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NASA NTRS1983

Redshifts of high-temperature emission lines in the far-ultraviolet spectra of late-type stars

High-dispersion IUE spectra of six late-type stars exhibit small but statistically significant differential redshifts of high-temperature emission lines, like Si IV and C IV, with respect to low-temperature lines like S I and O I. A well-exposed, small-aperture spectrum of the active chromosphere binary Capella (Alpha Aurigae A: G6 II+F9 III) establishes that the high-temperature lines are redshifted in an absolute sense with respect to the accurately determined photospheric velocity of the system at single-line phase 0.50. Several possible explanations for the stellar redshifts are discused, including a warm wind (100,000 K) in which aparent redshifts are produced in optically thick lines by an accelerating outfow, and the downflowing component of a vertical circulation system for which the up-leg portion of the flow is too cool, too hot, or too tenuous to be visible in Si IV and C IV. If the second scenario is true, the stellar redshifts may provide an important phenomenological link to the downflows observed in 100,000 K species over magnetic active regions in the sun.

Ayres, T. R.↗
NASA NTRS1985

Solar He-3-rich events and nonrelativistic electron events - A new association

In 15 months of observation by the ISEE-e spacecraft, it was found that virtually all solar greater than or approximately equal to 1.3 MeV/nucleon He-3-rich events are associated with impulsive 2 to approximately 100 keV electron events, although many electron events were not accompanied by detectable He-3 increases. Both the He-3 and the electrons exhibit nearly scatter-free propagation in the interplanetary medium, and the times of onset and maximum for the He-3 and electron increases are closely related by velocity dispersion. The electron events and their related type III solar radio bursts provide, for the first time, identification of the flares which produce the He-3-rich events. He-3 appears to be accelerated at the flash phase of solar flares along with nonrelativistic electrons.

Reames, D. V.↗
NASA NTRS1991

A carrier-arraying demonstration at Goldstone for receiving Pioneer 11 signals

A carrier arraying technique was demonstrated at Goldstone. The Block III receivers of two 34-m antennas, Deep Space Station 12 and 15, were arrayed together to receive S band (2.3 GHz) signals from the Pioneer 11 spacecraft. Carrier phases in the two receivers were synchronized by the analog phase lock loops, and carrier signals were added at an intermediate frequency to enhance tracking performance. The receiver at DSS 15, which has been unable to lock up and track the Pioneer 11 signal by itself due to a wider tracking loop bandwidth and a higher system temperature, was now able to track the carrier and produce usable baseband signals. The receiver at DSS 12 achieved a reduction of the rms phase error, increasing the telemetry symbol SNR by an average of 0.35 dB. The baseband signals from both antennas were then synchronized and combined using the existing Baseband Assembly, thereby achieving a total symbol SNR increase of 2.5 + or - 0.7 dB relative to DSS 12 alone. A more comprehensive model is presented to permit evaluation of both thermal and phase noise effects. The analysis agrees well with observed data.

Pham, T. T.↗
NASA NTRS1991

Tomographic separation of composite spectra - The components of the O-star spectroscopic binary AO Cassiopeiae

The UV photospheric lines of the short-period, double-lined O-star spectroscopic binary AO Cas are analyzed. Archival data from IUE (16 spectra uniformly distributed in orbital phase) were analyzed with a tomography algorithm to produce the separate spectra of the two stars in six spectral regions. The spectral classifications of the primary and secondary, O9.5 III and O8 V, respectively, were estimated through a comparison of UV line ratios with those in spectral standard stars. An intensity ratio of 0.5-0.7 (primary brighter) at 1600 A is compatible with the data.

Bagnuolo, William G., Jr.↗
NASA NTRS1994

The early ultraviolet, optical, and radio evolution of the soft X-ray transient GRO J0422+32

