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At least 289 records · Page 16

Investigation of N 2 /O 2 plasma interaction with Pt-catalyst: effect of metastable adsorbates on product hysteresis

The coupling of catalysts and atmospheric-pressure plasma has the potential to improve the efficiency of certain catalytic reactions. Understanding the changes that the catalyst surface undergoes during exposure to plasma is key to improving plasma–catalytic performance. In this work, long term exposure of Pt–Al 2 O 3 powder catalyst to an Ar/N 2 /O 2 non-equilibrium atmospheric-pressure plasma-jet was investigated. Products produced by the interaction were analyzed downstream with Fourier-transform infrared spectroscopy while surface species were analyzed operandi with diffuse reflectance infrared Fourier transform spectroscopy. During exposure, the catalyst temperature was ramped cyclically between 100 °C and 350 °C to understand how substrate temperature affects the plasma–catalyst interaction. Long-lasting changes were revealed to take place on the catalyst surface during plasma exposure. At low temperatures, Pt–O and Pt–NO accumulate on the surface which react at elevated temperatures to form NO 2 . NO 2 initially appears to spill on to the Al 2 O 3 support as nitrites and nitrates instead of desorbing. Stable surface conditions are only achieved after prolonged plasma exposure, when nitrate sites on the Al 2 O 3 support are filled. By changing the catalyst temperature at various rates, the impact of total plasma species flux to the surface was analyzed. It was found that decreasing the heating rate increased the hysteresis in the pattern of NO 2 formation during thermal cycling. The variation with temperature demonstrates that plasma exposure results in a buildup of surface NO x and oxygen species which react or desorb at high temperatures. The observed changes are discussed from the generic viewpoint that a non-equilibrium plasma interacting with a catalyst at low temperature introduces metastable steady-state surface conditions. Upon heating above a threshold temperature, the introduced surface modifications can change either due to thermal effects, or, for a plasma environment, by additional interaction with the incident plasma species flux. The surface/material changes take place in a highly predictable fashion and after sufficient time above the threshold temperature reach a steady-state condition that is different from the transient behavior that is observed during initial heating. During cooling the plasma-surface interaction exhibits a different behavior than during heating, and this results in hysteresis of diverse observables. The metastability/hysteresis description appears quite generic and analogous to hysteresis behavior seen for different systems. Furthermore, it is expected to be useful for understanding the consequences of plasma–catalyst surface interactions for various systems.

36 MATERIALS SCIENCE↗

Perovskite-Derived Cs 2 SnCl 6 –Silica Composites as Advanced Waste Forms for Chloride Salt Wastes

Advanced materials and processes are required to separate halides and fission products from complex salt waste streams associated with the chemical reprocessing of used nuclear fuels and molten salt reactor technologies for immobilization into chemically durable waste forms. Here, in this work, we explore an innovative concept using metal-halide perovskites as advanced host phases to incorporate Cs and Cl with very high waste loadings. Wet chemistry-synthesized Cs 2 SnCl 6 powders from CsCl salt solutions are successfully encapsulated into a silica matrix to form a composite using low-temperature spark plasma sintering with tunable Cs and Cl loadings up to 31 wt.% and 26 wt.%, respectively. Chemical durability testing of the composite waste forms by semi-dynamic leaching experiments demonstrates that incongruent leaching mechanism dominated. The metal-halide perovskite-silica composite waste forms display exceptional chemical durability with the long-term release rates of Cs and Cl comparable to or outperforming the state-of-the-art waste form materials but with significantly higher waste loadings. The scalable synthesis of the metal-halide perovskite from wet-chemistry processes opens up new opportunities in designing perovskite-glass composite waste forms for salt wastes with very high waste loadings and exceptional chemical durability for the sustainable development of advanced fuel cycles and next-generation reactor technologies.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Anodic arc discharge: Why pulsed?

