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The Journal of Physical Chemistry C

Sub-Kelvin Collision Temperatures in Merged Neutral Beams by Correlation in Phase-Space

Yuval Shagam, Edvardas Narevicius

Published Jul 29, 2013• 48 citations
Publisher

Abstract

Recent merged neutral beam experiments have introduced the possibility of measuring reactive collisions in the cold regime down to 10 mK. The lowest temperature attained in these experiments cannot be explained using the standard formalism developed for crossed molecular beam scattering. These low temperatures become accessible because pulsed supersonic beams develop a correlation in velocity-position space during free propagation such that the local velocity standard deviation decreases. This effect is responsible for a reduction in the attainable collision energy by more than 2 orders of magnitude along with an order of magnitude improvement in the resolution. We show that supersonic nozzles with short pulsed opening durations compared to the time-of-flight, such as the Even-Lavie valve, have a clear advantage in achieving low collision energies with improved resolution. We discuss possible improvements in the energy resolution by varying the detection time duration.

DOI
10.1021/jp4045868

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Recent merged neutral beam experiments have introduced the possibility of measuring reactive collisions in the cold regime down to 10 mK. The lowest temperature attained in these experiments cannot be explained using the standard formalism developed for crossed molecular beam scattering. These low temperatures become accessible because pulsed supersonic beams develop a correlation in velocity-position space during free propagation such that the local velocity standard deviation decreases. This effect is responsible for a reduction in the attainable collision energy by more than 2 orders of magnitude along with an order of magnitude improvement in the resolution. We show that supersonic nozzles with short pulsed opening durations compared to the time-of-flight, such as the Even-Lavie valve, have a clear advantage in achieving low collision energies with improved resolution. We discuss possible improvements in the energy resolution by varying the detection time duration.
We have developed an experiment for the investigation of neutral molecular collisions in the gas phase at temperatures as low as 100 mK. These low temperatures are obtained by merging two supersonic expansions, using an electric and a magnetic guide, and by matching the velocities of the beams. Since the energy available for the collisions, or the temperature, is determined only by the relative velocity of the reaction partners this enables the study of chemical processes at very low temperatures without the need to prepare slow molecules in the laboratory frame of reference. This paper describes the method and presents results on the Ne((3)P2)+NH3 Penning ionization.
We present two methods for studying reactive collisions between two atomic or molecular species: a collinear merged-beam method in which two gas pulses from a single supersonic beam source are coalesced and an intrabeam-scattering technique in which a single gas pulse is used. Both approaches, which rely on the laser cooling and deceleration of a laser-coolable species inside a Zeeman slower, can be used for a wide range of scattering studies. Possible experimental implementations of the proposed methods are outlined for autoionizing collisions between helium atoms in the metastable 2 3 S 1 state and a second, atomic or molecular species. Using numerical trajectory calculations, we provide estimates of the expected on-axis detection efficiency, collision-energy range, and collision-energy resolution of the approaches. We have experimentally tested the feasibility of such an experiment by producing two gas pulses at very short time intervals, and the results of these measurements are also detailed.
Within this thesis two experiments will be described. In the first experiment a velocity filter was used to obtain a beam of polar molecules (ND3) with a translational temperature of less than 5K. For the first time the dynamics of individual rotational states inside a velocity filter could be investigated directly. Usually a velocity filter defines only a maximumvelocity that can pass the filter. We successfully implemented two different approaches where molecules below a certain minimal velocity are removed from the beam, turning the velocity filter into a bandpass filter. The second and more interesting experiment is the merged beamexperiment. We developed and constructed the first apparatus which successfullymerged two guided beams, one consisting of polar molecules, the other of paramagnetic particles, into an overlapping parallel movement. With this approach we could lower the temperature at which the reaction of metastable Ne* with ND3, NH3 and CH3F has been investigated by 3 orders of magnitude down to the sub-kelvin regime. Especially the stereochemistry of those reactions revealed an unexpected energy-insensitivity at temperatures below 200K. As our setup is very general the investigation of manymore neutral-neutral reactions will be possible, opening a new route into an temperature regime where only a few reactions have been studied before.
Molecular collisions can be studied at very low relative kinetic energies, in the milliKelvin range, by merging codirectional beams with much higher translational energies, extending even to the kiloKelvin range, provided that the beam speeds can be closely matched. This technique provides far more intensity and wider chemical scope than methods that require slowing both collision partners. Previously, at far higher energies, merged beams have been widely used with ions and/or neutrals formed by charge transfer. Here, we assess for neutral, thermal molecular beams the range and resolution of collision energy that now appears attainable, determined chiefly by velocity spreads within the merged beams. Our treatment deals both with velocity distributions familiar for molecular beams formed by effusion or supersonic expansion, and an unorthodox variant produced by a rotating supersonic source capable of scanning the lab beam velocity over a wide range.
Experiments have lagged theory in exploring chemical interactions at temperatures so low that translational degrees of freedom can no longer be treated classically. The difficulty has been to realize in the laboratory low-enough collisional velocities between neutral reactants to access this regime. We report here the realization of merged neutral supersonic beams and the manifestation of clear nonclassical effects in the resulting reactions. We observed orbiting resonances in the Penning ionization reaction of argon and molecular hydrogen with metastable helium, leading to a sharp absolute ionization rate increase in the energy range corresponding to a few degrees kelvin down to 10 millikelvin. Our method should be widely applicable to many canonical chemical reactions.
We review the experimental findings on scattering resonances in molecular collisions occurring in the energy domain equivalent to temperatures of a few Kelvin. We discuss the conditions required to observe shape (or orbiting) and Feshbach resonances, the crucial factor being in all cases the number of partial waves involved in the process. This implies operating with supersonic beams with matched and low velocities, high velocity resolution and low beam-intersection angle. This is exemplified for elastic, inelastic and reactive collisions, where different strategies, thence experimental arrangements, are used. We review the first observation of resonances in elastic collisions from the 1970s and the recent results in inelastic and reactive collisions. The most striking result is obtained for O2 + para-H2 inelastic collisions for which rotational excitation occurs through a pure quantum process, yielding a well-resolved structure in the integral cross section assigned to definite well-separated partial waves.