We have monitored the evolution of the transient X-ray source GRO J0422+32 from approximately 2 weeks postdiscovery into its early decline phase at ultraviolet, optical, and radio wavelengths. Optical and ultraviolet spectra exhibit numerous, but relatively weak, high-excitation emission lines such as those arising from He II, N III, N V, and C IV superposed on an intrinsically blue continuum. High-resolution optical spectroscopy reveals line profiles which are double peaked, and in the case of the higher order Balmer lines, superposed on a broad absorption profile. The early outburst optical-ultraviolet continuum energy distribution is well represented by a two power-law fit with a break at approximately equal 4000 A. Radio observations with the Very Large Array (VLA) reveal a flat-spectrum source, slowly increasing in intensity at the earliest epochs observed, followed by an approximate power-law decay light curve with an index of -1. Light curves for each wavelength domain are presented and discussed. Notable are the multiple secondary outbursts seen in the optical more than 1 year postdiscovery, and spectral changes associated with secondary rises seen in the radio and UV. We find that the ultraviolet and optical characteristics of GRO J0422+32 as well as its radio evolution, are similar to other recent well-observed soft X-ray transients (also called X-ray novae) such as Cen X-4, A0620-00 (V616 Mon), and Nova Muscae 1991 (GS 1124-683), suggesting that GRO J0422+32 is also a member of that subclass of low-mass X-ray binaries. We present definitive astrometric determination of the source position, and place an upper limit of R approximately equals 20 from our analysis of the Palomar Observatory Sky Survey (POSS). Additionally, we derive distinct values for color excess from analysis of the optical (E(B-V) = 0.23) and ultraviolet (E(B-V) = 0.4) data, suggesting an intrinsic magnitude of 19-19.5 for the progenitor if it is mid-K dwarf. This leads to a likely range of 2.4-3.0 kpc for the source distance, which is consistent with our separate estimate of 2.4 +/- 0.4 kpc based on measurement of the NaD interstellar line profile. Adopting 2.4 kpc and E(B-V) = 0.23, the outburst absolute magnitude was M approximately equals 0.0, which is a typical value for this class of objects.

Shrader, C. R.↗
NASA NTRS2006

Lab-Scale Study of the Calcium Carbonate Dissolution and Deposition by Marine Cyanobacterium Phormidium subcapitatum

Suggestions that calcification in marine organisms changes in response to global variations in seawater chemistry continue to be advanced (Wilkinson, 1979; Degens et al. 1985; Kazmierczak et al. 1986; R. Riding 1992). However, the effect of [Na+] on calcification in marine cyanobacteria has not been discussed in detail although [Na+] fluctuations reflect both temperature and sea-level fluctuations. The goal of these lab-scale studies therefore was to study the effect of environmental pH and [Na+] on CaCO3 deposition and dissolution by marine cyanobacterium Phormidium subcapitatum. Marine cyanobacterium P. subcapitatum has been cultivated in ASN-III medium. [Ca2+] fluctuations were monitored with Ca(2+) probe. Na(+) concentrations were determined by the initial solution chemistry. It was found that the balance between CaCO3 dissolution and precipitation induced by P. subcapitatum grown in neutral ASN III medium is very close to zero. No CaCO3 precipitation induced by cyanobacterial growth occurred. Growth of P. subcapitatum in alkaline ASN III medium, however, was accompanied by significant oscillations in free Ca(2+) concentration within a Na(+) concentration range of 50-400 mM. Calcium carbonate precipitation occurred during the log phase of P. subcapitatum growth while carbonate dissolution was typical for the stationary phase of P. subcapitatum growth. The highest CaCO3 deposition was observed in the range of Na(+) concentrations between 200-400 mM. Alkaline pH also induced the clamping of P. subcapitatum filaments, which appeared to have a strong affinity to envelop particles of chemically deposited CaCO3 followed by enlargement of those particles size. EDS analysis revealed the presence of Mg-rich carbonate (or magnesium calcite) in the solution containing 10-100 mM Na(+); calcite in the solution containing 200 mM Na(+); and aragonite in the solution containing with 400 mM Na(+). Typical present-day seawater contains xxmM Na(+). Early (Archean) seawater was likely less saline. The division of marine cyanobacterium P. subcapitatum is associated with periodic deposition and dissolution of CaCO3, the rhythms and intensity of which are dependent on concentrations of both OH(-) and Na(+). Thus, the role of present-day marine cyanobacteria in the global carbonate cycle might be reduced to aggregation and recrystallization of available CaCO3 particles in marine water rather than long-term precipitation and accumulation of CaCO3 deposits. For lower Na(+) concentrations, precipitation of carbonates by cyanobacteria would be even less significant. These results suggest that the lack of calcified cyanobacteria in stromatalite-bearing Precambrian sequences can be explained not only by high dissolved inorganic carbon concentrations but also by lower salinity, as well as possible lower pH compared to present-day oceans.

