Metastable Neon Research Articles

Collisional alignment and molecular rotation control the chemi-ionization of individual conformers of hydroquinone with metastable neon.

The relationship between the shape of a molecule and its chemical reactivity is a central tenet in chemistry. However, the influence of the molecular geometry on reactivity can be subtle and result from several opposing effects. Here, using a crossed-molecular-beam experiment in which individual rotational quantum states of specific conformers of a molecule are separated, we study the chemi-ionization reaction of hydroquinone with metastable neon atoms. We show that collision-induced alignment of the reaction partners caused by geometry-dependent long-range forces influences reaction pathways, which is, however, countered by molecular rotation. The present work provides insights into the conformation-specific stereodynamics of complex polyatomic systems and illustrates the capability of advanced molecule-control techniques to unravel these effects.

Isomeric and rotational effects in the chemi-ionisation of 1,2-dibromoethene with metastable neon atoms.

The specific geometry of a molecule can have a pronounced influence on its chemical reactivity. However, experimental data on reactions of individual molecular isomers are still sparse because they are often difficult to separate and frequently interconvert into one another under ambient conditions. Here, we employ a novel crossed-beam experiment featuring an electrostatically controlled molecular beam combined with a source for radicals and metastables to spatially separate the cis and trans stereoisomers as well as individual rotational states of 1,2-dibromoethene and study their specific reactivities in the chemi-ionisation reaction with excited neon atoms. The experiments reveal pronounced isomeric and rotational specificities in the rates and product branching ratios of the reaction. The present study underlines the importance and combined role of molecular geometry and of rotational motion in the dynamics of chemi-ionisation reactions.

Observation of the p -wave shape resonance in atom-molecule collisions

Partial wave resonances are quasi-bound states that are formed by tunneling through the centrifugal barrier. Such states are important to collisions that deviate from the Langevin limit where direct collision path is suppressed due to quantum symmetry or a potential barrier. In such a case, quantum resonances play a major role in the dynamics at low temperatures where scattering process can be described mainly by the resonance contribution. Here we present the first observation of the lowest-lying partial wave resonance in the Penning ionization collisions between metastable neon and rovibrationally ground state HD molecules. We observe the resonance at an energy of $k_B\times$22mK taking advantage of the phase space correlation similar to atomic delta kick cooling. We show that the $p$-wave resonance position is particularly sensitive to the leading term of the van der Waals interaction. We also measure shape resonance at a higher angular momentum state, $l=6$, allowing us to disentangle and probe the short and the long parts of the intermolecular interaction.

A novel crossed-molecular-beam experiment for investigating reactions of state- and conformationally selected strong-field-seeking molecules

ABSTRACT The structure and quantum state of the reactants have a profound impact on the kinetics and dynamics of chemical reactions. Over the past years, significant advances have been achieved in the control and manipulation of molecules with external electric and magnetic fields in molecular-beam experiments for investigations of their state-, structure- and energy-specific chemical reactivity. Whereas studies for neutrals have so far mainly focused on weak-field-seeking species, we report here progress towards investigating reactions of strong-field-seeking molecules by introducing a novel crossed-molecular-beam experiment featuring an electrostatic deflector. The new setup enables the characterisation of state- and geometry-specific effects in reactions under single-collision conditions. As a proof of principle, we present results on the chemi-ionisation reaction of metastable neon atoms with rotationally state-selected carbonyl sulfide (OCS) molecules and show that the branching ratio between the Penning and dissociative ionisation pathways strongly depends on the initial rotational state of OCS.

Stereo-dynamical effects in chemi-ionization reactions of atmospheric O2 and N2 molecules promoted by collisions with Ne*(3P2,0) atoms

This letter focuses on general aspects of the stereodynamics of chemi-ionization reactions, triggered by collisions of O2 and N2 molecules with metastable neon atoms. Basic characteristics of the long-range intermolecular forces involved, some of chemical and others of physical origin, suggest that the weakly bound precursor state, determining the reaction transition state structure and stability, is rather different. Fundamental reaction selectivities are clarified, highlighting differences in the: i) optical potential whose real and imaginary parts must be interdependent; ii) polarizability, quadrupolar moments and orbital representation of the molecules involved, which allow to lay the foundations for future more in-depth investigations.

Measurement of pressure shift and broadening coefficients for Ne 3s[3/2]2→3p[5/2]3 transition in Ne and He using diode-laser absorption spectroscopy

Measurements of pressure broadening and shift coefficients for 640.2 nm Ne line were performed in an RF discharge without stabilization of neutral gas temperature. A diode laser with a short external cavity was used for metastable neon absorption spectroscopy in a natural mixture of neon isotopes. An appropriate fit function was constructed permitting deduction of Doppler and Lorentz components for the Voigt profile of the spectral line. To determine pressure broadening ξ and shift β coefficients for pure Ne and Ne:He mixture we used the information about Lorentz linewidth, position of the line center and gas temperature derived from spectral line shape fitted to a model line profile. The values of the collisional coefficients reduced to 300 K in units of 10-10 s-1 cm3, are ξNe-Ne = (1.9±0.2), ξNe-He = (3.4±0.2); βNe-Ne = -(0.7±0.1), βNe-He = (0.13±0.04).

