Low-temperature Hydrogen Peroxide Gas Plasma-a Sterilization Process Useful in Space Exploration Technology
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hydrogen peroxide material compatibility microbial↗
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Microwave-Fluidized Catalytic Reactor for the Direct Conversion of Methane to Higher Hydrocarbons (Final Report)
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03 NATURAL GAS↗
Particle Access and Charging Environments in the Lunar Wake
A plasma wake a region of low density, high temperature plasma forms on the far side of the Moon when solar wind, magnetosheath, and magnetotail plasma flows past the Moon [Manka, 1973; Ogilvie et al., 1996; Farrell et al., 1998; Halekas et al., 2005]. Ion populations in these flows typically have much smaller thermal velocity than bulk speed and are therefore excluded from the plasma wake while the large thermal electron velocity allows the lighter negatively charged particles to stream ahead of the ions into the wake. Charge separation due to electrons streaming ahead of the ions into the wake from the wake boundary establishes an ambipolar electric field which impedes the motion of electron flow and accelerates ions into the wake [Ogilvie et al., 1996; Farrell et al., 1997]. We have conducted a theoretical study of acceleration (and deceleration) of charged particles in lunar plasma environments, which investigated the mechanisms responsible for allowing solar wind entry into the lunar wake, and for producing energetic particle distributions observed within the lunar wake. To this end, the investigation utilized a macroscale 3D hybrid particle-in-cell numerical model of the interaction of the Moon with external plasma environments to compute electric fields in the lunar environment for a variety of external plasma conditions and interplanetary magnetic field orientations. Ion dynamics were attained from the hybrid code while electron dynamics were determined by considering electron test particle trajectories through the fields established in the hybrid code. Results from the code will be presented to evaluate charging environments within the lunar wake.
Parker, Linda↗
The boundary layers as the primary transport regions of the earth's magnetotail
A comprehensive survey of ISEE and IMP LEPEDEA plasma measurements in the earth's magnetotail reveals that the magnetospheric boundary layer and the plasma sheet boundary layer are the primary transport regions there. These plasma measurements also reveal various components of the plasma sheet, including the central plasma sheet and plasma sheet boundary layer. A significant new result reported here is that of cold- and hot-plasma components that are spatially co-present within the central plasma sheet. Such plasma components cannot be explained merely by temporal variations in spectra involving the entire plasma sheet. Contributions to a low temperature component of the plasma sheet enter directly from the boundary layer located along the magnetotail flanks. Field-aligned flows predominate within the plasma sheet boundary layer which is almost always present and is located near the high- and low-latitude border of the plasma sheet. The plasma sheet boundary layer comprises highly anisotropic ion distributions, including counter-streaming ion beams, that evolve into the hot, isotropic component of the plasma sheet. Tailward acceleration regions generate these ion beams with plasma input from the magnetospheric boundary layer. Antisunward-flowing ion beams, at E/q less than 1 kV and of ionospheric composition, are frequently observed in the plasma sheet boundary layer and in tail lobes. These ion beams are likely accelerated at low altitude over the polar cap and especially along auroral field lines.
