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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.
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Plasma probe manipulators, electromagnetic shielding, receiver signal to noise ratio, and plasma parameters for experiment and measurements on plasma properties
Chemical kinetics of electron plasma reactions, discussing energy states, ion-molecule reactions, charge transfer, transport properties, phase interactions, etc
The dissociative recombination of vibrationally excited O2(+) ions is studied in light of the possible importance of this reaction in upper atmospheric chemistry. A plasma spectroscopy experiment was performed in a microwave cavity filled by an argon-oxygen mixture, with O(1S) production monitored by measurements of the 5577-A afterglow, the O2(+) density and the electron concentration. Plasma and optical data reveal the predominant afterglow ions to be Ar2(+) and O2(+), with an effective O(1S) dissociative recombination coefficient of 2.1 x 10 to the -8th cu cm/sec, corresponding to a quantum yield of 10%. Experiments with an argon-krypton-oxygen mixture reveal that vibrationally excited O2(+) ions are the chief source of the O(1S) atoms, with a specific recombination coefficient for the dissociation of O2(+)(2 pi g) into O(1S) and O(1D) of 4.2 x 10 to the -9th cu cm/sec. A comparison of the laboratory results with Atmospheric Explorer data on the 5577-A airglow implies that O2(+) ions in the sunlit ionosphere are vibrationally excited to the same degree as in the laboratory, with the vibrational relaxation of these ions much slower than dissociative recombination. Results also predict a dawn-twilight asymmetry in the effective O(1S) yield due to the normal variation of electron content.
Multi-fluid modelling of the outflowing gases which sublimate from cometary nuclei as they approach the Sun is necessary for understanding the important physical and chemical processes occurring in this complex plasma. Coma chemistry models can be employed to interpret observational data and to ultimately determine chemical composition and structure of the nuclear ices and dust. We describe a combined chemical and hydrodynamical model [1] in which differential equations for the chemical abundances and the energy balance are solved as a function of distance from the cometary nucleus. The presence of negative ions (anions) in cometary comae is known from Giotto mass spectrometry of 1P/Halley. The anions O(-), OH(-), C(-), CH(-) and CN(-) have been detected, as well as unidentified anions with masses 22-65 and 85-110 amu [2]. Organic molecular anions such as C4H(-) and C6H(-) are known to have a significant impact on the charge balance of interstellar clouds and circumstellar envelopes and have been shown to act as catalysts for the gas-phase synthesis of larger hydrocarbon molecules in the ISM, but their importance in cometary comae has not yet been fully explored. We present details of new models for the chemistry of cometary comae that include atomic and molecular anions and calculate the impact of these anions on the coma physics and chemistry af the coma.
Titan's atmosphere, composed mainly of N2 and CH4, is the siege of a complex chemistry induced by solar UV radiation and electron bombardment from Saturn's magnetosphere. This organic chemistry occurs at temperatures lower than 200 K and leads to the production of heavy molecules and subsequently solid aerosols that form the orange haze surrounding Titan. The Titan Haze Simulation (THS) experiment has been developed on the COSMIC simulation chamber at NASA Ames in order to study the different steps of Titan's atmospheric chemistry at low temperature and to provide laboratory data in support for Cassini data analysis. The chemistry is simulated by plasma in the stream of a supersonic expansion. With this unique design, the gas mixture is adiabatically cooled to Titan-like temperature (approx. 150 K) before inducing the chemistry by plasma discharge. Different gas mixtures containing N2, CH4, and the first products of the N2,-CH4 chemistry (C2H2, C2H4, C6H6...) but also heavier molecules such as PAHs or nitrogen containing PAHs can be injected. Both the gas phase and solid phase products resulting from the plasma-induced chemistry can be monitored and analyzed. Here we present the results of recent gas phase and solid phase studies that highlight the chemical growth evolution when injecting heavier hydrocarbon trace elements in the initial N2-CH4 mixture. Due to the short residence time of the gas in the plasma discharge, only the first steps of the chemistry have time to occur in a N2-CH4 discharge. However by adding acetylene and benzene to the initial N2-CH4 mixture, we can study the intermediate steps of Titan's atmospheric chemistry as well as specific chemical pathways. These results show the uniqueness of the THS experiment to help understand the first and intermediate steps of Titan fs atmospheric chemistry as well as specific chemical pathways leading to Titan fs haze formation.
