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Physical Review A

Kinematic production of isolated millikelvin molecules

Kevin E. Strecker, David W. Chandler

Published Dec 3, 2008• 21 citations
Publisher

Abstract

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 $440\phantom{\rule{0.3em}{0ex}}\mathrm{mK}$. 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, $j=7.5$ 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 $\mathrm{NO}{(X)}_{j=7.5}$ 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 $\mathrm{NO}{(X)}_{j=7.5}$ of approximately $4.5\phantom{\rule{0.3em}{0ex}}\mathrm{m}∕\mathrm{s}$, consistent with simulations. The final observed average velocity is equated to a temperature of approximately $35\phantom{\rule{0.3em}{0ex}}\mathrm{mK}$, over an order of magnitude colder than our previous measurements.

DOI
10.1103/physreva.78.063406

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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.
We report the cooling of nitric oxide molecules in a single collision between an argon atom and an NO molecule at collision energies of 5.65 {+-} 0.36 kJ/mol and 14.7 {+-} 0.9 kJ/mol in a crossed molecular beam apparatus. We have produced in significant numbers ({approx}10{sup 8} molecules cm{sup -3} per quantum state) translationally cold NO({sup 2}{Pi}{sub 1/2}, {nu}' = 0, j' = 7.5) molecules in a specific quantum state with an upper-limit laboratory-frame rms velocity of 14.8 {+-} 1.1 m/s, corresponding to a temperature of 406 {+-} 28 mK. The translational cooling results from the kinematic collapse of the velocity distribution of the NO molecules after collision. Increasing the collision energy by increasing the velocity of the argon atoms, as we do here, does shift the scattering angle at which the cold molecules appear, but does not result in an experimentally measurable change in the velocity spread of the cold NO. This is entirely consistent with our analysis of the kinematics of the scattering which predicts that the velocity spread will actually decrease with increasing argon atom velocity.
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 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.
This thesis describes the development of a relatively novel technique for the gen- eration and subsequent trapping of cold species. Molecules in a pulsed supersonic expansion are photolysed, such that the centre-of-mass velocity vector of one of the fragments is equal in magnitude but opposed in orientation to the lab-frame velocity of the precursor molecule. This technique, known as ‘Photostop’, leaves a fraction of the fragments with a narrow velocity distribution, centered around zero velocity in the lab-frame. They can be shown to have zero velocity by changing the time between photodissociation and ionisation; fragments with a high kinetic energy will leave the ionisation volume prior to interrogation. The underlying velocity distribu- tion is uncovered by using the velocity-map imaging technique, and the temperature of the fragments can be determined.The method was originally optimised for the molecular case. Cold NO has been produced from the dissociation of NO₂ molecules, and a single rotational state has been shown to remain in the ionisation volume 10 μs after dissociation, implying a sample temperature of 1.17 K. Using the optimised experimental conditions de- rived from the velocity cancellation of NO, the atomic case is demonstrated for the dissociation of Br₂ to give zero-velocity Br fragments. The Br atoms are seen for delay times in excess of 100 μs, showing the greater applicability of the method to the atomic case. The temperature of the residual atoms is shown to be in the milliKelvin regime, as determined through detailed Monte Carlo simulation of the motion of the stopped atoms. The possibility of trapping the ultracold Br atoms in a magnetic field is explored, and a quadrupolar trap created between two per- manent bar magnets is demonstrated to confine the atoms spatially, within the ion extraction optics, for delays in excess of 1 ms.The Photostop technique is intended to be a stepping stone on the way to widening the number of chemical species available for study in the ultracold regime. The possibility of improvements to the experiment is considered, in order to increase the efficiency of the experiment such that the number density becomes high enough to be viable as a source of atoms for use in cold chemical reactive studies. The possibility of extending the method so as to be used as a tunable velocity source of atoms is also discussed.