Karakis, S. G.↗
NASA NTRS2016

Anomalous Temporal Behaviour of Broadband Ly Alpha Observations During Solar Flares from SDO/EVE

Although it is the most prominent emission line in the solar spectrum, there has been a notable lack of studies devoted to variations in Lyman-alpha (Ly-alpha) emission during solar flares in recent years. However, the few examples that do exist have shown Ly-alpha emission to be a substantial radiator of the total energy budget of solar flares (of the order of 10 percent). It is also a known driver of fluctuations in the Earth's ionosphere. The EUV (Extreme Ultra-Violet) Variability Experiment (EVE) on board the Solar Dynamics Observatory (SDO) now provides broadband, photometric Ly-alpha data at 10-second cadence with its Multiple EUV Grating Spectrograph-Photometer (MEGS-P) component, and has observed scores of solar flares in the 5 years since it was launched. However, the MEGS-P time profiles appear to display a rise time of tens of minutes around the time of the flare onset. This is in stark contrast to the rapid, impulsive increase observed in other intrinsically chromospheric features (H-alpha, Ly-beta, LyC, C III, etc.). Furthermore, the emission detected by MEGS-P peaks around the time of the peak of thermal soft X-ray emission and not during the impulsive phase when energy deposition in the chromosphere (often assumed to be in the form of non-thermal electrons) is greatest. The time derivative of Ly-alpha lightcurves also appears to resemble that of the time derivative of soft X-rays, reminiscent of the Neupert effect. Given that spectrally-resolved Ly-alpha observations during flares from SORCE / SOLSTICE (Solar Radiation and Climate Experiment / Solar Stellar Irradiance Comparison Experiment) peak during the impulsive phase as expected, this suggests that the atypical behaviour of MEGS-P data is a manifestation of the broadband nature of the observations. This could imply that other lines andor continuum emission that becomes enhanced during flares could be contributing to the passband. Users are hereby urged to exercise caution when interpreting broadband Ly-alpha observations of solar flares. Comparisons have also been made with other broadband Ly-alpha photometers such as PROBA2 (Project for On-Board Autonomy-2) / LYRA (Lyman Alpha Radiometer) and GOES (Geostationary Operational Environmental Satellite) / EUVE (Extreme Ultraviolet Explorer).

Milligan, Ryan O.↗
DOE OSTI2012

CONFINED POPULATION III ENRICHMENT AND THE PROSPECTS FOR PROMPT SECOND-GENERATION STAR FORMATION

It is widely recognized that nucleosynthetic output of the first Population III supernovae was a catalyst defining the character of subsequent stellar generations. Most of the work on the earliest enrichment was carried out assuming that the first stars were extremely massive and that the associated supernovae were unusually energetic, enough to completely unbind the baryons in the host cosmic minihalo and disperse the synthesized metals into the intergalactic medium. Recent work, however, suggests that the first stars may in fact have been somewhat less massive, with a characteristic mass scale of a few tens of solar masses. We present a cosmological simulation following the transport of the metals synthesized in a Population III supernova assuming that it had an energy of 10{sup 51} erg, compatible with standard Type II supernovae. A young supernova remnant is inserted in the first star's relic H II region in the free expansion phase and is followed for 40 Myr employing adaptive mesh refinement and Lagrangian tracer particle techniques. The supernova remnant remains partially trapped within the minihalo, and the thin snowplow shell develops pronounced instability and fingering. Roughly half of the ejecta turn around and fall back toward the center of the halo, with 1% of the ejecta reaching the center in {approx}30 kyr and 10% in {approx}10 Myr. The average metallicity of the combined returning ejecta and the pristine filaments feeding into the halo center from the cosmic web is {approx}0.001-0.01 Z{sub Sun }, but the two remain unmixed until accreting onto the central hydrostatic core that is unresolved at the end of the simulation. We conclude that if Population III stars had less extreme masses, they promptly enriched the host minihalos with metals and triggered Population II star formation.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Vapor–liquid equilibrium estimation of n-alkane/nitrogen mixtures using neural networks

Understanding fluid phase behavior, like VLE, in high P&T conditions is crucial for developing high-fidelity simulations of chemically reacting flows in liquid-fueled combustion systems and also forms an integral part of the design-modeling of the control processes in chemical industries. Two data-driven models have been proposed here in this study, each of which was competent in estimating VLE for the Type III binary systems of C 10 /N 2 and C 12 /N 2 , at pressures ranging up to 50–60 MPa. Both models showed better performance in predicting equilibrium pressure as compared to VLE modeled using PR-EOS. A modified model has also been proposed, capable of estimating the full phase envelope for the binary systems of C 10 /N 2 and C 12 /N 2 across a wide range of temperatures, and thus exhibit the mixture critical pressure at the concerned temperature. The diverse applicability of the proposed network architecture was further exhibited while estimating the VLE of a ternary system of C 1 /C 10 /N 2 .