Here, we report measurements of time-resolved Ta, TaO and TaN emission spectroscopic signatures from a laser-produced plasma. Plasmas were generated using 1064 nm, 6 ns pulses from an Nd:YAG laser focused onto a pure Ta metal target in a gaseous environment with varying percentages of O 2 /N 2 for controlling gas-phase oxidation/plasma chemistry. Time-resolved analysis showed that Ta oxide emission is prominent at later times in plasma evolution, whereas strong atomic emission is present at early times in air. Emission spectral features as a function of O 2 partial pressure showed that TaO emission intensity increases, while the peak intensity of TaO appears earlier with increasing O 2 availability. We also report emission spectra of TaN, and show that plasma chemistry favors TaO formation instead of TaN when O 2 is present in the environment.
Many applications involving plasma–liquid interactions depend on the reactive processes occurring at the plasma–liquid interface. In this article, we report on a falling liquid film plasma reactor allowing for in situ optical absorption measurements of the time-dependence of the ferricyanide/ferrocyanide redox reactivity, complemented with ex situ measurement of the decomposition of formate. We found excellent agreement between the measured decomposition percentages and the diffusion-limited decomposition of formate by interfacial plasma-enabled reactions, except at high pH in thin liquid films, indicating the involvement of previously unexplored plasma-induced liquid phase chemistry enabled by long-lived reactive species. We also determined that high pH facilitates a reduction-favoring environment in ferricyanide/ferrocyanide redox solutions. In situ conversion measurements of a 1:1 ferricyanide/ferrocyanide redox mixture exceed the measured ex situ conversion and show that conversion of a 1:1 ferricyanide/ferrocyanide mixture is strongly dependent on film thickness. We identified three dominant processes: reduction faster than ms time scales for film thicknesses >100 µm, •OH-driven oxidation on time scales of <10 ms, and reduction on 15 ms time scales for film thickness <100 µm. We attribute the slow reduction and larger formate decomposition at high pH to HO$^−_2$ formed from plasma-produced H 2 O 2 enabled by the high pH at the plasma–liquid interface as confirmed experimentally and by computed reaction rates of HO$^−_2$ with ferricyanide. Overall, this work demonstrates the utility of liquid film reactors in enabling the discovery of new plasma-interfacial chemistry and the utility of atmospheric plasmas for electrodeless electrochemistry.
Here, we demonstrate that ambient pressure x-ray photoelectron spectroscopy (APXPS) can be used for in situ studies of dynamic changes in surface chemistry in a plasma environment. This opens a new and vast application space for XPS and greatly complements modern spectroscopy techniques to probe plasma-solid/liquid interactions relevant to process monitoring in the semiconductor industry, bio-medical plasma applications and plasma remediation technologies. Hexagonal boron nitride (h-BN) grown on Cu was used in this study as a well-defined model system for plasma process monitoring and because of its unique chemical, optical and electrical properties that make it a prospective material for advanced electronics. To better understand the stability and surface chemistry of h-BN during plasma assisted processing, we track in real time the plasma-induced chemical state changes of B, N and the underlying Cu substrate using APXPS equipped with an AC discharge plasma source operating at 13 Pa. Residual gas analysis (RGA) mass-spectra were concurrently collected during plasma-XPS to track reaction products formed during plasma exposure. A clear reduction of Cu x O is seen, while an h-BN layer remains intact, suggesting hydrogen radical (H • ) species can attack the exposed and h-BN covered Cu oxide patches and partially reduce the underlying substrate without significantly damaging the overlaying h-BN, which is of practical importance for development of h-BN encapsulated devices and interfaces. In addition to demonstration of plasma-XPS capabilities we discuss the observed challenges (e.g., parasitic plasma-chamber walls reactions and charging effects) and propose potential solutions.
