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The Journal of Chemical Physics

Ultra-precise particle velocities in pulsed supersonic beams

Wolfgang Christen

Published Jul 8, 2013• 6 citations
Publisher

Abstract

We describe an improved experimental method for the generation of cold, directed particle bunches, and the highly accurate determination of their velocities in a pulsed supersonic beam, allowing for high-resolution experiments of atoms, molecules, and clusters. It is characterized by a pulsed high pressure jet source with high brilliance and optimum repeatability, a flight distance of few metres that can be varied with a tolerance of setting of 50 μm, and a precision in the mean flight time of particles of better than 10(-4). The technique achieves unmatched accuracies in particle velocities and kinetic energies and also permits the reliable determination of enthalpy changes with very high precision.

DOI
10.1063/1.4812371

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We describe an improved experimental method for the generation of cold, directed particle bunches, and the highly accurate determination of their velocities in a pulsed supersonic beam, allowing for high-resolution experiments of atoms, molecules, and clusters. It is characterized by a pulsed high pressure jet source with high brilliance and optimum repeatability, a flight distance of few metres that can be varied with a tolerance of setting of 50 μm, and a precision in the mean flight time of particles of better than 10(-4). The technique achieves unmatched accuracies in particle velocities and kinetic energies and also permits the reliable determination of enthalpy changes with very high precision.
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We describe modifications of a pulsed rotating supersonic beam source that improve performance, particularly increasing the beam density and sharpening the pulse profiles. As well as providing the familiar virtues of a supersonic molecular beam (high intensity, narrowed velocity distribution, and drastic cooling of rotation and vibration), the rotating source enables scanning the translational velocity over a wide range. Thereby, beams of any atom or molecule available as a gas can be slowed or speeded. Using Xe beams in the slowing mode, we have obtained lab speeds down to about 40 ± 5 m/s with density near 10(11) cm(-3) and in the speeding mode lab speeds up to about 660 m/s and density near 10(14) cm(-3). We discuss some congenial applications. Providing low lab speeds can markedly enhance experiments using electric or magnetic fields to deflect, steer, or further slow polar or paramagnetic molecules. The capability to scan molecular speeds facilitates merging velocities with a codirectional partner beam, enabling study of collisions at very low relative kinetic energies, without requiring either beam to be slow.
The mathematical term for the mean flow velocity in supersonic beams of ideal gases is extended to include real gas properties. This procedure yields an explicit dependence of the flow velocity on pressure, as observed in recent experiments of free jet expansions. Applied to stagnation conditions slightly above the critical point, the model suggests that seeded high-pressure jet expansions might be suitable for slowing down virtually any molecule with maximum efficiency. Moreover, we discuss the consequence of a pressure-dependent flow velocity v0{v}_{0}v0​ for the speed ratio $S={v}_{0}/\ensuremath{\Delta}{v}_{\ensuremath{\parallel}}$ with respect to collisional cooling and suggest to use the velocity spread $\ensuremath{\Delta}{v}_{\ensuremath{\parallel}}$ as a more nonambiguous measure of translational temperature in high-pressure jet expansions.
Describes the construction and characterisation of a pulsed, superthermal molecular beam source incorporating a rotor accelerator and a synchronously pulsed electron bombarder. The addition of the pulsed bombarder greatly improves the kinetic energy resolution of the superthermal metastable atomic and molecular beams, particularly for light particles at low velocities and eliminates problems of 'wrap-around' at low velocities. The optimum conditions of resolution at a desired signal level are discussed: a typical velocity distribution for Ar( 3 P 2 ) at a most probable beam velocity of 1500 m s -1 would have a standard deviation sigma approximately=0.07.
In this thesis I describe the second generation of a rotating supersonic beam source. The purpose of this device is to produce velocity augmented molecular beams for use with scattering experiments or subsequent slowing methods. The beam emerges from a nozzle inserted at the tip of a hollow aluminum rotor which can be spun at high speeds in either the forward or backwards direction. The forward direction mode increases the laboratory frame velocity distribution of the emitted beam and the backward direction mode decreases this velocity distribution.\n\nBoth rotor modes are analyzed theoretically and experimentally within the text. I introduce a pulsed gas inlet system for the rotating source as well as cryocooling of the vacuum chamber. This new version provides moderately intense beams of slow molecules, containing ∼1012 molecules at lab speeds as low as 35 m/s, and very intense beams of fast molecules, containing ∼1015 molecules at 400 m/s. Beams of any molecule available in gas phase can be produced utilizing this system. For collision experiments, the ability to scan the velocity utilizing the rotating source is very advantageous when using two merged beams. If the two velocities can be closely matched, very low relative collision energies can be produced without making either beam slow.