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Physical Review Letters

Sub-Kelvin Stereodynamics of the Ne(P32)+N2 Reaction

Junwen Zou, Sean D. S. Gordon, Andreas Osterwalder

Published Sep 23, 2019• 29 citations
Publisher

Abstract

We present an experimental study of the low-energy stereodynamics of the Ne(^{3}P_{2})+N_{2} reaction. Supersonic expansions of the two reactants are superposed in a merged beam experiment, where individual velocity control of the two beams allows us to reach average relative velocities of zero, yielding minimum collision energies around 60 mK. We combine the merged beam technique with the orientation of the metastable neon atoms and measure the branching between two reaction channels, Penning ionization and associative ionization, as a function of neon orientation and collision energy, covering the range 0.06-700 K. We find that we lose the ability to orient Ne below ≈100 K due to dynamic reorientation. Associative ionization products Ne-N_{2}^{+} predissociate with a probability of 30%-60% and that associative ionization is entirely due to reactions of the Ω=2 state, where the singly occupied p orbital of the Ne^{*} is oriented along the interatomic axis.

DOI
10.1103/physrevlett.123.133401

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We present an experimental study of the low-energy stereodynamics of the Ne(^{3}P_{2})+N_{2} reaction. Supersonic expansions of the two reactants are superposed in a merged beam experiment, where individual velocity control of the two beams allows us to reach average relative velocities of zero, yielding minimum collision energies around 60 mK. We combine the merged beam technique with the orientation of the metastable neon atoms and measure the branching between two reaction channels, Penning ionization and associative ionization, as a function of neon orientation and collision energy, covering the range 0.06-700 K. We find that we lose the ability to orient Ne below ≈100 K due to dynamic reorientation. Associative ionization products Ne-N_{2}^{+} predissociate with a probability of 30%-60% and that associative ionization is entirely due to reactions of the Ω=2 state, where the singly occupied p orbital of the Ne^{*} is oriented along the interatomic axis.
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.
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.
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.
This thesis presents investigations into the collision dynamics of cold metastable neon atoms in a magneto-optical trap (MOT). At very cold temperatures (approx. 1 mK) the atomic interaction occurs at long range and cannot be treated classically as the interaction between two nuclear point particles. In addition, the collision dynamics can be considerably altered in the presence of an optical eld. In this thesis results are presented for collisions that are altered by the presence of an optical eld and also collisions where the optical eld can be neglected. Controlled optical collisions of cold, metastable Ne atoms are performed by using a control laser tuned close to the (3s)3P2 to (3p)3D3 cooling transition. The control laser modies the rate of ionizing collisions by promoting a pair of colliding atoms onto an excited state potential. In order to induce collisions between pairs of trapped metastables, a control laser is tuned to the red of the transition where we measure a factor of 4 increase in the rate for ionizing collisions. We also investigate the eect of optical shielding by tuning the laser to the blue of the transition and observe a factor of 5 suppression in the ionization rate. However, the measured ionization spectrum does not contain resonances due to the formation of photoassociated molecules as predicted by Doery et al [1]. Instead, we observe a broad unresolvable ionization spectrum that is well described by established theory [2]. Collision cross sections are measured for neon in the (3s)3P2 metastable state with ground state, thermal atoms and molecules. The technique is based on the measurement of the loss rate due to collisions with a background gas. Generally, these type of collisions are considered undesirable, however, it is possible to infer information about the collision cross section if the rate of collisions is accurately known. This novel technique is described and collision cross section measurements are presented for metastable neon in the (3s)3P2 state with He, Ne, Ar, H2, O2, and N2. The average thermal energy of the collision ranges from 11 meV to 27 meV and the measurements have relatively small errors, of the order of 10%.
We have developed a ``beam brightener'' in which several different laser cooling methods produce a highly monochromatic, unidirectional and intense beam of metastable Ne(3s;^3P_2) atoms. The beam brightener consists of four main stages. From an exited neon source we capture in a collimating section 5× 10^11 Ne(3s)/s from which ≈ 50 % is slowed to 100 m/s in a Zeeman slower. The final velocity distribution shows a width of 3.3 m/s uc(RMS,) corresponding to a temperature of 12 mK. A fraction of ≈ 25 % of these cold atoms is captured by a magneto-optic compressor and molded into a 0.7 mm uc(FWHM) wide atomic beam that contains up to 5× 10^10 Ne(3s)/s. The resulting density is 1.1× 10^9 Ne(3s)/cm^3. In the final step, a Doppler cooler is used to minimize the divergence of the beam to 10 mrad. This value will further improve once the Doppler cooler is replaced by a sub-Doppler cooler. We plan to use this ``bright beam'' to investigate the ionization probabilities in Ne(3s)+Ne(3s) collisions. Emphasis will be on the suppression of ionization when the atoms are spin-polarized. This has important implications for the possibilities of using metastable atoms for BEC-type experiments. Present adress: NIST
Penning ionization reactions in merged beams with precisely controlled collision energies have been shown to accurately probe quantum mechanical effects in reactive collisions. A complete microscopic understanding of the reaction is, however, faced with two major challenges-the highly excited character of the reaction's entrance channel and the limited precision of even the best state-of-the-art ab initio potential energy surfaces. Here, we suggest photoassociation spectroscopy as a tool to identify the character of orbiting resonances in the entrance channel and probe the ionization width as a function of interparticle separation. We introduce the basic concept, using the example of metastable helium and argon, and discuss the general conditions under which this type of spectroscopy will be successful.