The ignition of plasmas in liquids has applications from medical instrumentation to manipulation of liquid chemistry. Formation of plasmas directly in a liquid often requires prohibitively large voltages to initiate breakdown. Producing plasma streamers in bubbles submerged in a liquid with higher permittivity can significantly lower the voltage needed to initiate a discharge by reducing the electric field required to produce breakdown. The proximity of the bubble to the electrodes and the shape of the bubbles play critical roles in the manner in which the plasma is produced in, and propagates through, the bubble. In this paper, we discuss results from a three-dimensional direct numerical simulation (DNS) used to investigate the shapes of bubbles formed by injection of air into water. Comparisons are made to results from a companion experiment. A two-dimensional plasma hydrodynamics model was then used to capture the plasma streamer propagation in the bubble using a static bubble geometry generated by the DNS The simulations showed two different modes for streamer formation depending on the bubble shape. In an elliptical bubble, a short electron avalanche triggered a surface ionization wave (SIWs) resulting in plasma propagating along the surface of the bubble. In a circular bubble, an electron avalanche first traveled through the middle of the bubble before two SIWs began to propagate from the point closest to the grounded electrode where a volumetric streamer intersected the surface. In an elliptical bubble approaching a powered electrode in a pin-to-pin configuration, we experimentally observed streamer behavior that qualitatively corresponds with computational results. Optical emission captured over the lifetime of the streamer curve along the path of deformed bubbles, suggesting propagation of the streamer along the liquid/gas boundary interface. Plasma generation supported by the local field enhancement of the deformed bubble surface boundaries is a mechanism that is likely responsible for initiating streamer formation.
This work numerically investigates the effects of non-equilibrium nanosecond plasma discharge pulse rep- etition frequency, pulse number, and flow velocity on the critical ignition volume, minimum ignition energy, and chemistry in a plasma-assisted H 2 /air flow at 300 K and 1 atm using a multi-scale adaptive reduced chemistry solver for plasma assisted combustion (MARCS-PAC). The interactions between discharges/ignition kernels spanning decoupled, partially-coupled and fully-coupled regimes in a pulse train are studied. For a single pulse discharge, increased flow velocity increases the minimum ignition energy required due to the increase of convective heat loss and flame stretch. The results show that the minimum ignition kernel prop- agation speed at the critical ignition kernel volume increases with the flow velocity. The minimum critical ignition volume decreases with the increase of plasma discharge energy. For sequential two-pulse discharges, ignition fails at both decoupled and partially-coupled regimes even when the total discharge energy is above the minimum ignition energy, but succeeds only in the fully-coupled regime at a shorter inter-pulse time. Overlap of the OH radical pool between the sequential two-pulse discharges and the increase of the chemistry effect due to the increase of reduced electric field in the fully-coupled regime contribute to the ignition enhancement. In addition, for two-pulse discharges in the fully-coupled discharge regime, the mixture can be ignited at a total energy below the minimum ignition energy of a single pulse with the same flow conditions. Moreover, for a given total discharge energy with multiple pulsed discharges, the enhancement of the ignition kernel volume has a non-monotonic dependence on discharge frequency and pulse number. The effective ignition enhancement can be achieved with an optimal pulse repetition frequency and pulse number. Furthermore, this work provides a new understanding of the mechanism for repetitive plasma ignition and insights for the optimization of plasma ignition in a reactive flow.
