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At least 757 records · Page 42

Laser Ablation Plasmas and Spectroscopy for Nuclear Applications

The development of measurement methodologies to detect and monitor nuclear-relevant materials remains a consistent and significant interest across the nuclear energy, nonproliferation, safeguards, and forensics communities. Optical spectroscopy of laser-produced plasmas is becoming an increasingly popular diagnostic technique to measure radiological and nuclear materials in the field without sample preparation, where current capabilities encompass the standoff, isotopically resolved and phase-identifiable (e.g., UO and UO[Formula: see text]) detection of elements across the periodic table. These methods rely on the process of laser ablation (LA), where a high-powered pulsed laser is used to excite a sample (solid, liquid, or gas) into a luminous microplasma that rapidly undergoes de-excitation through the emission of electromagnetic radiation, which serves as a spectroscopic fingerprint for that sample. This review focuses on LA plasmas and spectroscopy for nuclear applications, covering topics from the wide-area environmental sampling and atmospheric sensing of radionuclides to recent implementations of multivariate machine learning methods that work to enable the real-time analysis of spectrochemical measurements with an emphasis on fundamental research and development activities over the past two decades. Background on the physical breakdown mechanisms and interactions of matter with nanosecond and ultrafast laser pulses that lead to the generation of laser-produced microplasmas is provided, followed by a description of the transient spatiotemporal plasma conditions that control the behavior of spectroscopic signatures recorded by analytical methods in atomic and molecular spectroscopy. High-temperature chemical and thermodynamic processes governing reactive LA plasmas are also examined alongside investigations into the condensation pathways of the plasma, which are believed to serve as chemical surrogates for fallout particles formed in nuclear fireballs. Laser-supported absorption waves and laser-induced shockwaves that accompany LA plasmas are also discussed, which could provide insights into atmospheric ionization phenomena from strong shocks following nuclear detonations. Furthermore, the standoff detection of trace radioactive aerosols and fission gases is reviewed in the context of monitoring atmospheric radiation plumes and off-gas streams of molten salt reactors. Finally, concluding remarks will present future outlooks on the role of LA plasma spectroscopy in the nuclear community.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Stability of Mn-Doped TiO 2 Thin-Film Anodes during Water Oxidation Reactions

Incorporating manganese atoms into TiO 2 has been shown to improve its activity for water oxidation. However, its activity has been observed to steadily degrade under constant applied potential, especially at more oxidizing applied potentials. Here, the compositional profile and electrochemical stability of Mn-doped TiO 2 (Mn:TiO 2 ) thin-film electrodes precisely fabricated by atomic layer deposition (ALD) were evaluated to elucidate the mechanisms of electrode degradation. Although ALD enables the deposition of Mn dopants throughout the film thickness, only Mn within 1.5 nm of the surface was observed to be redox active. Annealing Mn:TiO 2 films in air leads to the diffusion of Mn toward the electrode surface and oxidation of the Mn and alters the redox behavior. Annealing endows greater stability to Mn redox behavior but does not fully stabilize the water oxidation current, suggesting that the two electrochemical processes are not precisely correlated. In situ inductively coupled plasma mass spectrometry reveals that Mn is lost from Mn:TiO 2 films at potentials greater than 1.8 V vs RHE. However, the initial Mn loss is equivalent to less than a single ALD layer of MnO x . Longer-term constant potential experiments suggest that Mn is lost from up to 1 nm of the electrode surface but that this loss may account for only a portion of the diminished water oxidation activity.

atomic layer deposition↗

Ligand-induced transmembrane conformational coupling in monomeric $\mathrm{EGFR}$