Charge transfer from doubly charged ions of transition elements in a neon glow discharge: evidence based on emission spectra

An extensive study of Mn II, Fe II, Ti II, Cr II and Cu II emission spectra from a Grimm-type glow discharge in neon was performed, using the formalism of transition rate (TR) diagrams. In this method, radiative depopulation rates of individual excited levels of a species under study are established based on the emission spectrum, prospective contributions from radiative decay of higher excited levels (cascade excitation) are subtracted and the resulting net depopulation rates are plotted as function of energy of the levels involved. A peak at a particular energy in such a diagram reflects a collisional process in operation, selectively populating levels in a narrow interval around that energy. By comparing net TR diagrams of ionic spectra of the elements listed above, a common pattern was found indicating that singly charged ions of these elements are created, in addition to other mechanisms, by charge transfer between doubly charged ions of the element under study and metastable neutral neon atoms. This mechanism appears to be significant and needs to be taken into account in collisional–radiative models describing excitation and ionization of some elements in neon glow discharges.

Glow discharge excitation and ionization of chromium, comparison with iron

Cr I and Cr II emission spectra from a Grimm-type glow discharge (GD) in argon and neon were analyzed. Intensities of strong resonance Cr I lines were corrected for self-absorption and population functions (experimental Boltzmann plots) of the Cr I system were established. A prevailing excitation mechanism in Cr I is the electron impact (EI) excitation. Cr II spectra in both discharges were described by transition rate (TR) diagrams, under the model of radiatively-dominated deexcitation. The contribution of cascade excitation was subtracted and the resulting net-TR diagrams of Cr II were analyzed. Unlike ionic spectra of some other transition elements, asymmetric charge transfer (ACT) between the ions of the discharge gas and ground state Cr atoms does not play a role in the excitation of the Cr II spectrum, because of the absence of suitable states in Cr II that would allow simultaneous conservation of energy and total angular momentum. Cr II states below ≈17 eV are populated largely by EI excitation from long-lived low Cr II states. In a neon discharge, ACT reactions between neutral neon metastables and doubly charged Cr ions and between neutral chromium and neon molecular ions were identified. The findings reported here were compared with the excitation of Fe I and Fe II systems at similar conditions. A well-known ‘hydrogen effect’, an enhancement of the Cr II line at 267.7165 nm in the presence of hydrogen in a GD plasma, was explained by charge transfer reaction between H+ ions and neutral chromium.

Sub-Kelvin Stereodynamics of the Ne(^{3}P_{2})+N_{2} Reaction.

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 60mK. 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 0.06-700K. 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.

Imaging Recoil Ions from Optical Collisions between Ultracold, Metastable Neon Isotopes.

We present an experimental scheme that combines the well-established method of velocity-map imaging with a cold trapped metastable neon target. The device is used for obtaining the branching ratios and recoil-ion energy distributions for the penning ionization process in optical collisions of ultracold metastable neon. The potential depth of the highly excited dimer potential is extracted and compared with theoretical calculations. The simplicity to construct, characterize, and apply such a device makes it a unique tool for the low-energy nuclear physics community, enabling opportunities for precision measurements in nuclear decays of cold, trapped, short-lived radioactive isotopes.

Cold temperatures invert product ratios in Penning ionisation reactions with argon

In many chemical reactions with more than one possible outcome, the branching ratio, which is the ratio between the different reaction paths, is nearly constant over a wide range of collision energies. In barrierless systems governed by long-range interactions, however, the branching ratio is more sensitive to collision energy, and its dependence on it can be useful for better understanding the dynamics and reconstructing interaction potentials. Here we present the reaction rates of Penning and associative ionisation of metastable neon and helium with argon atoms. We obtain reaction rates in merge beam experiments, over a wide range of collision energies corresponding to that of room temperature, all the way down to a few millikelvins. We observe a change of two orders of magnitude in the branching ratio in the measured collision energy range and explain these changes using theoretical calculations.

Energy and orientation independence of the channel branching in Ne* + ND3 chemi-ionisation.

Collisions of excited neon atoms with ammonia molecules can lead to two reaction processes, dissociative ionisation and Penning ionisation. Both processes result in the ionisation of the ammonia molecule and redistribution of the electronic energy into the internal ammonia ion rovibrational modes. We performed energy dependent, crossed-beam stereodynamics studies of the branching ratio between the two ionisation processes. It was found that the branching ratio is totally and completely insensitive to both the neon orientation and the collision energy across the range we sampled, 370-520 cm-1. The total lack of stereodynamics can be explained by the structure of the ammonia and that its orientation, which we do not attempt to control, is the critical factor in the reaction outcome.

