Electron density and temperature measurements in a magnetized expanding hydrogen plasma.

We report measurements of electron densities, n_{e}, and temperatures, T_{e}, in a magnetized expanding hydrogen plasma performed using Thomson scattering. The effects of applying an axial magnetic field and changing the background pressure in the plasma vessel on n_{e} and T_{e} along the expansion axis are reported. Magnetic field strengths (B field) up to 170 mT were applied, which are one order of magnitude larger than previously reported. The main effect of the applied B field is the plasma confinement, which leads to higher n_{e}. At B fields larger than 88 mT the electron density along the expansion axis does not depend strongly on the magnetic field strength. However, T_{e} is susceptible to the B field and reaches at 170 mT a maximum of 2.5 eV at a distance of 1.5 cm from the exit of the cascaded arc. To determine also the effect of the arc current through the arc, measurements were performed with arc currents of 45, 60, and 75 A at background pressures of 9.7 and 88.3 Pa. At constant magnetic field n_{e} decreases from the exit of the arc along the expansion axis when the arc current is decreased. At 88.3 Pa n_{e} shows a higher value close to the exit of the arc, but a faster decay along the expansion axis with respect to the 9.7 Pa case. T_{e} is overall higher at lower pressure reaching a maximum of 3.2 eV at the lower arc current of 45 A. The results of this study complement our understanding and the characterization of expanding hydrogen plasmas.

Taming microwave plasma to beat thermodynamics in CO2 dissociation.

The strong non-equilibrium conditions provided by the plasma phase offer the opportunity to beat traditional thermal process energy efficiencies via preferential excitation of molecular vibrations. Simple molecular physics considerations are presented to explain potential dissociation pathways in plasma and their effect on energy efficiency. A common microwave reactor approach is evaluated experimentally with Rayleigh scattering and Fourier transform infrared spectroscopy to assess gas temperatures (exceeding 10(4) K) and conversion degrees (up to 30%), respectively. The results are interpreted on a basis of estimates of the plasma dynamics obtained with electron energy distribution functions calculated with a Boltzmann solver. It indicates that the intrinsic electron energies are higher than is favorable for preferential vibrational excitation due to dissociative excitation, which causes thermodynamic equilibrium chemistry to dominate. The highest observed energy efficiencies of 45% indicate that non-equilibrium dynamics had been at play. A novel approach involving additives of low ionization potential to tailor the electron energies to the vibrational excitation regime is proposed.

Note: Rotational Raman scattering on CO2 plasma using a volume Bragg grating as a notch filter.

We present a novel approach for filtering Rayleigh scattering and stray light from Raman scattering in a gas discharge, using a volume Bragg grating as a notch filter. For low frequency rotational Raman contributions, it is essential to filter out Rayleigh scattering and stray light at the laser wavelength to be able to measure an undisturbed Raman spectrum. Using the Bragg grating, having an optical density of 3.1 at the central wavelength of 532 nm and a full width at half maximum of 7 cm(-1), we were able to measure a nearly full rotational CO2 spectrum (1.56 cm(-1) peak-to-peak separation). The rotational temperature in a CO2 discharge was determined with an accuracy of 2%.

Population inversion in a magnetized hydrogen plasma expansion as a consequence of the molecular mutual neutralization process.

A weakly magnetized expanding hydrogen plasma, created by a cascaded arc, was investigated using optical emission spectroscopy. The emission of the expanding plasma is dominated by H{α} emission in the first part of the plasma expansion, after which a sharp transition to a blue afterglow is observed. The position of this sharp transition along the expansion axis depends on the magnetic field strength. The blue afterglow emission is associated with population inversion of the electronically excited atomic hydrogen states n=4-6 with respect to n=3. By comparing the measured densities with the densities using an atomic collisional radiative model, we conclude that atomic recombination processes cannot account for the large population densities observed. Therefore, molecular processes must be important for the formation of excited states and for the occurrence of population inversion. This is further corroborated at the transition from red to blue, where a hollow profile of the excited states n=4-6 in the radial direction is observed. This hollow profile is explained by the molecular mutual neutralization process of H2+ with H⁻, which has a maximum production for excited atomic hydrogen 1-2 cm outside the plasma center.