Pulsed anodic arc discharge is a novel synthesis method of nanomaterials by means of low-temperature atmospheric plasma. The technique consists in periodically supplying DC power to two vertically aligned electrodes in the form of short unipolar pulses with peak currents of a few hundred Amperes in helium atmosphere. The pulsed arc plasmas are sustained at frequencies of the order of 1 Hz with around 10% of duty cycle. It constitutes a versatile technique thanks to a series of advantages compared to continuous DC arc processes, in particular: flexibility in the experimental conditions, process stability and repeatability, better utilization of ablating anode material, lower production of macroparticles, and lower thermal loads. Such features are discussed in this article. A brief overview concerning the recent accomplishments of pulsed arc discharge on deposition of carbon nanostructures (graphene and carbon nanotubes) and few-layer flakes of molybdenum disulphide (MoS 2 ) is provided, as well as an outlook on future applications of this method for the discovery of new materials with tailored functional properties.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Volumetric recombination in EMC3-EIRENE: Implementation and first application to the pre-fusion power operation phase in ITER

An upgrade to the 3D plasma boundary model EMC3-EIRENE for detached divertor plasmas is introduced and evaluated. Stabilization of the iterative approximation of a self-consistent plasma–neutral gas solution is required at low divertor plasma temperatures, and this has been achieved by linearization of the energy loss term associated with the electron–neutral gas interaction. An implicit method for volumetric recombination has been implemented, which improves agreement with SOLPS-ITER results for the pre-fusion power operation phase in ITER. Resonant magnetic perturbations for control of edge localized modes are found to result in a partially detached divertor plasma with a significantly broader reduction of particle loads in the traditional strike zone, which is attributed to volumetric recombination. The additional non-axisymmetric far scrape-off layer strike points, on the other hand, remain attached at relatively high temperature so that volumetric recombination is not effective there.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

First impurity powder injection experiments in LHD

Injection of impurities in the form of sub-millimeter powder grains is performed for the first time in the Large Helical Device (LHD) plasma, employing the Impurity Powder Dropper (IPD) [A. Nagy et al., RSI 2018], developed and built by PPPL. Controlled amounts of boron (B) and boron nitride (BN) powder are injected into the helical plasma. Visible camera imaging, UV and charge exchange spectroscopy measurements show that the injected impurities effectively penetrate into the plasma in two different magnetic configurations.The prompt effects of the impurities on the plasma are characterized as the injection rate is scanned. The injected impurities provide a supplemental electron source, causing the plasma density to increase, together with the radiated power. Beneficial effects on the confined plasma temperature are observed at low plasma densities, due to an increased efficiency in NBI power absorption. For $n_{e,av}<10^{19}m^{-3}$ the powder grains penetrate deeper into the plasma, as they can be less effectively deflected by the plasma flow in the divertor leg, which they have to cross first as they are injected from the top of the machine.In this case, the created B ions are observed to move outwards from UV spectroscopy and charge exchange measurements, due to the outwards direction of the radial electric field. This makes low density plasmas a better candidate for powder boronization techniques.

Boron↗

Decarbonization of Off-Road, Rail, Marine, and Aviation (DORMA) Program (2023 Annual Progress Report)

This document summarizes the progress of VTO's Decarbonization of Off-Road, Rail, Marine, and Aviation (DORMA) program during the fiscal year 2023. DORMA's R&D focus was on research, development, and demonstration of new propulsion and vehicle technologies that will reduce greenhouse gas emissions in difficult-to-decarbonize transportation applications.

33 ADVANCED PROPULSION SYSTEMS↗

Ion streams in the magnetotail

Ion mass spectrometer observations of low-temperature streaming plasmas in the earth's magnetotail are reported. Measurements in the energy per charge range 0 to 17 keV/e were made at geocentric radial distances less than 23 earth radii from the ISEE 1 spacecraft. Ion streams of solar wind origin in the magnetotail boundary layer and of ionospheric origin in the tail lobes and plasma sheet are described. A statistical study of some of the characteristics of the streams allows the inference that the central tail lobe plasmas are primarily constituted of ion streams of ionospheric origin and that the ionosphere is a significant contributor to the hot plasmas that form the plasma sheet.

Sharp, R. D.↗

Charging of a large object in low polar Earth orbit

The charging of a large sphere subject to the environment encountered by the shuttle orbiter as it passes through the auroral regions in its low polar Earth orbit was investigated. The environment consists of a low temperature dense plasma and a relatively intense (200 mu A/sq m) field aligned flux of energetic electrons (approximately 5 to 10 keV). The potential on a sphere in eclipse is presented as a function of the ratio kappa of the charging rate produced by precipitating electrons to the discharging rate produced by ram ions. It was found that a 5 meter conducting sphere charges to potentials of order 1 kilovolt for kappa approximately 2, even though a 0.5 meter sphere charges to less than 100 volts. It is concluded that the natural charging environment can induce large potentials (approximately 1 kilovolt) on the shuttle orbiter.