Single pass cell surface receptors regulate cellular processes by transmitting ligand-encoded signals across the plasma membrane via changes to their extracellular and intracellular conformations. This transmembrane signaling is generally initiated by ligand binding to the receptors in their monomeric form. While subsequent receptor-receptor interactions are established as key aspects of transmembrane signaling, the contribution of monomeric receptors has been challenging to isolate due to the complexity and ligand-dependence of these interactions. By combining membrane nanodiscs produced with cell-free expression, single-molecule Förster Resonance Energy Transfer measurements, and molecular dynamics simulations, we report that ligand binding induces intracellular conformational changes within monomeric, full-length epidermal growth factor receptor (EGFR). Our observations establish the existence of extracellular/intracellular conformational coupling within a single receptor molecule. We implicate a series of electrostatic interactions in the conformational coupling and find the coupling is inhibited by targeted therapeutics and mutations that also inhibit phosphorylation in cells. Collectively, these results introduce a facile mechanism to link the extracellular and intracellular regions through the single transmembrane helix of monomeric EGFR, and raise the possibility that intramolecular transmembrane conformational changes upon ligand binding are common to single-pass membrane proteins.

59 BASIC BIOLOGICAL SCIENCES↗

Optimization Methodology of Polar Direct-Drive Illumination for the National Ignition Facility

Improved laser illumination uniformity drives shocks and implosions to create more extreme high energy density environments. Predominantly, the geometry of experiments that can be performed is dictated by the layout of beams at laser facilities, limiting inter-facility and multiscale investigations. This Letter presents the first automated, algorithmic approach for generating illumination configurations for high energy density experiments. The method is demonstrated in comparison to a polar direct drive solid target experiment at the National Ignition Facility. The new illumination configuration is simulated to create greater than ×3 higher peak pressure and almost ×2 higher density by maintaining better shock uniformity. Furthermore, the optimization process is performed with reduced computational expense and isotropic plasma profiles, while accounting for the impact of cross-beam energy transfer.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

An overview of new measurements of flow, chirality and vorticity from STAR experiment

In relativistic heavy-ion collisions, the properties of quark–gluon plasma (QGP) and complex dynamics of multi-scale processes in Quantum Chromodynamics (QCD) are studied by analyzing the final state produced particles in a variety of different ways. In these proceedings, we present an overview of new detailed measurements of flow, chirality and vorticity by the STAR experiment at Relativistic Heavy Ion Collider (RHIC). Furthermore, STAR’s future opportunities for the precision measurements on small systems, fixed-target (FXT) mode, and Beam Energy Scan (BES-II) program are discussed.

Physics↗

Measurement and Modeling of Electron Temperature in Laboratory Photoionized Plasmas Relevant to Astrophysics

The electron temperature of photoionized plasmas characterizes the thermalization of photoelectrons, impacts the charge-state distribution, emissivity, and opacity through atomic recombination processes, and is needed to perform detailed comparisons with theory predictions. We discuss temperature measurements in laboratory photoionized plasmas and a comparison with model calculations done with several theory approximations and codes. These include a radiation-hydrodynamics simulation and two nonequilibrium heating and ionization models that tracked the evolution of the internal energy of the electrons. Furthermore, for the same physics model and X-ray flux time history, calculations were performed assuming steady-state or time-dependent conditions. The time history of steady-state results correlates with that of the X-ray flux, while that of the time-dependent cases does not, and it is qualitatively and quantitatively different from the steady-state case. Steady-state results significantly overestimated temperature measurements, while time-dependent results produced better approximations, which suggests the importance of transient effects in the experiment and also the need for time-resolved measurements.

Laboratory astrophysics↗

Energy Partition in Collisionless Counterstreaming Plasmas

Fast, counterstreaming plasma outflows drive magnetic field amplification, plasma heating, and particle acceleration in numerous astrophysical environments, from supernova remnant shocks to active galactic nuclei jets. Understanding how, in the absence of Coulomb collisions, energy is redistributed between the different plasma species remains a fundamental open question. We use three-dimensional, fully kinetic simulations to investigate energy partition in weakly magnetized counterpropagating plasmas. Our results reveal a complex interplay between different processes, where at early times the Weibel instability drives a first stage of magnetic field amplification and at late times the kinking of current filaments drives a second amplification stage via a dynamo-type mechanism. Electrons are heated primarily during the latter phase through magnetic pumping. By the time the flows thermalize, we observe that the final temperature ratio T e /T i and energy partition depend on the ion-to-electron mass ratio. For electron–proton flows, the electron thermal energy only reaches up to a few percent of the initial ion kinetic energy.

