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DOE OSTI2023

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↗

NASA NTRS1990

Radiative shocks and nonequilibrium chemistry in the early universe - Galaxy and primordial star formation

The nonequilibrium radiative cooling, recombination, and molecule formation behind steady-state shock waves in primordial composition gas is studied. The hydrodynamical conservation equations are solved as well as equations for nonequilibrium ionization, recombination, and molecule formation and the equation of radiative transfer. The shocked gas is found to cool faster than it can recombine; as a result it is able to form an H2 concentration as high as 0.001 or higher via the formation of H(-) and H2(+) intermediaries due to the enhanced nonequilibrium ionization at 10,000 K. With such an H2 concentration, the gas cools by rotational-vibrational line excitation of H2 molecules to well below the canonical final temperature of 10,000 K for a molecule-free gas without metals. It is shown that, as the level of external ionizing and dissociating radiation flux is increased, the formation of and cooling by H2 molecules can be inhibited and delayed.

Shapiro, Paul R.↗

NASA NTRS1999

Rocket/Radar Sporadic-E Experiment Conducted during the El Coqui 2 Campaign

In order to investigate the complex electrodynamics and neutral-plasma coupling inherent to sporadic-E layers in the earth's mid-latitude ionosphere, a series of rocket/radar experiments were planned as part of the NASA El Coqui H Campaign from Tortuguero Launch Range, Puerto Rico, in March-April, 1998. The rocket experiments consisted of two pairs of "mother-daughter" payloads with limited apogees so that the payloads "hovered" in the sporadic-E region (95-125 km). Each payload pair included vector DC and AC electric field detectors, a highly accurate flux-gate DC magnetometer, an ion mass spectrometer, an ionization gauge, and spaced-electric field receivers to measure the wavelength and phase velocity of the unstable plasma waves. Separate rockets were included to simultaneously carry aloft TMA trails to measure the neutral wind and its velocity shear, believed responsible for the sporadic-E layer formation. In addition to the rocket experiments, incoherent scatter radar measurements of plasma density and drift velocity were gathered almost every night during the 3 week campaign. Continuous VHF backscatter radar operations were carried out from a site near Salinas, Puerto Rico, where 3-m backscatter echoes were observed associated with sporadic-E and other types of low altitude ionospheric layers. Other radars that operated during the campaign included an HF backscatter system near Ponce, Puerto Rico, and a second VHF backscatter radar set up near Aguadila Puerto Rico. On 24 March 1998, one of the instrumented rockets was launched, attaining an apogee of 129 km. The payloads successfully pierced an intense sporadic-E layer observed by both the Arecibo radar and the in-situ density and ion mass spectrometer probes. In-situ DC electric fields revealed very low (about 1-2 mV/m) ambient fields with small amplitude structures of the same order. No high frequency (short scale) waves were observed, consistent with the VHF backscatter observations at the time of the launch. An overview of the observations will be presented.

Pfaff, R.F.↗

NASA NTRS2012

Water in Pyroxene and Olivine from Martian Meteorites

Water in the interior of terrestrial planets can be dissolved in fluids or melts and hydrous phases, but can also be locked as protons attached to structural oxygen in lattice defects in nominally anhydrous minerals (NAM) like olivine, pyroxene, or feldspar [1-3]. Although these minerals contain only tens to hundreds of ppm H2O, this water can amount to at least one ocean in mass when added at planetary scales because of the modal dominance of NAM in the mantle and crust [4]. Moreover these trace amounts of water can have drastic effects on melting temperature, rheology, electrical and heat conductivity, and seismic wave attenuation [5]. There is presently a debate on how much water is present in the martian mantle. Secondary ionization mass spectrometry (SIMS) studies of NAM [6], amphiboles and glass in melt inclusions [7-10], and apatites [11, 12] from Martian meteorites report finding as much water as in the same phases from Earth's igneous rocks. Most martian hydrous minerals, however, generally have the relevant sites filled with Cl and F instead of H [13, 14], and experiments using Cl [15] in parent melts can reproduce Martian basalt compositions as well as those with water [16]. We are in the process of analyzing Martian meteorite minerals by Fourier transform infrared spectrometry (FTIR) in order to constrain the role of water in this planet s formation and magmatic evolution