Nonequilibrium rovibrational energy distributions of hydrogen isotopologues in an expanding plasma jet.

State resolved densities of high rovibrationally excited hydrogen isotopologues H(2), HD, and D(2) in the electronic ground state have been measured in a supersonically expanding plasma jet. The obtained state distributions differ substantially from thermal equilibrium. Moreover, the distributions are not the same for H(2), HD, and D(2) indicating different formation and relaxation rates for each isotopologue. Mechanisms for this deviation from a Boltzmann distribution are given and compared to hydrogen reactions in other environments. The difference between the measured highest occupied rovibrational states in H(2), HD, and D(2) is ascribed to an isotope effect in the dissociation process.

Formation and relaxation of rovibrationally excited H2 molecules due to plasma-surface interaction.

We report on the interaction of hydrogen atoms and molecules under high flux conditions with a cooled copper surface and its impact on gas phase densities and internal excitation of the molecules. These densities were measured by means of laser-induced fluorescence using tunable radiation sources in the vacuum-ultraviolet (vuv). While H atoms were detected by two-photon absorption laser-induced fluorescence, the necessary vuv radiation for the detection of rovibrationally excited H2 molecules in the electronic ground state were produced by stimulated anti-Stokes Raman scattering. The results reveal a strong loss mechanism of H atoms and the formation of rovibrationally excited H2 molecules due to surface interaction. The surface reaction probability of H atoms under high flux conditions on copper was estimated. Surface collisions are shown to have a profound influence on the density distribution of rovibrationally excited H2 molecules: The distributions follow lower temperatures and are less Boltzmann-like, i.e., the distributions of the internal excitation of H2 molecules differ more from thermodynamic equilibrium.

Influence of rarefaction on the flow dynamics of a stationary supersonic hot-gas expansion.

The gas dynamics of a stationary hot-gas jet supersonically expanding into a low pressure environment is studied through numerical simulations. A hybrid coupled continuum-molecular approach is used to model the flow field. Due to the low pressure and high thermodynamic gradients, continuum mechanics results are doubtful, while, because of its excessive time expenses, a full molecular method is not feasible. The results of the hybrid coupled continuum-molecular approach proposed have been successfully validated against experimental data by R. Engeln [Plasma Sources Sci. Technol. 10, 595 (2001)] obtained by means of laser induced fluorescence. Two main questions are addressed: the necessity of applying a molecular approach where rarefaction effects are present in order to correctly model the flow and the demonstration of an invasion of the supersonic part of the flow by background particles. A comparison between the hybrid method and full continuum simulations demonstrates the inadequacy of the latter, due to the influence of rarefaction effects on both velocity and temperature fields. An analysis of the particle velocity distribution in the expansion-shock region shows clear departure from thermodynamic equilibrium and confirms the invasion of the supersonic part of the flow by background particles. A study made through particles and collisions tracking in the supersonic region further proves the presence of background particles in this region and explains how they cause thermodynamic nonequilibrium by colliding and interacting with the local particles.

High sensitivity imaging Thomson scattering for low temperature plasma.

A highly sensitive imaging Thomson scattering system was developed for low temperature (0.1-10 eV) plasma applications at the Pilot-PSI linear plasma generator. The essential parts of the diagnostic are a neodymium doped yttrium aluminum garnet laser operating at the second harmonic (532 nm), a laser beam line with a unique stray light suppression system and a detection branch consisting of a Littrow spectrometer equipped with an efficient detector based on a "Generation III" image intensifier combined with an intensified charged coupled device camera. The system is capable of measuring electron density and temperature profiles of a plasma column of 30 mm in diameter with a spatial resolution of 0.6 mm and an observational error of 3% in the electron density (n(e)) and 6% in the electron temperature (T(e)) at n(e) = 4 x 10(19) m(-3). This is achievable at an accumulated laser input energy of 11 J (from 30 laser pulses at 10 Hz repetition frequency). The stray light contribution is below 9 x 10(17) m(-3) in electron density equivalents by the application of a unique stray light suppression system. The amount of laser energy that is required for a n(e) and T(e) measurement is 7 x 10(20)n(e) J, which means that single shot measurements are possible for n(e)>2 x 10(21) m(-3).