Marret, Alexis [SLAC National Accelerator Laborato↗

Advanced Isotope Separation Technology for Fusion Fuel

Deuterium-tritium fusion is the easiest nuclear fusion reaction among known fusion reactions. Since tritium is extremely rare, it is artificially produced by irradiating lithium metal. The separation, isolation, and storage of the tritium isotope has been a major focus of the Savannah River Site (SRS) for many decades. Thermal diffusion, fractional absorption, and cryogenic distillation have all been used in the past, and each has significant operational and safety challenges. A process known as the Thermal Cycling Absorption Process (TCAP) was invented at SRS, and because of its overwhelming advantages in safety, efficiency, size, and reduced tritium inventory, it has replaced all other hydrogen isotope separation processes at SRS. Here, the working principles and current development of hydrogen isotope separation using TCAP at SRS are explained as a potential advanced isotope separation process for the fusion fuel cycle.

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↗

Use of computer vision for analysis of image datasets from high temperature plasma experiments

Great strides have been made in improving the quality of x-ray radiographs in high energy density plasma experiments, enabled in part by innovations in engineering and manufacturing of integrated circuits and materials. As a consequence, the radiographs of today are filled with a great deal of detail, but few of these features are extracted in a systematic way. Analysis techniques familiar to plasma physicists tend toward brittle 1D lineout or Fourier transform type analyses. The techniques applied to process our data have not kept pace with improvements in the quality of our data. Fortunately, the field of computer vision has a wealth of tools to offer, which have been widely used in industrial imaging and, more recently, adopted in biological imaging. We demonstrate the application of computer vision techniques to the analysis of x-ray radiographs from high energy density plasma experiments, as well as give a brief tutorial on the computer vision techniques themselves. These tools robustly extract 2D contours of shocks, boundaries of inhomogeneities, and secondary flows, thereby allowing for increased automation of analysis, as well as direct and quantitative comparisons with simulations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Design Considerations for Controlling Silicon Nanoparticle Nucleation and Growth in a Nonthermal Plasma

Controlling the nucleation and growth of nanoparticles in low temperature plasma systems is imperative for controlling nanoparticle size distributions; and for some applications such as deposition and etching in microelectronic processing, preventing particle contamination. In this work, silicon nanoparticle (NP) production from silane is used as a model system to investigate the nucleation process. Although the mechanisms responsible for silicon NP nucleation and growth have been studied, it is unclear how controllable system parameters (e.g., pressure, system geometry, and gas composition) can be used to inhibit or promote NP formation. For example, the transport of reactive silane species is expected to significantly affect the feed fraction of silane required to nucleate silicon NP (the nucleation onset fraction) due to losses at the reactor walls. In this work, NP mass density was determined as a function of system pressure, gas composition, and reactor diameter for a tubular flow-through radiofrequency (RF) plasma using Ar/H2/He/SiH4 gas mixtures. A quartz crystal microbalance (QCM) impactor was developed to measure the total aerosol mass density downstream of the plasma and thereby identify the nucleation onset and its dependence on process parameters. Finally, a reaction mechanism was developed and incorporated into a global plasma chemistry model to better understand the nucleation onset and NP growth.

36 MATERIALS SCIENCE↗

Propagation of positive discharges in an air bubble having an embedded water droplet

Low temperature plasmas generated inside gas bubbles immersed in water is an effective method of rapidly transferring plasma generated reactive species to the water for applications in biomedicine, agriculture and environment. Reactive species are generally produced in the gas phase plasma and then solvate into the liquid. The large surface-to-volume ratio (SVR) of the bubble accelerates this process. In generating bubbles in water, aerosols and droplets are also contained within the bubble. These droplets also have a large SVR and so can be rapidly plasma activated. However, the presence of the droplets can also impact the propagation of the plasma in the bubble. In this paper, results are discussed from computational and experimental investigations of the formation and evolution of discharges in an air bubble immersed in water with an embedded water droplet. The computations were performed with a two-dimensional plasma hydrodynamics model. Experiments were performed with a quasi-2D bubble apparatus. In bubbles having a droplet, a plasma filament typically bridges from the powered electrode to the droplet, and then from the droplet to the bubble surface. A surface-hugging streamer also occurs on the inner bubble surface and on the surface of the droplet. Both surface streamers result in part from surface charge accumulation and can dominate the formation of reactive species that transport into the droplet. Increasing droplet conductivity suppresses propagation of the surface discharge and leads to a lower density of aqueous reactive species. Increasing conductivity of the surrounding water does not change the overall structure of the discharge but does slightly elevate the discharge intensity. Finally, the size and shape of the embedded droplet can significantly affect the formation and propagation of the streamer.