Peslier, A. H.↗

NASA NTRS2022

Extreme Poleward Expanding Super Plasma Bubbles Over Asia-Pacific Region Triggered By Tonga Volcano Eruption During the Recovery-Phase of Geomagnetic Storm

The Tonga volcano eruption of 15 January 2022 unleashed a variety of atmospheric perturbations, coinciding with the recovery-phase of a geomagnetic storm. The ensuing thermospheric variations created rare display of extreme poleward-expanding conjugate plasma bubbles seen in the rate of total electron content index over 100–150°E, reaching ∼40°N geographic latitude. This is associated with fluctuations in FORMOSAT-7/COSMIC-2 (F7/C2) ion-density measurements and spread-F in ionograms. Preceding to this, an unusually strong pre-reversal enhancement (PRE) occurred in the global ionospheric specification (GIS) electron density profiles derived from F7/C2 observations. The GIS also revealed a decrease of equatorial ionization anomaly (EIA) crest density due to the storm impact. Reduced E-region conductivity by volcano-induced waves and enhanced F-region wind, further accelerated by reduced ion-drag over the EIA, apparently intensified the PRE. Accompanied with the strong PRE, volcano-induced seed perturbations triggered the super plasma bubble activity.

P. K. Rajesh↗

DOE OSTI2021

Gravito-turbulence and dynamo in poorly ionized protostellar discs – I. Zero-net-flux case

In their early stages, protoplanetary discs are sufficiently massive to undergo gravitational instability (GI). This instability is thought to be involved in mass accretion, planet formation via gas fragmentation, the generation of spiral density waves, and outbursts. A key and very recent area of research is the interaction between the GI and magnetic fields in young protoplanetary discs, in particular whether this instability is able to sustain a magnetic field via a dynamo. We conduct 3D, stratified shearing-box simulations using two independent codes, PLUTO and Athena++, to characterize the GI dynamo in poorly ionized protostellar discs subject to ambipolar diffusion. We find that the dynamo operates across a large range of ambipolar Elssaser number Am (which characterizes the strength of ambipolar diffusion) and is particularly strong in the regime Am = 10–100, with typical magnetic to thermal energy ratios of order unity. The dynamo is only weakly dependent on resolution (at least for Am ≲ 100), box size, and cooling law. The magnetic field is produced by the combination of differential rotation and large-scale vertical roll motions associated with spiral density waves. Our results have direct implications for the dynamo process in young protoplanetary discs and possibly some regions of active galactic nucleus discs.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

Coherent electronic-vibrational dynamics in deuterium bromide probed via attosecond transient-absorption spectroscopy

Ultrafast laser excitation can trigger multiplex coherent dynamics in molecules. Here, we report attosecond transient-absorption experiments addressing simultaneous probing of electronic and vibrational dynamics in a prototype molecule, deuterium bromide (DBr), following its strong-field ionization. Electronic and vibrational coherences in the ionic X$^2\Pi_{3/2}$ and X$^2\Pi_{1/2}$ states are characterized in the Br-$3d$ core-level absorption spectra via quantum beats with 12.6-fs and 19.9-fs periodicities, respectively. Polarization scans reveal that the phase of the electronic quantum beats depends on the probe direction, experimentally showing that the coherent electronic motion corresponds to the oscillation of the hole density along the ionization-field direction. The vibrational quantum beats are found to maintain a relatively constant amplitude, whereas the electronic quantum beats exhibit a partial decrease in time. Quantum wave-packet simulations show that the decoherence effect from the vibrational motion is insignificant because of the parallel relation between the X$^2\Pi_{3/2}$ and X$^2\Pi_{1/2}$ potentials. Finally, a comparison between the DBr and HBr results suggests that rotation motion is responsible for the decoherence since it leads to initial alignment prepared by the strong-field ionization.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS1997