Parks, D. E.↗

Ultraviolet observations of stellar coronae - Early results from HST

The first GHRS spectra of two very different late-type giant stars - Capella and Gamma Dra are reported. Capella is a 104 day period binary system consisting of two stars (G9 III and GO III) each of which shows bright emission lines formed in solar-like transition region and coronae. By contrast, Gamma Dra is a hybrid-chromosphere star with very weak emission lines from high-temperature plasma. Low-dispersion spectra of these stars covering the 1160 to 1717 A spectral range show unresolved emission lines from neutral species through N V. The very different surface fluxes detected in the spectra of these stars suggest different types of heating mechanisms.

Linsky, Jeffrey L.↗

Neutrino Heat Conduction and Inhomogeneities in the Early Universe

Constraints on parameters of inhomogeneous nucteosynthesis, namely, the overdensity and size of baryon lumps, are found by calculatig the blackbody neutrino heat conduction into the lumps, which tends to inflate them away. The scale size for efficient heat conduction is determined by the mean free path lambda of the neutrino, and so we compute lambda in our case of a high-temperature plasma with low chemical potential, and find a general result that many-body effects are unimportant, simplifying the calculation. We find that in the region of interest for nucleosynthesis, neutrino inflation is important for overdensities greater than 10(exp 4).

Heckler, A.↗

Solar-B X-ray Telescope (XRT) Concept Study Report

The X-ray observations from the Yohkoh SXT provided the greatest step forward in our understanding of the solar corona in nearly two decades. Expanding on the accomplishments of Yohkoh, we believe that the scientific objectives of the Solar-B mission are achieved with a significantly improved X-ray telescope (XRT) similar to the SXT. The Solar-B XRT will have twice the spatial resolution and a broader temperature response, while building on the knowledge gained from the successful Yohkoh mission. We present the scientific justification for this view, discuss the instrumental requirements that flow from the scientific objectives, and describe the instrumentation to meet these requirements. We then provide a detailed discussion of the design activities carried out during Phase A, noting the conclusions that were reached in terms of their implications for the detailed design activities which are now commencing. Details of the instrument that have changed as a result of the Phase A studied are specifically noted, and areas of concern going into Phase B are highlighted. XRT is a grazing-incidence (GI) modified Wolter I X-ray telescope, of 35cm inner diameter and 2.7m focal length. The 2048x2048 back-illuminated CCD (now an ISAS responsibility) has 13.5 micron pixels, corresponding to 1.0 arcsec and giving full Sun field of view. This will be the highest resolution GI X-ray telescope ever flown for Solar coronal studies, and it has been designed specifically to observe both the high and low temperature coronal plasma. A small optical telescope provides visible light images for co-alignment with the Solar-B optical and EUV instruments. The XRT science team is working in close cooperation with our Japanese colleagues in the design and construction of this instrument. All of the expertise and resources of the High Energy and Solar/Stellar Divisions of the Center for Astrophysics are being made available to this program, and our team will carry its full share of responsibility for mission operations, data reduction and education and public outreach. All aspects of the XRT design were reviewed during Phase A. The study focussed particularly on those aspects that have the greatest affect on instrument performance and extended lifetime, on the image quality error budget, and on the camera (mechanical and electrical) interface and the instrument mounting interfaces. The present instrument design differs in some details from that originally proposed. Selection of the XRT for Phase A study was contingent upon the removal of the camera and its associated electronics, and the acceptance of a stringent cost cap. The removal of the electronics left the XRT without control electronics for the instrument mechanisms. A mechanism controller was therefore added. The removal of the camera resulted in major complications to the integration and test plan. After many discussions, it was decided that the system would be less expensive, and the risk of unacceptable performance lower, if we include a focus mechanism. The remainder of the XRT design baseline matches the proposed configuration. Data requirements for the XRT are driven by the science plans, which are based on the physical processes in the solar outer atmosphere. Discussions to date of the XRT observing plan, both alone and in conjunction with the other Solar-B instruments, shows that the XRT needs 2 Gbits of on-board storage, at least one circulating buffer of 640 Mbits, and twelve 10- minute downlinks per day in order to carry out its required programs.

Golub, Leon↗

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↗