2D fluid modelling↗

Partitioning of Radionuclides in Various Streams of the Mo-99 Purification Process

The Universal Neutron Irradiator (UNI) was designed to irradiate a small volume of uranium solution and to achieve high fission power without creating a large radionuclide (RN) inventory. The UNI system is equipped with a fully enclosed off-gas system with online hydrogen gas monitoring to prevent the production of an explosive atmosphere, as well as storage cylinders for capturing fission gases. It also includes a catalytic recombiner in the target capsule (to immediately recombine radiolytic hydrogen and oxygen gas in the system) and access ports for sampling the target solution and capsule headspace. In UNI Phase I experiments, 50 mL of uranyl sulfate solution was irradiated at 0.3–0.5 W/mL fission power using a tantalum target assembly to produce photoneutrons via irradiation with an electron beam. The purposes of the Phase I experiments were to test the efficacy of adding 200 ppm Fe 2+ to the target solution to prevent uranyl peroxide precipitation under representative irradiation conditions, and to monitor iodine speciation in the irradiated uranyl sulfate solution. The focus of the UNI Phase II experiments was to use an irradiated uranyl sulfate solution containing a mixture of fission products and monitor their distribution in various streams during the primary recovery column (titania-based column) that separates Mo-99 from uranium. Irradiations were designed to create sufficient activity for tracking their distribution in various processing streams using a combination of gamma counting and inductively coupled plasma mass spectrometry (ICP-MS) analyses. Obtained data will be used to better understand the composition of waste streams, accumulation of RN on the titania column, and identify what RNs accumulate in the uranyl sulfate solution. Furthermore, this knowledge will allow us to determine waste classifications for various streams produced during the Mo-99 purification process and develop an appropriate waste clean-up strategy.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Theoretical studies of chemical reactions related to the formation and growth of polycyclic aromatic hydrocarbons (PAH) and molecular properties of their key intermediates (Final Progress Report)

The formation mechanisms of polycyclic aromatic hydrocarbons, (PAHs) – organic molecules carrying fused benzene rings – are of great interest to scientists and engineers due to their importance in combustion chemistry and astrochemistry. On Earth, PAHs are largely produced in incomplete combustion of fossil fuel and are considered as critical precursors to unwanted soot particles leading to combustion inefficiency and causing air pollution along with detrimental health effects. Simple PAH molecules initially formed in the gas phase, are further involved in a build-up process in combustion flames leading to larger PAH, bowl-shaped nanostructures, fullerenes, and solid-phase species including carbonaceous dust, graphene particles, and soot. In deep space, PAH and their derivatives are potential key intermediates and nucleation sites leading eventually to carbonaceous nanoparticles (“interstellar grains”). Therefore, the understanding of the key processes in the synthesis of PAHs along with their precursors and their degradation mechanisms in combustion systems and in interstellar, circumstellar, and planetary atmospheric environments will provide critical insights into how complex aromatic structures, carbonaceous nanoparticles, and fullerenes are formed and destroyed. Achieving this understanding is an important step in the development of the efficient combustion processes and of the ecofriendly devices with reduced environmental pollution as well as technological strategies for the production of hydrogen and solid carbon through thermal or plasma-assisted pyrolysis of natural gas and biomass. Also, the understanding of the key processes of PAH and soot growth will help in our comprehension of chemical evolution in the universe. Detailed information on the mechanisms and reliable rate constants of the key elementary chemical reactions involved in PAH formation and destruction processes and in inception of soot particles is often missing, with the main deficiencies being the absence of temperature- and pressure-dependent rate constants for the broad range of conditions occurring in various terrestrial and interstellar processes and the lack of data on the reaction products and their branching ratios. Complementary to experimental studies, these gaps in knowledge can be filled by using quantum chemical calculations of reaction potential energy surfaces providing us with accurate energies of reaction products, intermediates, and transition states, revealing the reaction mechanism, and giving the molecular properties required to compute rate constants for relevant reaction steps and product branching ratios using the RRKM-Master Equation (ME) method. Molecular dynamics (MD) simulations can be used in cases when a reaction rate cannot be properly described by statistical theories. During the terminal renewal project period we employed these ab initio/RRKM-ME and MD approaches to complete our studies on several key reactions relevant to the formation/growth of PAH and inception of soot particles including (1) the reaction mechanism and kinetics of the resonance stabilized fulvenallenyl radical with propargyl and C 3 H 4 isomers; (2) the reaction mechanism and kinetics for the C + indene and C 2 + styrene reactions producing naphthyl or azulenyl radicals in low-temperature environments; (3) the MD study of non-equilibrium dimerization of acepyrene and coronene and its radical. The information derived from our theoretical calculations contributed to a better fundamental understanding of the reaction mechanisms and provide missing critical kinetic data to improve combustion models of hydrocarbon fuels and astrochemical models of the growth of carbonaceous molecules and particles in cold molecular clouds, circumstellar envelopes, and planetary atmospheres.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Powering the Future: Fusion & Plasmas

