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Physical Review Letters

Laser-Assisted Evaporative Cooling of Anions

G. Cerchiari, P. Yzombard, A. Kellerbauer

Published Sep 6, 2019• 18 citations
Publisher

Abstract

We report the first cooling of atomic anions by laser radiation. O^{-} ions confined in a linear Paul trap were cooled by selectively photodetaching the hottest particles. For this purpose, anions with the highest total energy were illuminated with a 532 nm laser at their maximal radial excursion. Using laser-particle interaction, we realized a both colder and denser ion cloud, achieving a more than threefold temperature reduction from 1.15 to 0.33 eV. Compared with the interaction with a dilute buffer gas, the energy-selective addressing and removal of anions resulted in lower final temperatures, yet acted 10 times faster and preserved twice as large a fraction of ions in the final state. An ensemble of cold negative ions affords the ability to sympathetically cool any other negative ion species, enabling or facilitating a broad range of fundamental studies from interstellar chemistry to antimatter gravity. The technique can be extended to any negative ion species that can be neutralized via photodetachment.

DOI
10.1103/physrevlett.123.103201

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Physical Review A•Sep 13, 2017•10 citations
We report the first cooling of atomic anions by laser radiation. O^{-} ions confined in a linear Paul trap were cooled by selectively photodetaching the hottest particles. For this purpose, anions with the highest total energy were illuminated with a 532 nm laser at their maximal radial excursion. Using laser-particle interaction, we realized a both colder and denser ion cloud, achieving a more than threefold temperature reduction from 1.15 to 0.33 eV. Compared with the interaction with a dilute buffer gas, the energy-selective addressing and removal of anions resulted in lower final temperatures, yet acted 10 times faster and preserved twice as large a fraction of ions in the final state. An ensemble of cold negative ions affords the ability to sympathetically cool any other negative ion species, enabling or facilitating a broad range of fundamental studies from interstellar chemistry to antimatter gravity. The technique can be extended to any negative ion species that can be neutralized via photodetachment.
The study of cold and controlled molecular ions is pivotal for fundamental research in modern physics and chemistry. Investigations into cooling molecular anions, in particular, have proven to be of key consequence for the production of cold antihydrogen, the creation, and study of anionic Coulomb crystals as well as in atmospheric research and astrochemistry. The commonly used anion cooling technique via collisions with a buffer gas is limited by the temperature of the used cryogenic cooling medium. Here, we demonstrate forced evaporative cooling of anions via a laser beam with photon energies far above the photodetachment threshold of the anion. We reach runaway evaporative cooling of an anionic OH−^{-}− ensemble from an initial temperature of 370(12) K down to 2.2(8) K. This corresponds to three orders of magnitude increase in the ions' phase space density approaching the near-strong Coulomb coupling regime. A quantitative analysis of the experimental results, via a full thermodynamic model including the role of intrinsic collisional heating, represents the anion cooling dynamics without any fitting parameters. This technique can be used to cool, in principle, any anionic species below liquid helium temperature, providing a novel tool to push the frontiers of anion cooling to much lower than the state-of-the-art temperature regimes.
Atomic anions are generally not amenable to optical spectroscopy because they are loosely bound systems and rarely have bound excited states. Until recently, there was only one known negative ion with a strong bound–bound electronic transition, the osmium anion Os − . The electric-dipole transition between the 4 F e 9/2 ground and 6 D o J excited state of this ion provides unique insight into the structure of atomic anions. In addition, it may enable the preparation of ultracold ensembles of negative ions. Laser excitation of the electric-dipole transition in Os − ions could be used to laser-cool them to microkelvin temperatures. If demonstrated to be successful, the technique would allow the cooling of any species of negatively charged ions - from subatomic particles to molecular anions - to ultracold temperatures by sympathetic cooling. We have been investigating the bound-bound electric-dipole transition in Os − by high-resolution laser spectroscopy with a view to using it for the first laser cooling of negative ions. The principle of the method, its potential applications, as well as experimental results are presented.