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2026

Machine Learning–Augmented Laser-Induced Breakdown Spectroscopy for Spectral Discrimination of Iron Oxalates

Enhanced characterization and phase identification of post-PUREX Pu Oxalates (PuOXA) are pivotal for nonproliferation and pre-detonation nuclear forensics. Despite significant advances in the characterization of PuO 2 samples, little is known about the impact of both the chemical structure and oxidation states of PuOXA (i.e., Pu(III) and Pu(IV)) have on optical emission signatures. Here, we demonstrate the analytical capabilities of laser-induced breakdown spectroscopy (LIBS) applied to Fe(II) and Fe(III) oxalate samples as surrogates for PuOXA, highlighting the discriminating features in the LIBS emission spectra arising from differences in the oxidation states within mixed FeOXA samples. We report the enhancement of spectral feature selection using Principal Component Analysis (PCA), which enables the analytical superiority of machine learning algorithms such as Linear Discriminant Analysis (LDA), Quadratic Discriminant Analysis (QDA), Partial Least Squares Regression (PLSR), Support Vector Regression (SVR), and Random Forest Regression (RFR) over conventional univariate techniques for phase discrimination and chemometric analysis. Cluster analysis revealed how both matrix effects and laser ablation influence cluster separability by introducing spectral artifacts that misdirect the maximization of variance. PCA-selected emission lines were used in the regression models, demonstrating that both univariate and multivariate linear regression models (i.e., PLSR and SVR) can achieve acceptable performance, with machine learning models outperforming conventional calibration regressions. Furthermore, the application of non-linearly activated PCA-selected emission lines illustrates how simplifying the data while retaining captured variance enables the use of less complex and more computationally efficient models. Furthermore, this is particularly evident in the underperformance of RFR, which suffers from increased computational costs and overfitting owing to its high complexity.

Oxalates↗
DOE OSTI2016

Gaussian-windowed frame based method of moments formulation of surface-integral-equation for extended apertures

Scattering or coupling of electromagnetic beam-field at a surface discontinuity separating two homogeneous or inhomogeneous media with different propagation characteristics is formulated using surface integral equation, which are solved by the Method of Moments with the aid of the Gabor-based Gaussian window frame set of basis and testing functions. The application of the Gaussian window frame provides (i) a mathematically exact and robust tool for spatial-spectral phase-space formulation and analysis of the problem; (ii) a system of linear equations in a transmission-line like form relating mode-like wave objects of one medium with mode-like wave objects of the second medium; (iii) furthermore, an appropriate setting of the frame parameters yields mode-like wave objects that blend plane wave properties (as if solving in the spectral domain) with Green's function properties (as if solving in the spatial domain); and (iv) a representation of the scattered field with Gaussian-beam propagators that may be used in many large (in terms of wavelengths) systems.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Effect of HEH[EHP] impurities on the ALSEP solvent extraction process

In solvent extraction processes, organic phase impurities can negatively impact separation factors, hydrolytic performance, and overall system robustness. The resulting inconsistent performance can affect the process-level viability of a separation concept, and thus knowledge of the impurities present, their effects on the process, and how to remove them are vital. Deleterious impurities may be introduced into a system from reagent synthesis, or result from degradation via radiolysis and hydrolysis during use. In this work, the acidic extractant, 2-ethylhexylphosphonic acid mono-2-ethylhexyl ester (HEH[EHP])—proposed for application in extractive processes aimed at separating trivalent minor actinides from lanthanides and other fission products—is characterized with respect to its common impurities and their impact on Am(III) stripping in the Actinide Lanthanide SEParation (ALSEP) system. Furthermore, to control impurities in HEH[EHP], existing purification technologies commonly applied for the acidic organophosphorus reagent were assessed and a new chromatographic purification method specific to HEH[EHP] is presented.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Effect of Precursor Selection on the Photocatalytic Performance of Indium Oxide Nanomaterials for Gas-Phase CO 2 Reduction

Nonstoichiometric indium oxide nanoparticles, In 2 O 3–x (OH)y, have been shown to function as active photocatalysts for gas-phase CO 2 reduction under simulated solar irradiation. We demonstrate that the choice of starting material has a strong effect on the photocatalytic activity of indium oxide nanoparticles. We also examine three indium oxide materials prepared via the thermal decomposition of either indium(III) hydroxide or indium(III) nitrate and correlate their stability and photocatalytic activity to the number and type of defect present in the material. Furthermore, we use 13CO 2 isotope-tracing experiments to clearly identify the origins of the observed carbon-containing products. Significantly, we find that the oxidizing nature of the precursor anion has a substantial impact on the defect formation within the sample. Our study demonstrates the importance of surface defects in designing an active heterogeneous photocatalyst and provides valuable insight into key parameters for the precursor design, selection, and performance optimization of materials for gas-phase CO 2 reduction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Dual Tunability for Uncatalyzed N‐Alkylation of Primary Amines Enabled by Plasma‐Microdroplet Fusion