Positive column of a glow discharge in neon with charged dust grains (a review)

The effect of charged micron-size dust grains (microparticles) on the electric parameters of the positive column of a low-pressure dc glow discharge in neon has been studied experimentally and numerically. Numerical analysis is carried out in the diffusion-drift approximation with allowance for the interaction of dust grains with metastable neon atoms. In a discharge with a dust grain cloud, the longitudinal electric field increases. As the number density of dust grains in an axisymmetric cylindrical dust cloud rises, the growth of the electric field saturates. It is shown that the contribution of metastable atoms to ionization is higher in a discharge with dust grains, in spite of the quenching of metastable atoms on dust grains. The processes of charging of dust grains and the dust cloud are considered. As the number density of dust grains rises, their charge decreases, while the space charge of the dust cloud increases. The results obtained can be used in plasma technologies involving microparticles.

Communication: Neutral atom imaging using a pulsed electromagnetic lens.

We report on progress towards a neutral atom imaging device that will be used for chemically sensitive surface microscopy and nanofabrication. Our novel technique for improving refractive power and correcting chromatic aberration in atom lenses is based on a fundamental paradigm shift from continuous-beam focusing to a pulsed, three-dimensional approach. Simulations of this system suggest that it will pave the way toward the long-sought goal of true atom imaging on the nanoscale. Using a prototype lens with a supersonic beam of metastable neon, we have imaged complex patterns with lower distortion and higher resolution than has been shown in any previous experiment. Comparison with simulations corroborates the underlying theory and encourages further refinement of the process.

Measurement of the Ne transition isotope shift using a single, phase-modulated laser beam

We develop a simple technique to accurately measure frequency differences between far-lying resonances in a spectroscopy signal using a single, unlocked laser. This technique was used to measure the isotope shift (IS) of the cooling transition of metastable neon. Our result of 1626.287(53) MHz is the most accurate determination of this value to date.

Influence of dust particles on ionization and excitation in neon dc discharge

The influence of dust particles on the concentration of metastable neon atoms and ionization was investigated using the developed drift/diffusion model for plasma of positive column of glow discharge. The detailed de-excitation in neon was considered. In addition to usual plasma losses in dusty plasmas, the quenching of metastable atoms on dust particle surface was considered. The strong influence of dust particles on the ionization rate and concentration of metastable neon atoms in a positive column of glow discharge is shown to result from the change in the longitudinal electric field strength.

The interaction of ultrashort laser pulses and exotic atoms

SynopsisIn this work we present results for the ionization of metastable neon with ultrashort laser pulses. In addition to improving on the accuracy of previous measurements of ion yield, we show comparisons to advanced TDSE based theory. This work presents preliminary experimental evidence of the effects of preparing the target atoms into particular angular momentum projection (mj) states on the total ionization yield.

Characterization of a metastable neon beam extracted from a commercial RF ion source

We have used a commercial RF ion-source to extract a beam of metastable neon atoms. The source was easily incorporated into our existing system and was operative within a day of installation. The metastable velocity distribution, flux, flow, and efficiency were investigated for different RF powers and pressures, and an optimum was found at a flux density of 2 × 1012 atoms/s/sr. To obtain an accurate measurement of the amount of metastable atoms leaving the source, we insert a Faraday cup in the beam line and quench some of them using a weak 633 nm laser beam. In order to determine how much of the beam was quenched before reaching our detector, we devised a simple model for the quenching transition and investigated it for different laser powers. This detection method can be easily adapted to other noble gas atoms.

Two-dimensional positive column structure in a discharge tube with radius discontinuity

The low-pressure (40 and 90 Pa) low-current (4 and 10 mA) direct current discharge in a tube with a sharp change of its radius is studied both numerically and experimentally. A fully self-consistent hybrid numerical model of a two-dimensional non-uniform positive column in neon is developed using a nonlocal approach. The model combines kinetic simulation of the electrons (under two-terms approach) and fluid description of the neon ions and permits to calculate the distribution of all plasma parameters in the direct current discharges in the cameras with cylindrical geometry and radius discontinuity. The simulation results are compared with the measured 585.3 nm neon spectral line absolute intensities and excited 1s3 metastable neon atom number densities. Non-local electron kinetics in the transition region and formation of standing strata are discussed.

Effect of metastable neon atoms in a positive column of glow discharge with dust particles

The diffusion/drift model of the positive column of glow discharge in neon was used for the analysis of the role of neon metastable atoms in the interaction between neon plasma and dust particles. The radial profiles of electrons and metastable atoms were simulated in the typical range of neon pressure and discharge current where dust particles may form dense dust structures changing the plasma properties. The results showed the nonlocal effect of dust particles on the plasma composition. Within the dust structure, the metastable atom concentration was shown to be higher than in the discharge without dust particles at the same discharge parameters; the ratio of concentrations of metastable atoms and electrons may increase with increasing dust particle concentration in a certain range of discharge parameters. The partial contribution of metastable atoms to the ionization was found to be higher than their losses on the surface of dust particles and increased when the gas pressure was increased.