M30 propellant grains that had been ignited in interrupted closed bomb experiments were characterize by scanning electron microscopy (SEM). Previous chemical analysis of extinguished grains had given no indications of plasma-propellant chemical interactions that could explain the increased burning rates that had been previously observed in full-pressure closed bomb experiments. (This does not mean that there is no unique chemistry occurring with plasma ignition. It may occur very early in the ignition event and then become obscured by the burning chemistry.) In this work, SEM was used to look at grain morphologies to determine if there were increases in the surface areas of the plasma-ignited grains which would contribute to the apparent increase in the burning rate. Charges were made using 30 propellant grains (approximately 32 grams) stacked in two tiers and in two concentric circles around a plastic straw. Each grain was notched so that, when the grains were expelled from the bomb during extinguishment, it could be determined in which tier and which circle each grain was originally packed. Charges were ignited in a closed bomb by either a nickel wire/Mylar-capillary plasma or black powder. The bomb contained a blowout disk that ruptured when the pressure reached 35 MPa, and the propellant was vented into a collection chamber packed with polyurethane foam. SEM analysis of the grains fired with a conventional black powder igniter showed no signs of unusual burning characteristics. The surfaces seemed to be evenly burned on the exteriors of the grains and in the perforations. Grains that had been subjected to plasma ignition, however, had pits, gouges, chasms, and cracks in the surfaces. The sides of the grains closest to the plasma had the greatest amount of damage, but even surfaces facing the outer wall of the bomb had small pits. The perforations contained gouges and abnormally burned regions (wormholes) that extended into the web. The SEM photos indicated that a grain from the top tier, which was farther away from the plasma ignition source, sustained more plasma-induced damage to the perforations and the web than did the grains on the bottom tier.
Polycarbonate films are subjected to plasma treatment in a number of applications such as improving adhesion between polycarbonate and silicon alloy in protective and optical coatings. The changes in surface chemistry due to plasma treatment have tendency to revert back. Thus stability of the plasma induced changes on polymer surfaces over desired time period is very important. The objective of this study was to examine the effect of ageing on atmospheric pressure helium-plasma treated polycarbonate (PC) sample as a function of treatment time. The ageing effects were studied over a period of 10 days. The samples were plasma treated for 0.5, 2, 5 and 10 minutes. Contact angle measurements were made to study surface energy changes. Modification of surface chemical structure was examined using, X-ray Photoelectron Spectroscopy (XPS). Contact angle measurements on untreated and plasma treated surfaces were made immediately, 24, 48, 72 and 96 hrs after treatment. Contact angle decreased from 93 deg for untreated sample to 30 deg for sample plasma treated for 10 minutes. After 10 days the contact angles for the 10 minute plasma treated sample increased to 67 deg, but it never reverted back to that of untreated surface. Similarly the O/C ratio increased from 0.136 for untreated sample to 0.321 for 10 minute plasma treated sample indication increase in surface energy.
We have used a combination of pico-to-nano temporal/spatial scale computational physics and chemistry modeling of plasma–material interfaces in the tokamak fusion plasma edges to unravel the evolving characteristics, not readily accessible by empirical means, of lithium-, oxygen-, and hydrogen-containing materials of plasma-facing components under irradiation by hydrogen and its isotopes. In the present calculation, amorphous lithium compound surfaces containing oxygen, Li 2 O, and LiOH were irradiated by 1-100 eV particles at incident angles on the surface ranging from perpendicular to almost grazing angles. Consequential surface processes, reflection, retention, and sputtering were studied at “the same footing” and compared to earlier results from amorphous Li and LiH surfaces. In conclusion, the critical role of charging dynamics of lithium, oxygen, and hydrogen atoms in the surface chemistry during hydrogen-fuel irradiation was found to drive the kinetics and dynamics of these surfaces in unexpected ways that ultimately could have profound effects on fusion plasma confinement behavior and surface erosion.