Data Base for CFD Validation

The flow behind the shock wave formed around objects which fly at hypervelocity behaves differently from that of a perfect gas. Molecules become vibrationally excited, dissociated, and ionized. The hot gas may emit or absorb radiation. When the atoms produced by dissociation reach the wall surface, chemical reactions, including recombination, may occur. The thermochemical phenomena of vibration, dissociation, ionization, surface chemical reaction, and radiation are referred to commonly as high-temperature real-gas phenomena. The phenomena cause changes in the dynamic behavior of the flow and the surface pressure and heat transfer distribution around the object. The character of a real gas is described by the internal degrees of freedom and state of constituent molecules; nitrogen and oxygen for air. The internal energy states, rotation, vibration and electronic, of the molecules are excited and, in the limit, the molecular bonds are exceeded and the gas dissociated into atomic and, possibly, ionic constituents. The process of energy transfer causing excitation, dissociation and recombination is a rate process controlled by particle collisions. Binary, two-body, collisions are sufficient to cause internal excitation, dissociation and ionization while three-body collisions are required to recombine the particles into molecular constituents. If the rates of energy transfer are fast with respect to the local fluid dynamic time scale the gas is in, or nearly in, equilibrium. If the energy transfer rates are very slow the gas can be described as frozen. In all other instances, wherein any of the energy exchange rates are comparable to the local fluid time scale, the gas will be thermally or chemically reacting and out of equilibrium. Real gas thermochemical nonequilibrium processes are important in the determination of aerodynamic heating; both convective (including wall catalytic effects) and radiative heating. To illustrate this we consider the hypervelocity flow over a bluff body typical of an atmospheric entry vehicle or an aerospace transfer vehicle (ASTV). The qualitative aspects of a hypersonic flow field over a bluff body are discussed in two parts, forebody and afterbody, with attention to which particular physical effects must be included in an analysis. This will indicate what type of numerical modeling will be adequate in each region of the flow. A bluff forebody flow field is dominated by the presence of the strong bow shock wave and the consequent heating, and chemical reaction of the gas. At high altitude hypersonic flight conditions the thermal excitation and chemical reaction of the gas occur slowly enough that a significant portion of the flow field is in a state of thermochemical nonequilibrium. A second important effect is the presence of the thick boundary layer along the forebody surface. In this region there are large thermal and chemical species gradients due to the interaction of the gas with the wall. Also at high altitudes the shock wave and the boundary layer may become so thick that they merge; in this case the entire shock layer is dominated by viscous effects.

Deiwert, George S.↗

NASA NTRS1988

Upper hybrid and Langmuir turbulence in the auroral E region

Oscillations at a frequency between the local upper hybrid and plasma frequencies have been detected in the upper E region of the morning auroral oval. The emission occurs in a narrow band of frequencies when the dipole antenna is nearly perpendicular to B but broadens when the antenna has a component parallel to B. The waves have a low-altitude cutoff at about 125-130 km, and their intensity increases in regions of low plasma density. No theoretical explanation yet exists for these waves, which may be the manifestation of a plasma instability process due to the suprathermal electron flux which accompanies collisional ionization in the auroral E region.

Kelley, Michael C.↗

NASA NTRS1988

A magnetic loop model for structure and activity in the Galactic center

A simple model for the production and propagation of magnetized loops in the Galactic center is developed. It is found that a magnetized model can reproduce the filamentary, asymmetric structures on all scales from 100 pc to subparsec scales in the Galactic center. The radio and molecular gas morphology on all scales inside the Galactic center lobe may be explained in terms of the expansion of strongly magnetized loops and their interaction with the 2-5 pc torus and 30-50 pc portion of the center lobe. The magnetic loops have a toroidal field which explains the braided appearance of the radio continuum emission on the 2 pc scale. The barlike feature on the 2 pc radio continuum maps can be viewed as a piece of a magnetic loop with field strength about 0.01 G which is colliding and reconnecting with the ionized inner edge of the 2 pc molecular torus. The loop-torus interaction feeds energetic particles and shear Alfven waves into the torus, and deposits mass and energy.

