have recently found a wide range of applications in both chemistry and physics. The very low temperatures of the ions (down to millikelvins), their tight localisation in the trap and the ability to control and manipulate single isolated molecules on the quantum level offer intriguing possibilities for new experiments in the realms of cold chemistry, precision molecular spectroscopy, mass spectrometry and quantum technology. The present article gives an overview of the basic experimental methods, current topics and recent developments in this field.
We report the sympathetic cooling and Coulomb crystallization of molecular ions above the surface of an ion-trap chip. N2+{\mathrm{N}}_{2}^{+}N2+​ and CaH+{\mathrm{CaH}}^{+}CaH+ ions were confined in a surface-electrode radio-frequency (rf) ion trap and cooled by the interaction with laser-cooled Ca+{\mathrm{Ca}}^{+}Ca+ ions to secular translational temperatures in the millikelvin range. The configuration of trapping potentials generated by the surface electrodes enabled the formation of planar bicomponent Coulomb crystals and the spatial separation of the molecular from the atomic ions on the chip. The structural and thermal properties of the Coulomb crystals were characterized using molecular dynamics simulations. The present study extends chip-based trapping techniques to cold molecular ions with potential applications in mass spectrometry, chemistry, quantum information science, and spectroscopy.
Cold molecular ions are of great interest for applications in cold collision studies, chemistry, precision spectroscopy and quantum technologies. In this context, sympathetic cooling of molecular ions by the interaction with laser-cooled atomic ions is a powerful method to cool their translational motion and achieve translational temperatures in the millikelvin range. Recently, we implemented this method in a surface-electrode ion trap. The flexibility in shaping the trapping potentials offered by the surface-electrode structure enabled us to generate planar bicomponent Coulomb crystals and spatially separate the molecular from the atomic ions. Here, we present a detailed description of the fabrication and simulation of the trap as well as a theoretical and experimental investigation of the structural and energetic properties of the Coulomb crystals obtained in the device. We discuss in more detail the separation of different ion species using static electric fields and explore the effects of trap anharmoncities on the shape of bicomponent crystals.
Laser cooling of atomic ions has long been used as a tool in physics to explore quantum entanglement for applications in quantum computing and information. More recently, laser-cooled atomic ions have been used as a platform for studying cold chemistry. Here, we describe an experimental system called a “Coulomb crystal,” where laser-cooled ions are confined in traps at sufficiently low translational energies that they form an ordered structure. We then present a range of experiments undertaken using this platform, from studies of reactions with an atomic species to reaction systems of increased complexity, involving molecular ions and neutral molecules. We also describe a few spectroscopic studies enabled by Coulomb crystals before discussing some possible future directions of the field. This is not meant to be a comprehensive review of the entire field, but rather a sampling of the types of experiments that can be performed and the knowledge gained from these studies.
The generation and study of 'cold' gas-phase molecules characterised by very low translational temperatures Ttrans ? 1 K is an upcoming field of research in physical chemistry which has received considerable attention over the past years. A particular interesting form of cold molecules are ensembles of cold localised cations in ion traps which form ordered structures known as 'Coulomb crystals'. The present article reviews the experimental methods used for the generation of atomic and molecular Coulomb crystals and highlights recent experiments which take advantage of their intriguing properties in order to study chemical reactions at very low temperatures with single-particle sensitivity.
In this Perspective, we examine the use of laser-cooled atomic ions and sympathetically cooled molecular ions in Coulomb crystals for molecular spectroscopy. Coulomb crystals are well-isolated environments that provide localization and long storage times for sensitive measurements of weak signals and cold temperatures for precise spectroscopy. Coulomb crystals of molecular and atomic ions enable the detection of single-photon molecular ion transitions at a range of wavelengths by a change in atomic ion fluorescence at visible wavelengths. We give an overview of the state of the art from action spectroscopy to quantum logic spectroscopy for a wide range of molecular transitions from rotational sublevels separated by 10 –7 cm –1 to rovibronic transitions at 25 000 cm –1 . We emphasize how this system allows for unparalleled control of the molecular ion state for precision spectroscopy with applications in astrochemistry and fundamental physics. We conclude with an outlook of the use of this control in cold molecular ion reactions.