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Faraday Discussions

Production of cold ND3 by kinematic cooling

Jeffrey J Kay, Sebastiaan Y. T. van de Meerakker, Kevin E. Strecker, David W. Chandler

Published Jan 1, 2009• 16 citations
Publisher

Abstract

We have produced translationally cold ammonia (ND3) molecules in various quantum states by kinematic cooling. In these experiments, ND3 molecules are brought nearly to rest in the (J, K) = (2,0), (2,1), (2,2), (3,1), (3,2), and (3,3) rotational levels of the ground vibronic state by rotationally-inelastic collisions with Ne atoms. The cold molecules are produced in quantum-state-dependent velocity distributions whose laboratory frame velocities are measured to be between 21 m s(-1) (E(trans)/k = 530 mk) and 32 m s(-1) (E(trans)/k = 1.2 K), and are calculated to be between 7.5 m s(-1) (E(trans)/k = 70 mK) and 27 m s(-1) (E(trans)/k = 880 mK). Due to systematic experimental effects, the measured velocities are upper limits to the actual velocities. These temperatures are low enough that it should be possible to use electrostatic traps to confine cold molecules in many of these quantum states.

DOI
10.1039/b819256c

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Faraday Discussions•Jan 1, 2009•76 citations
We have produced translationally cold ammonia (ND3) molecules in various quantum states by kinematic cooling. In these experiments, ND3 molecules are brought nearly to rest in the (J, K) = (2,0), (2,1), (2,2), (3,1), (3,2), and (3,3) rotational levels of the ground vibronic state by rotationally-inelastic collisions with Ne atoms. The cold molecules are produced in quantum-state-dependent velocity distributions whose laboratory frame velocities are measured to be between 21 m s(-1) (E(trans)/k = 530 mk) and 32 m s(-1) (E(trans)/k = 1.2 K), and are calculated to be between 7.5 m s(-1) (E(trans)/k = 70 mK) and 27 m s(-1) (E(trans)/k = 880 mK). Due to systematic experimental effects, the measured velocities are upper limits to the actual velocities. These temperatures are low enough that it should be possible to use electrostatic traps to confine cold molecules in many of these quantum states.
The measurement of the rotational state distribution of a velocity-selected, buffer-gas-cooled beam of ND3 is described. In an apparatus recently constructed to study cold ion-molecule collisions, the ND3 beam is extracted from a cryogenically cooled buffer-gas cell using a 2.15 m long electrostatic quadrupole guide with three 90° bends. (2+1) resonance enhanced multiphoton ionization spectra of molecules exiting the guide show that beams of ND3 can be produced with rotational state populations corresponding to approximately T(rot) = 9-18 K, achieved through manipulation of the temperature of the buffer-gas cell (operated at 6 K or 17 K), the identity of the buffer gas (He or Ne), or the relative densities of the buffer gas and ND3. The translational temperature of the guided ND3 is found to be similar in a 6 K helium and 17 K neon buffer-gas cell (peak kinetic energies of 6.92(0.13) K and 5.90(0.01) K, respectively). The characterization of this cold-molecule source provides an opportunity for the first experimental investigations into the rotational dependence of reaction cross sections in low temperature collisions.
Recently we developed a technique for producing cold molecules from a supersonic molecular beam via single collisions with a supersonic atomic beam [M. S. Elioff, J. J. Valentini, and D. W. Chandler, Science 302, 1940 (2003)]. This cooling technique necessarily produces the cold molecules at the relatively high density crossing of the atomic and molecular beams. In previous reports, secondary glancing collisions with the remnant atomic and molecular beams lead to rapid depletion of the cold molecules limiting the observation time to less than $10\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ with an estimated temperature of 440mK440\phantom{\rule{0.3em}{0ex}}\mathrm{mK}440mK. Here we present experimental conditions for the kinematic cooling technique which overcome the limitations of the previous experiments. We demonstrate the success of this experiment for the production of cold nitric oxide (NO) in the ground vibrational, j=7.5j=7.5j=7.5 