Eastman, T. E.↗
Multi‐Scale Model‐Informed Deep Learning for Plasma‐Nanoparticle Interaction
The Overarching Goal of this proposed research is to understand and quantitively determine the interactions between non-thermal plasma (hot electrons, reactive radicals, vibrationally excited species) and surface reactions on influencing the activity and selectivity of the desired reactions via developing multi-scale model informed deep learning algorithm. Investigating non-thermal plasma-surface interaction is feasible due to the low bulk temperature in the discharge region. To investigate the role of plasma-nanoparticle interaction on enhancing the reaction kinetics, we will focus on ammonia cracking to generate clean hydrogen over earth-abundant, non-critical metallic nanoparticles, which is of great significance for decarbonization. We hypothesize that (1) reactive radicals interacting with surface reaction species via Eley–Rideal mechanism will significantly lower the energetics of the potential rate-limiting step of nitrogen formation; (2) the surface will be charged heterogeneously under non-thermal plasma conditions and the charged site will lower the energetics of ammonia cracking through Langmuir– Hinshelwood mechanism; (3) vibrationally excited ammonia will further promote the initial N-H bond cleavage. To access the hypothesis, we will (1) reveal the surface charge effects on tunning the reaction energetics via interpretable, physics-informed deep learning accelerated density functional theory (DFT) calculations; (2) determine the reactive radicals interacting with surface reaction species on tuning the reaction energetics via DFT; (3) reveal the surface charge effects on tunning the reaction energetics via DFT and deep learning models, (4) quantify how vibrationally excited species, reactive radicals, and surface charging effects on enhancing the catalysis via developing DFT-based microkinetic modeling (MKM) and active learning. Deep and active learning of plasma-nanoparticle interactions effects on enhancing ammonia cracking to generate hydrogen represents a new paradigm for designing high performance plasma materials. The fundamental science of how plasma-nanoparticle interactions will change the plasma kinetics and will improve the energy efficiency for decarbonization and sustainability. The interpretable and physics-informed machine learning model will accelerate low temperature plasma chemistry and material discovery with physics rules and model interpretation.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
Low-temperature etching of silicon oxide and silicon nitride with hydrogen fluoride
Etching of high aspect ratio features into alternating SiO 2 and SiN layers is an enabling technology for the manufacturing of 3D NAND flash memories. In this paper, we study a low-temperature or cryo plasma etch process, which utilizes HF gas together with other gas additives. Compared with a low-temperature process that uses separate fluorine and hydrogen gases, the etching rate of the SiO 2 /SiN stack doubles. Both materials etch faster with this so-called second generation cryo etch process. Pure HF plasma enhances the SiN etching rate, while SiO 2 requires an additional fluorine source such as PF 3 to etch meaningfully. Further, the insertion of H 2 O plasma steps into the second generation cryo etch process boosts the SiN etching rate by a factor of 2.4, while SiO 2 etches only 1.3 times faster. We observe a rate enhancing effect of H 2 O coadsorption in thermal etching experiments of SiN with HF. Ammonium fluorosilicate (AFS) plays a salient role in etching of SiN with HF with and without plasma. AFS appears weakened in the presence of H 2 O. Density functional theory calculations confirm the reduction of the bonding energy when NH 4 F in AFS is replaced by H 2 O.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Plasma-catalyst modeling for materials selection: challenges and opportunities in nitrogen oxidation
Reliable kinetic models are essential to rationalize observations and to guide the selection of appropriate plasma-catalyst combinations. Kinetic models coupling plasma- and heterogeneous-catalytic-chemistries, however, are primitive. Here, we combine reduced plasma chemistries and density functional theory parameterized surface reactions to model NO formation from N2 oxidation, an alternative nitrogen fixation process. We first show plasma excited species can enhance turnover frequencies of both Pt and Au. The enhancing potential is a function of plasma species and their densities. We then compare NO production between plasma/Pt and plasma/Au with an integral reactor model and explore the dependence of NO production as a function of plasma conditions, reactor configurations and chemical compositions. Plasma/Pt generates more NO than plasma/Au under most thermal and plasma parametric conditions. Plasma/Au outperforms plasma/Pt under high plasma excitations at low temperatures. Furthermore, these results highlight that selection of plasma-catalyst combinations should consider the properties of plasmas, materials and the coupling of the two.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Plasma chemistry for inorganic materials
Practical application of plasma chemistry to the development of inorganic materials using both low temperature and warm plasmas are summarized. Topics cover: the surface nitrification and oxidation of metals; chemical vapor deposition; formation of minute oxide particles; the composition of oxides from chloride vapor; the composition of carbides and nitrides; freezing high temperature phases by plasma arc welding and plasma jet; use of plasma in the development of a substitute for petroleum; the production of silicon for use in solar cell batteries; and insulating the inner surface of nuclear fusion reactor walls.