Heyvaerts, Jean↗

NASA NTRS1998

X-Ray Emission from Protostellar Jets

The goals of this program were to identify the termination shocks in several parsec-scale protostellar jets through the thermal soft X-rays emitted by the high-velocity terminal shock waves, and to assess the impact these outflows have on the surrounding interstellar and intercloud medium. The terminal shock waves that plow into the undisturbed interstellar medium may have shock velocities commensurate with the observed space motions of several hundred km s(exp -1). Such shocks will heat and ionize the interstellar medium, perhaps creating large ovoid bubbles of hot gas. Identifying the location of the terminal shocks in these outflows would also allow us to place constraints on the ages of these outflows, and hence the duration of the mass-loss phase that accompanies the formation of a star. We targeted four outflows where the outer optical shock waves are projected against low-extinction backgrounds. From the two dozen or so parsec-scale flows known, we chose those that have the highest velocities, brightest optical counterparts, and/or the richest concentration of shock waves in a small area on the sky. Four giant HH flows have been observed with the ROSAT HRI at Priority A for 30 ksec each. Results: Unfortunately, we failed to detect X-ray emission from the terminal bow shocks of the giant HH flows using the ROSAT HRI. The reasons are likely to be: (1) The shock velocities may be too low to emit in the soft X-rays. (2) The sensitivity of the HRI is too low to detect the diffuse emission. The fields that we observed were chosen to be low extinction sight-lines, with the consequence that the tenuous media into which the outer bow shocks are propagating produce low fluxes. Despite the failure to achieve the primary science goals, we have identified in each image a half a dozen or so point-source young stellar objects. The HRI images have been very useful for discerning potential outflow sources and are being combined with optical, near-IR, and radio imaging data of each outflow field. The first paper on L1551 NE is currently in preparation.

Morse, Jon A.↗

NASA NTRS1984

s-wave threshold in electron attachment - Results in 2-C4F6 and CFCl3 at ultra-low electron energies

Electron attachment lineshapes and cross sections are reported for the processes 2-C4F6(-)/2-C4F6 and Cl(-)/CFCl3 at electron energies of 0-120 and 0-140 meV, and at resolutions of 6 and 7 meV (FWHM), respectively. As in previous measurements in CCl4 and SF6, the results show resolution-limited narrow structure in the cross section at electron energies below 15 meV. This structure arises from the divergence of the s-wave cross section in the limit of zero electron energy. Comparisons are given with swarm-measured results, and with collisional ionization (high-Rydberg attachment) data in this energy range.

Chutjian, A.↗

NASA NTRS1988

Ionization of K-shell electrons by highly relativistic protons

A comparative study of three theoretical formalisms by Anholt et al. (1976), Scofield (1978), and Becker et al. (1985) for K-shell ionization by highly relativistic protons has been carried out. The importance of the spin-flip mechanism is emphasized. It is concluded that in the analysis of such inner-shell ionization processes, an accurate description of the projectile-target interaction is of much more significance than the accuracy of the wave functions of the atomic electrons.

Rustgi, M. L.↗

NASA NTRS1990

SPEAR-1: An experiment to measure current collection in the ionosphere by high voltage biased conductors