rotational, state in order to compare with our previously reported data. With the present setup, we are able to extract the cold molecules from the pulsed molecular and atomic beams and we observe these cold NO(X)j=7.5\mathrm{NO}{(X)}_{j=7.5}NO(X)j=7.5​ persisting for over $150\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$. This long observation time demonstrates our ability to temporally and spatially separate the cold molecules from the parent atomic and molecular beams, simultaneously allowing for a better measurement of the final average velocity for the kinematically cooled molecules. From the data we find a final average velocity of the NO(X)j=7.5\mathrm{NO}{(X)}_{j=7.5}NO(X)j=7.5​ of approximately 4.5m∕s4.5\phantom{\rule{0.3em}{0ex}}\mathrm{m}∕\mathrm{s}4.5m∕s, consistent with simulations. The final observed average velocity is equated to a temperature of approximately 35mK35\phantom{\rule{0.3em}{0ex}}\mathrm{mK}35mK, over an order of magnitude colder than our previous measurements.
We present a theoretical study of elastic and rotationally inelastic collisions of NH3 and ND3 with rare gas atoms (He, Ne, Ar, Kr, Xe) at low energy. Quantum close-coupling calculations have been performed for energies between 0.001 and 300 cm(-1). We focus on collisions in which NH3 is initially in the upper state of the inversion doublet with j = 1, k = 1, which is the most relevant in an experimental context as it can be trapped electrostatically and Stark-decelerated. We discuss the presence of resonances in the elastic and inelastic cross sections, as well as the trends in the inelastic cross sections along the rare gas series and the differences between NH3 and ND3 as a colliding partner. We also demonstrate the importance of explicitly taking into account the umbrella (inversion) motion of NH3 in order to obtain accurate scattering cross sections at low collision energy. Finally, we investigate the possibility of sympathetic cooling of ammonia using cold or ultracold rare gas atoms. We show that some systems exhibit a large ratio of elastic to inelastic cross sections in the cold regime, which is promising for sympathetic cooling experiments. The close-coupling calculations are based on previously reported ab initio potential energy surfaces for NH3-He and NH3-Ar, as well as on new, four-dimensional, potential energy surfaces for the interaction of ammonia with Ne, Kr, and Xe, which were computed using the coupled-cluster method and large basis sets. We compare the properties of the potential energy surfaces corresponding to the interaction of ammonia with the various rare gas atoms.
We report the preparation and observation of translationally cold atoms using kinematic cooling. In these experiments, krypton atoms are cooled to subkelvin temperatures by elastic collisions in crossed atomic beams. Two independent velocity measurements indicate an upper-bound mean velocity of 13 m/s (Etrans/k=850mK{E}_{\mathrm{trans}}/k=850 \mathrm{mK}Etrans​/k=850mK) and are consistent with a much lower mean velocity of 4 m/s (Etrans/k=80mK{E}_{\mathrm{trans}}/k=80 \mathrm{mK}Etrans​/k=80mK) (kkk is Boltzmann's constant). The density of the cold atoms is measured to be 109{10}^{9}109 atoms/cm3{}^{3}3. Scattering calculations and diffusion models support these velocity and density measurements. The results demonstrate that cold, dense samples of ground-state atoms and molecules can be prepared by elastic collisions between identical collision partners.
We report the cooling of nitric oxide using a single collision between an argon atom and a molecule of NO. We have produced significant numbers (108 to 109 molecules per cubic centimeter per quantum state) of translationally cold NO molecules in a specific quantum state with an upper-limit root mean square laboratory velocity of 15 plus or minus 1 meters per second, corresponding to a 406 plus or minus 23 millikelvin upper limit of temperature, in a crossed molecular beam apparatus. The technique, which relies on a kinematic collapse of the velocity distributions of the molecular beams for the scattering events that produce cold molecules, is general and independent of the energy of the colliding partner.
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.