This report provides a decade-long vision for the field of fusion energy and plasma science and presents a path to a promising future of new scientific discoveries, industrial applications, and, ultimately, the delivery of fusion energy. We identify critical areas for research and development and prioritize investments to maximize impact. The research community worked for more than a year to develop a wealth of creative ideas designed to accelerate fusion energy and advance plasma science. The effort culminated in the consensus Community Planning Process report. Our work is based heavily on that report, and we extend our sincere gratitude to our colleagues for their efforts. Following the research community’s lead, we worked through consensus to generate this report. Many ideas were heard and were thoughtfully deliberated until a shared view on each issue emerged. This process allowed us to discuss and appreciate our different points of view and come to consensus language. Ultimately, we speak with one voice in conveying a vision for a vibrant program that will bring significant benefit to society.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Implementing a microphysics model in hydrodynamic simulations to study the initial plasma formation in dielectric ablator materials for direct-drive implosions

A microphysics model to describe the photoionization and impact ionization processes in dielectric ablator materials like plastic has been implemented into the 1-D hydrodynamic code LILAC for planar and spherical targets. Currently, the initial plasma formation during the early stages of a laser drive are modeled in an ad hoc manner, until the formation of a critical surface. Implementation of the physics-based models predict higher values of electron density, electron temperature, and pressure than the ad hoc model. Moreover, the numerical predictions are consistent with previous experimental observations of the shinethrough mechanism in plastic ablators. For planar targets, a decompression of the rear end of the target was observed, that is similar to recent experiments. An application of this model is to understand the laser-imprint mechanism that is caused by nonuniform laser irradiation due to single beam speckle.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Imaging plasma formation in isolated nanoparticles with ultrafast resonant scattering

We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Computing the Paschen curve for argon with speed-limited particle-in-cell simulation

Upon inclusion of collisions, the speed-limited particle-in-cell (SLPIC) simulation method successfully computed the Paschen curve for argon. The 1D3V simulations modeled an electron cascade across an argon-filled capacitor, including electron-neutral ionization, electron-neutral elastic collisions, electron-neutral excitation, and ion-induced secondary electron emission. In electrical breakdown, the timescale difference between ion and electron motion makes traditional PIC methods computationally slow. To decrease this timescale difference and speed up computation, here we used SLPIC, a time-domain algorithm that limits the speed of the fastest electrons in the simulation. The SLPIC algorithm facilitates a straightforward, fully kinetic treatment of dynamics and collisions. SLPIC was as accurate as PIC, but ran up to 200 times faster. SLPIC accurately computed the Paschen curve for argon over three orders of magnitude in pressure.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