Matsumoto, O.↗
Signatures of shock drivers in the solar wind and their dependence on the solar source location
Solar wind and energetic ion observations following 40 interplanetary shocks with well-established solar source locations have been examined in order to determine whether signatures characteristic of the coronal material forming the shock driver are present. The signatures considered include magnetic-field-aligned bidirectional ion flows observed by the ISEE 3 and IMP 8 spacecraft; bidirectional solar wind electron heat fluxes; solar wind plasma proton and electron temperature depressions; low-beta plasma; enhanced, low-variance magnetic fields; and energetic ion depressions. Several shock driver signatures are commonly observed following shocks originating from within about 50 deg of central meridian, and are generally absent for other events. We conclude that shock drivers generally extend up to about 100 deg in longitude, centered on the solar source longitude. Since shocks from central meridian events are not usually associated with all the shock driver signatures examined, the absence of a driver cannot be confirmed from consideration of one of these signatures alone. We also find evidence that a few bidirectional energetic ion and solar wind electron heat flux events following shocks (in particular from far eastern sources) may occur on open field lines outside of shock drivers.
Richardson, I. G.↗
Efficient ECCD non-inductive plasma current start-up, ramp-up, and sustainment for an ST fusion reactor
The elimination of the need for an Ohmic heating solenoid may be the most impactful design driver for the realization of economical compact fusion tokamak reactor systems. However, this would require fully non-inductive start-up and current ramp-up from zero plasma current and low electron temperature of sub-keV to the full plasma current of ~10–15 MA at 20–30 keV electron temperature. To address this challenge, an efficient solenoid-free start-up and ramp-up scenario utilizing a low-field-side-launched extraordinary mode at the fundamental electron cyclotron harmonic frequency (X–I) is proposed, which has more than two orders of magnitude higher electron cyclotron current drive (ECCD) efficiency than the conventional ECCD for the sub-keV start-up regime. A time dependent model was developed to simulate the start-up scenarios. For the Spherical Tokamak Advanced Reactor (STAR) (Menard et al 2023 Next-Step Low-Aspect-Ratio Tokamak Design Studies (IAEA)), it was found that to fully non-inductively ramp-up to 15 MA, it would take about 25 MW of EC power at 170 GHz. Because of the relatively large plasma volume of STAR, radiation losses must be considered. It is important to make sure that high Z impurities are kept sufficiently low during the early current start-up phase where the temperature is sub-keV range. Since the initial current ramp up takes place at a factor of ten lower density compared to the sustained regimes, it is important to transition into a higher bootstrap fraction discharge at lower density to minimize the ECCD power requirement during the densification. For the sustainment phase an array of eight gyrotron launchers with a total of about 60 MW of fundamental O-mode was found to be sufficient to provide the required axis-peaked external current drive. High efficiencies between 19–57 kA MW –1 were found with optimal aiming, and these were resilient to small changes in aiming angles and density and temperature profiles.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Computational Fluid Dynamics Modeling of Low Temperature Ignition Processes From a Nanosecond Pulsed Discharge at Quiescent Conditions
Recent interest in nonequilibrium plasma discharges as sources of ignition for the automotive industry has not yet been accompanied by the availability of dedicated models to perform this task in computational fluid dynamics (CFD) engine simulations. The need for a low-temperature plasma (LTP) ignition model has motivated much work in simulating these discharges from first principles. Most ignition models assume that an equilibrium plasma comprises the bulk of discharge kernels. LTP discharges, however, exhibit highly nonequilibrium behavior. In this work, a method to determine a consistent initialization of LTP discharge kernels for use in engine CFD codes like CONVERGE is proposed. The method utilizes first principles discharge simulations. Such an LTP kernel is introduced in a flammable mixture of air and fuel, and the subsequent plasma expansion and ignition simulation is carried out using a reacting flow solver with detailed chemistry. Finally, the proposed numerical approach is shown to produce results that agree with experimental observations regarding the ignitability of methane-air and ethylene-air mixtures by LTP discharges.
33 ADVANCED PROPULSION SYSTEMS↗
Microwave diagnostic for the determination of the electron temperature of a low density shock-heated argon plasma
The diffraction, defocusing and beam bending effects of microwaves transmitted through a bounded shock-heated argon plasma with low electron density are investigated with the purpose of developing an accurate method for electron temperature (Te) determination. This report describes the evaluation technique and presents results for an argon plasma with pressure between 3 and 10 torr, and T2 between 5500 and 9500 K. The electron temperature values obtained have a range of uncertainty between -20% and +10% only. The electron temperature is equal or lower by approximately 1000 K in comparison to the heavy particle temperature (T2).