We propose to extend laser-cooling techniques, so far only achieved for neutral molecules, to molecular anions. A detailed computational study is performed for molecules stored in Penning traps using GPU based Monte Carlo simulations. Two cooling schemes—Doppler laser cooling and photodetachment cooling—are investigated. The sympathetic cooling of antiprotons is studied for the Doppler cooling scheme, where it is shown that cooling of antiprotons to subKelvin temperatures could becomes feasible, with impacts on the field of antimatter physics. The presented cooling schemes also have applications for the generation of cold, negatively charged particle sources and for the sympathetic cooling of other molecular anions.
This thesis reports on experimental and theoretical studies of the sympathetic cooling of complex molecular ions demonstrating that this general method for cooling atomic and molecular ions is reliable and efficient. For this purpose, complex molecular ions and barium ions have been confined simultaneously in a linear Paul trap. The complex molecular ions are generated in an electrospray ionization system and transferred to the trap via a 2 m long octopole ion guide. These molecular ions are pre-cooled by room temperature helium buffer gas so that they can be captured by the trap. The atomic barium ions are loaded from a barium evaporator oven and are laser-cooled by a 493 nm cooling laser and a 650 nm repumping laser. Due to the mutual Coulomb interaction among these charged particles, the kinetic energy of the complex molecular ions can be reduced significantly. In our experiments we have demonstrated the sympathetic cooling of various molecules (CO2, Alexa Fluor 350, glycyrrhetinic acid, cytochrome c) covering a wide mass range from a few tens to 13000 amu. In every case the molecular ions could be cooled down to millikelvin temperatures. Photo-chemical reactions of the 138Ba+ ions in the (2P1/2) excited state with gases such as O2, CO2, or N2O, could be observed. If the initial 138Ba+ ion ensemble is cold, the produced 138BaO+ ions are cold as well, with a similar temperature as the laser-cooled barium ions (a few tens of millikelvin). The back-reaction of 138BaO+ ions with neutral CO to 138Ba+ is possible and was observed in our experiments as well. A powerful molecular dynamics (MD) simulation program has been developed. With this program dynamic properties of ion ensembles, such as sympathetic interactions or heating effects, have been investigated and experimental results have been analyzed to obtain, for example, ion numbers and temperatures. Additionally, the feasibility of nondestructive spectroscopy via an optical dipole excitation and the lineshape of rovibrational transitions of 1.4 and 5.1 μm have been studied.
We propose a scheme for laser cooling of negatively charged molecules. We briefly summarize the requirements for such laser cooling and we identify a number of potential candidates. A detailed computation study with C_{2}^{-}, the most studied molecular anion, is carried out. Simulations of 3D laser cooling in a gas phase show that this molecule could be cooled down to below 1 mK in only a few tens of milliseconds, using standard lasers. Sisyphus cooling, where no photodetachment process is present, as well as Doppler laser cooling of trapped C_{2}^{-}, are also simulated. This cooling scheme has an impact on the study of cold molecules, molecular anions, charged particle sources, and antimatter physics.
We discuss the possibility of using optical dipole forces for Sisyphus cooling of ions stored in a Penning trap by addressing the specific case of the molecular cooling candidate ${{\mathrm{C}}_{2}}^{\ensuremath{-}}$. Using a GPU accelerated code for Penning trap simulations, which we extended to include the molecule-light interaction, we show that this scheme can decrease the time required for cooling by an order of magnitude with respect to Doppler cooling. In our simulation we found that a reduction of the axial anion temperature from 10K10\phantom{\rule{0.28em}{0ex}}\mathrm{K}10K to 50mK50\phantom{\rule{0.28em}{0ex}}\mathrm{mK}50mK in around 10s10\phantom{\rule{0.28em}{0ex}}\mathrm{s}10s is possible. The temperature of the radial degrees of freedom was seen to thermalize to 150mK150\phantom{\rule{0.28em}{0ex}}\mathrm{mK}150mK. Based on the laser-cooled ${{\mathrm{C}}_{2}}^{\ensuremath{-}}$, a study on the sympathetic cooling of anions with masses 1--50 nucleon was performed, covering relevant candidates for investigations of chemical anion reactions at ultracold temperatures as well as for antimatter studies.