Production mechanisms of NH and NH2 radicals in N2-H2 plasmas.

We measured the densities of NH and NH(2) radicals by cavity ring-down spectroscopy in N(2)-H(2) plasmas expanding from a remote thermal plasma source and in N(2) plasmas to which H(2) was added in the background. The NH radical was observed via transitions in the (0,0), (1,1), and (2,2) vibrational bands of the A(3)Pi <-- X(3)Sigma- electronic transition and the NH(2) radical via transitions in the (0,9,0) <-- (0,0,0) band of the A(2)A(1) <-- X(2)B(1) electronic transition. The measurements revealed typical densities of 5 x 10(18) m(-3) for the NH radical in both plasmas and up to 7 x 10(18) m(-3) for the NH(2) radical when N(2) and H(2) are both fed through the plasma source. In N(2) plasma with H(2) injected in the background, no NH(2) was detected, indicating that the density is below our detection limit of 3 x 1016 m-3. The error in the measured densities is estimated to be around 20%. From the trends of the NH(x) radicals as a function of the relative H(2) flow to the total N(2) and H(2) flow at several positions in the expanding plasma beam, the key reactions for the formation of NH and NH(2) have been determined. The NH radicals are mainly produced via the reaction of N atoms emitted by the plasma source with H(2) molecules with a minor contribution from the reaction of N+ with H(2). The NH(2) radicals are formed by reactions of NH(3) molecules, produced at the walls of the plasma reactor, and H atoms emitted by the plasma source. The NH radicals can also be produced by H abstraction of NH(2) radicals. The flux densities of the NH(x) radicals with respect to the atomic radicals are appreciable in the first part of the expansion. Further downstream the NH(x) radicals are dissociated, and their densities become smaller than those of the atomic radicals. It is concluded that the NH(x) radicals play an important role as precursors for the N and H atoms, which are key to the surface production of N(2), H(2), and NH(3) molecules.

Relaxation behavior of rovibrationally excited H2 in a rarefied expansion.

The evolution of the rotational and vibrational distributions of molecular hydrogen in a hydrogen plasma expansion is measured using laser induced fluorescence in the vacuum-UV range. The evolution of the distributions along the expansion axis shows the relaxation of the molecular hydrogen from the high temperature in the upstream region to the low ambient temperature in the downstream region. During the relaxation, the vibrational distribution, which has been recorded up to v = 6, is almost frozen in the expansion and resembles a Boltzmann distribution at T approximately 2200 K. However, the rotational distributions, which have been recorded up to J = 17 in v = 2 and up to J = 11 in v = 3, cannot be described with a single Boltzmann distribution. In the course of the expansion, the lower rotational levels (J < 5) adapt quickly to the ambient temperature ( approximately 500 K), while the distribution of the higher rotational levels (J > 7) is measured to be frozen in the expansion at a temperature between 2000 and 2500 K. A model based on rotation-translation energy transfer is used to describe the evolution of the rotational distribution of vibrational level v = 2 in the plasma expansion. The behavior of the low rotational levels (J < 5) is described satisfactory. However, the densities of the higher rotational levels decay faster than predicted.

Behavior of the H atom velocity distribution function within the shock wave of a hydrogen plasma jet.

The evolution of the ground-state hydrogen atom velocity distribution function throughout the stationary shock wave of a supersonic hydrogen plasma jet (3

Transport of ground-state hydrogen atoms in a plasma expansion.

The transport of ground-state atomic hydrogen in the expansion of a thermal plasma generated from an Ar-H2 mixture is studied by means of laser-based diagnostic techniques. The flow of hydrogen atoms is investigated by two-photon excitation laser-induced fluorescence (LIF), whereas Ar atoms are probed by LIF as well as by UV Rayleigh scattering. The transport of Ar atoms can be fully understood in terms of a free jet flow; H atoms on the contrary exhibit an anomalous behavior. In the course of the plasma expansion, hydrogen atoms decouple from the argon fluid by a diffusion process as a direct consequence of recombination of H atoms at the vessel walls. In this contribution it is shown, on the basis of experimental results, how plasma-surface interactions can strongly influence the flow pattern of an atomic radical fluid.