Schneider, C. P.↗
Toward sustainable production of N-containing products via nonthermal plasma-enhanced conversion of natural gas resources
Nonthermal plasmas can directly activate and cleave the strong chemical bonds in molecular nitrogen and methane to facilitate the transformation of these inherently stable molecules through the application of electrical energy. Here, we report a low temperature, atmospheric pressure, nonthermal plasma for the “one-pot” synthesis of olefins, alkynes, higher molecular weight hydrocarbons, ammonia, and nitrogen-containing liquids from a representative shale gas feed enriched with nitrogen. Furthermore, we reproducibly observe a wide range of valuable and synthetically challenging gas-phase and liquid-phase products containing C-N, C-C, and N-H bonding by controlling the N 2 concentration in the inlet feed stream. In nitrogen-lean regimes, hydrocarbon products dominate (e.g., ethylene, acetylene, etc.), while nitrogen-rich regimes promote incorporation of nitrogen into the products, leading to the formation of ammonia and liquid products containing a variety of functionalities (e.g., nitriles, amines, heterocycles). High resolution electrospray ionization mass spectrometry was used to measure molecular weights and identify the chemical formulas of the liquid products. Van Krevelen diagrams were created and showed many products with compositions around H/C = 2 and N/C = 0.5, indicating the potential importance of intermediate species with these ratios for liquid formation (e.g., CH 3 CN + H).
03 NATURAL GAS↗
Electron-field instability: Excitation of electron plasma waves by an electric field
Electric fields are commonplace in plasmas and affect transport by driving currents and, in some cases, instabilities. The necessary condition for instability in collisionless plasmas is commonly understood to be described by the Penrose criterion, which quantifies a sufficient relative drift between different populations of particles that must be present for wave amplification via inverse Landau damping. For example, electric fields generate drifts between electrons and ions that can excite the ion-acoustic instability. Here, we use particle-in-cell simulations and linear stability analysis to show that the electric field can drive a fundamentally different type of kinetic instability, named the electron-field instability. This instability excites electron plasma waves with wavelengths ≳30λ De , has a growth rate that is proportional to the electric field strength, and does not require a relative drift between electrons and ions. The Penrose criterion does not apply when accounting for the electric field. Furthermore, the large value of the observed frequency, near the electron plasma frequency, further distinguishes it from the standard ion-acoustic instability, which oscillates near the ion plasma frequency. The ubiquity of macroscopic electric fields in quasineutral plasmas suggests that this instability is possible in a host of systems, including low-temperature and space plasmas. In fact, damping from neutral collisions in such systems is often not enough to completely damp the instability, adding to the robustness of the instability across plasma conditions.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Understanding the Impact of Return-Current Losses on the X-Ray Emission from Solar Flares
I obtain and examine the implications of one-dimensional analytic solutions for return-current losses on an initially power-law distribution of energetic electrons with a sharp low-energy cutoff in flare plasma with classical (collisional) resistivity. These solutions show, for example, that return-current losses are not sensitive to plasma density, but are sensitive to plasma temperature and the low energy cutoff of the injected nonthermal electron distribution. A characteristic distance from the electron injection site, x(sub rc), is derived. At distances less than x(sub rc) the electron flux density is not reduced by return-current losses, but plasma heating can be substantial in this region, in the upper, coronal part of the flare loop. Before the electrons reach the collisional thick-target region of the flare loop, an injected power-law electron distribution with a low-energy cutoff maintains that structure, but with a flat energy distribution below the cutoff energy, which is now determined by the total potential drop experienced by the electrons. Modifications due to the presence of collisional losses are discussed. I compare these results with earlier analytical results and with more recent numerical simulations. Emslie's 1980 conjecture that there is a maximum integrated X-ray source brightness on the order of 10(exp -15) photons per square centimeter per second per square centimeter is examined. I find that this is not actually a maximum brightness and its value is parameter dependent, but it is nevertheless a valuable benchmark for identifying return-current losses in hard X-ray spectra. I discuss an observational approach to identifying return-current losses in flare data, including identification of a return-current "bump" in X-ray light curves at low photon energies.