Abstract Steady-state deuterium plasma exposures were performed on ultra-high temperature ceramics titanium diboride (TiB 2 ) and zirconium diboride (ZrB 2 ) using the PISCES-RF linear plasma device (LPD) as early screening for first wall, plasma-facing applications. Deuterium plasma exposures were performed using 40 eV ion energies at 240, 525, and 800 °C sample temperatures and 90 eV ion energies at 240 °C sample temperatures to analyze TiB 2 and ZrB 2 surface morphology and chemistry evolution behavior. Post-plasma exposure chemistry characterization of the near surface ( < 50 nm) region of the samples all show transition metal enrichment, indicating boron preferential erosion. Transition metal to boron fractions vary with plasma exposure temperature under the 40 eV ion energy; metal enrichment is maximized at 800 °C and then minimized at 525 °C. SEM micrographs of all plasma exposed sample surfaces show no significant or noticeable plasma induced damage from cracking or blistering.
The methyl radical plays a central role in plasma-assisted hydrocarbon chemistry but is challenging to detect due to its high reactivity and strongly pre-dissociative electronically excited states. In this work, we report the development of a photo-fragmentation laser-induced fluorescence (PF-LIF) diagnostic for quantitative 2D imaging of methyl profiles in a plasma. This technique provides temporally and spatially resolved measurements of local methyl distributions, including in near-surface regions that are important for plasma-surface interactions such as plasma-assisted catalysis. The technique relies on photo-dissociation of methyl by the fifth harmonic of a Nd:YAG laser at 212.8 nm to produce CH fragments. These photofragments are then detected with LIF imaging by exciting a transition in the B-X(0, 0) band of CH with a second laser at 390 nm. Fluorescence from the overlapping A-X(0, 0), A-X(1, 1), and B-X(0, 1) bands of CH is detected near 430 nm with the A-state populated by collisional B-A electronic energy transfer. This non-resonant detection scheme enables interrogation close to a surface. The PF-LIF diagnostic is calibrated by producing a known amount of methyl through photo-dissociation of acetone vapor in a calibration gas mixture. We demonstrate PF-LIF imaging of methyl production in methane-containing nanosecond pulsed plasmas impinging on dielectric surfaces. Absolute calibration of the diagnostic is demonstrated in a diffuse, plane-to-plane discharge. Measured profiles show a relatively uniform distribution of up to 30 ppm of methyl. Relative methyl measurements in a filamentary plane-to-plane discharge and a plasma jet reveal highly localized intense production of methyl. The utility of the PF-LIF technique is further demonstrated by combining methyl measurements with formaldehyde LIF imaging to capture spatiotemporal correlations between methyl and formaldehyde, which is an important intermediate species in plasma-assisted oxidative coupling of methane.
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Understanding the effects of contaminant plasmas generated within the Z machine at Sandia is critical to understanding current loss mechanisms. The plasmas are generated at the accelerator electrode surfaces and include desorbed species found in the surface and substrate of the walls. These desorbed species can become ionized. The timing and location of contaminant species desorbed from the wall surface depend non-linearly on the local surface temperature. For accurate modeling, it is necessary to utilize wall heating models to estimate the amount and timing of material desorption. One of these heating mechanisms is Joule heating. In this paper, we propose several extended semi-analytic magnetic diffusion heating models for computing surface Joule heating and demonstrate their effects for several representative current histories. We quantitatively assess under what circumstances these extensions to classical formulas may provide a validatable improvement to the understanding of contaminant desorption timing.
Radioactive contaminants on the surfaces of detector components can be a problematic source of background events for physics experiments searching for rare processes. Exposure to radon is a specific concern because it can result in the relatively long-lived 210 Pb (and progeny) being implanted to significant subsurface depths such that removal is challenging. Here, in this article, we present results from a broad exploration of cleaning treatments to remove implanted 210 Pb and 210 Po contamination from silicon, which is a material frequently used in rare-events searches. We demonstrate for the first time that heat treatments (“baking”) can effectively mitigate such surface contamination, with a 1200 °C bake resulting in a 97$^{+2}_{-3}$% reduction. We also report results using wet-chemistry and plasma-based methods, which show that etching can be highly effective provided the etch depth is sufficiently aggressive. Our survey of cleaning methods suggests consideration of multiple approaches during the different phases of detector construction to enable greater flexibility for efficient removal of 210 Pb and 210 Po surface contamination.