An experiment is described in which a high electrical potential difference, up to 45 kV, was applied between deployed conducting spheres and a sounding rocket in the ionosphere. Measurements were made of the applied voltage and the resulting currents for each of 24 applications of different high potentials. In addition, diagnostic measurements of optical emissions in the vicinity of the spheres, energetic particle flow to the sounding rocket, dc electric field and wave data were made. The ambient plasma and neutral environments were measured by a Langmuir probe and a cold cathode neutral ionization gauge, respectively. The payload is described and examples of the measured current and voltage characteristics are presented. The characteristics of the measured currents are discussed in terms of the diagnostic measurements and the in-situ measurements of the vehicle environment. In general, it was found that the currents observed were at a level typical of magnetically limited currents from the ionospheric plasma for potentials less than 12 kV, and slightly higher for larger potentials. However, due to the failure to expose the plasma contactor, the vehicle sheath modified the sphere sheaths and made comparisons with the analytic models of Langmuir-Blodgett and Parker-Murphy less meaningful. Examples of localized enhancements of ambient gas density resulting from the operation of the attitude control system thrusters (cold nitrogen) were obtained. Current measurements and optical data indicated localized discharges due to enhanced gas density that reduced the vehicle-ionosphere impedance.

Raitt, W. John↗

DOE OSTI2022

On the choice of reference orbitals for linear-response calculations of solution-phase K-edge X-ray absorption spectra

The simplest response theory methods for computing vertical excitation spectra in condensed-phase are configuration interaction with single excitations (CIS) and linear-response time-dependent density functional theory (TDDFT) within the Tamm–Dancoff approximation. In applications to X-ray absorption spectroscopy (XAS), methods like CIS and TDDFT that codify only single excitations into the wave function are prone to catastrophic errors in main-edge and post-edge features whose shapes act as a crucial fingerprint in structural analyses of liquids. Here, we show that these errors manifest primarily due to a lack of orbital relaxation in conventional linear-response theories and that core-ionized (n - 1-electron) references, like those of electron-affinity TDDFT, can eliminate the errors in the spectral profile, even in the highest-energy parts of the post-edge. Crucially, we find that single excitations atop core-ionized references are sufficient to elucidate liquid-phase XAS spectra with semi-quantitative accuracy, opening the door for methods like electron-affinity CIS/TDDFT to be used as efficient alternatives to higher-order wave function approaches.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Covalency in Fe 2 O 3 and FeO: Consequences for XPS satellite intensity

The covalent character of the interaction between the metal cation and the oxygen ligands has been examined for two Fe oxides with different nominal oxidation states, Fe(II)O, and Fe(III) 2 O 3 . The covalent character is examined for the initial, ground state configuration and for the ionic states involving the removal of a shallow core, Fe 3p, and a deep core, Fe 2p, electron. The covalency is assessed based on novel theoretical analyses of wave functions for the various cases. It is found that the covalency is considerably different for different oxidation states and for different ionized and non-ionized configurations. The changes in covalency for the ions are shown to be responsible for important changes in relaxation energies for X-Ray Photoelectron Spectroscopy (XPS) spectra and in the intensity lost from main XPS peaks to shake satellites. While these consequences are not observables themselves, they are important for the interpretation of the XPS spectra, in particular, for efforts to extract stoichiometries of these iron oxides from XPS data. This is a finding likely applicable across various 3d transition metal oxide materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1970

Theoretical study of a plasma accelerator

Two-dimensional unsteady flow established in an electrodeless traveling wave plasma accelerator was theoretically analyzed to help explain, and possibly predict, phenomena appearing during experiments on problems of acceleration of an ionized fluid plasma.

Peyret, R.↗

NASA NTRS1978

Strange doings on Io

Some unusual properties of Io are discussed, and possible explanations for these are considered. The properties discussed include Io's ability to modify radio waves emitted by Jupiter in the decametric band, the satellite's ionosphere and sodium cloud, its extraordinary brightness, and the presence of ionized sulfur just inside the satellite's orbit. Io's ability to modulate Jovian decametric radio emission is explained on the basis of the hypothesis that the satellite conducts electricity and interacts with Jupiter's magnetic field. Characteristics of the sodium cloud are reviewed, and the probable mechanism responsible for this cloud is outlined. It is concluded that the only plausible explanation for the brightness of Io is the presence of cat's-eye-type reflectors, possibly composed of crystalline deposits, on the satellite's surface.

Goody, R.↗