Holman, Gordon D.↗
Spacecraft Charging in Low Temperature Environments
Spacecraft charging in plasma and radiation environments is a temperature dependent phenomenon due to the reduction of electrical conductivity in dielectric materials at low temperatures. Charging time constants are proportional to l/conductivity may become very large (on the order of days to years) at low temperatures and accumulation of charge densities in insulators in charging environments traditionally considered benign at ambient temperatures may be sufficient to produce charge densities and electric fields of concern in insulators at low temperatures. Low temperature charging is of interest because a number of spacecraft-primarily infrared astronomy and microwave cosmology observatories-are currently being design, built, and or operated at very cold temperatures on the order of 40K to 100K. This paper reviews the temperature dependence of spacecraft charging processes and material parameters important to charging as a function of temperature with an emphasis on low temperatures regimes.
Parker, Linda N.↗
The impedance characteristic of a spherical probe in an isotropic plasma.
Experimental investigation of the impedance characteristic of a spherical plasma probe for a quantitative assessment of theoretical work, and of hydrodynamic or fluid theory in particular. A stable, low-temperature (about 500K) plasma was produced in nitrogen by a cold-cathode discharge, with a plasma frequency of the order of 15 MHz and with an electron collision frequency in the range from one to ten million per sec. Hydrodynamic probe theory was tested against the experimental results for the specific cases corresponding to the probe at floating potential and at space potential. Good agreement was obtained for both the real and imaginary parts. The real part of the impedance shows a peak near the plasma frequency, a small shift being explicable in terms of realistic sheath profiles. Electron density can thus be deduced rather accurately, and electron temperature approximately, on the basis of hydrodynamic theory. Accurate values of the electron-neutral collision frequency were also obtained for plasmas where the collision frequency was larger than 0.4 times the radian plasma frequency. At lower pressures the presence of collisionless or Landau damping was clearly established, and the more accurate kinetic theory is necessary to explain the experimental results.
Tarstrup, J.↗
Impact of CH 4 addition on the electron properties and electric field dynamics in a Ar nanosecond-pulsed dielectric barrier discharge
Non-equilibrium plasmas derive their low temperature reactivity from producing and driving energetic electrons and active species under large electric fields. Therefore, the impact of reactants on the plasma properties including electron number density, electric field, and electron temperature is critical for applications such as plasma CH 4 reforming. Due to experimental complexity, electron properties and the electric field are rarely measured together in the same discharge. Here, we combine time-resolved Thomson scattering and electric field induced second harmonic generation (EFISH) to probe electron temperature, electron density, and electric field strength in a 60 Torr CH 4 /Ar nanosecond-pulsed dielectric barrier discharge (ns-DBD) while varying the CH 4 mole fraction from 0 to 8%. These measurements are compared to a 1-D numerical model to benchmark its predictions and identify areas of uncertainty. Nonlinear coupling between CH 4 addition, electron temperature, electron density, and the electric field was directly observed. Contrary to previous measurements in He, the electron temperature increased with CH 4 mole fraction. This rise in electron temperature is identified as electron heating by residual electric fields that increased with larger CH 4 mole fraction. Moreover, the electron number density has been found to decrease rapidly with the increase of methane mole fraction. Comparison of these measurements with the model yielded better agreement at higher CH 4 mole fractions and with the usage of ab initio calculated Ar electron-impact cross-sections from the B-spline R-matrix (BSR) database. Furthermore, the calculated plasma properties are shown to be sensitive to the residual surface charge implanted on the quartz dielectric surfaces. Without considering surface charge in the simulations, the calculated electric field profiles agreed well with the measurements, but the electron properties were underpredicted by more than a factor of three. Therefore, measurements of either the electric field or electron properties measurements alone are insufficient to fully validate modelling predictions.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