Abstract The fusion of non‐thermal plasma with charged microdroplets facilitates catalyst‐free N‐alkylation for a variety of primary amines, without halide salt biproduct generation. Significant reaction enhancement (up to >200×) is observed over microdroplet reactions generated from electrospray. This enhancement for the plasma‐microdroplet system is attributed to the combined effects of energetic collisions and the presence of reactive oxygen species (ROS). The ROS (e.g., O 2 ⋅ − ) act as a proton sink to increase abundance of free neutral amines in the charged microdroplet environment. The effect of ROS on N‐alkylation is confirmed through three unique experiments: (i) utilization of radical scavenging reagent, (ii) characterization of internal energy distribution, and (iii) controls performed without plasma, which lacked reaction acceleration. Establishing plasma discharge in the wake of charged microdroplets as a green synthetic methodology overcomes two major challenges within conventional gas‐phase plasma chemistry, including the lack of selectivity and product scale‐up. Both limitations are overcome here, where dual tunability is achieved by controlling reagent concentration and residence time in the microdroplet environment, affording single or double N‐alkylated products. Products are readily collected yielding milligram quantities in eight hours. These results showcase a novel synthetic strategy that represents a straightforward and sustainable C−N bond‐forming process.

Chemistry↗
DOE OSTI2023

Pore connectivity influences mass transport in natural rocks: Pore structure, gas diffusion and batch sorption studies

For this work, six rocks (one granodiorite, one limestone, two chalks, one mudstone, and one dolostone) with different extents of heterogeneity at six different particle sizes (from 75 to 8000 μm) were studied to describe the effects of pore connectivity on mass transport. The methods applied were (i) porosity measurement of granular rocks, (ii) analyses of gas-phase diffusive transport in a bed of packed particles, along with a solid quartz method at these six particle sizes being developed to identify the contribution of intraparticle diffusion, and (iii) batch sorption tests of multiple ions (anions and cations) with subsequent analyses of inductively coupled plasma-mass spectrometry. Granular porosity measurement results reveal that with decreasing particle sizes, the effective porosities for the “heterogenous” group of rocks (Grimsel granodiorite and Edwards limestone) increase, whereas the porosities of another “homogeneous” group (two Israel chalk samples, Japan mudstone, and Wyoming dolostone) remain constant. Gas diffusion results show that the intraparticle gas diffusion coefficient among these two sample groups, varying in the magnitude of 10 -8 to 10 -6 m 2 /s, are not directly correlated to the porosity differences. Moreover, the batch sorption work displays a different affinity of rocks for various tracers. For Grimsel granodiorite, Japan mudstone, and Wyoming dolostone, the adsorption capacity of Sm 3+ and Eu 3+ increases as the particle size decreases. In general, this integrated research of grain size distribution, granular rock porosity, intraparticle diffusivity, and ionic sorption capacity gives insights into the pore connectivity effect on both physical and chemical transport behaviors for different lithologies and/or different particle sizes.

58 GEOSCIENCES↗
DOE OSTI2012

The effect of electron beam pitch angle and density gradient on solar type III radio bursts

1.5D particle-in-cell simulations of a hot, low density electron beam injected into magnetized, maxwellian plasma were used to further explore the alternative non-gyrotropic beam driven electromagnetic (EM) emission mechanism, first studied in Tsiklauri, Phys. Plasmas 18, 052903 (2011). Variation of beam injection angle and background density gradient showed that the emission process is caused by the perpendicular component of the beam injection current, whereas the parallel component only produces Langmuir waves, which play no role in the generation of EM waves in our mechanism. Particular emphasis was put on the case, where the beam is injected perpendicularly to the background magnetic field, as this turned off any electrostatic wave generation along the field and left a purely electromagnetic signal in the perpendicular components. The simulations establish the following key findings: (i) Initially, waves at a few {omega}{sub ce}/{gamma} are excited, mode converted and emitted at Almost-Equal-To {omega}{sub pe} (ii) The emission intensity along the beam axis is proportional to the respective component of the kinetic energy of the beam; (iii) The frequency of the escaping EM emission is independent of the injection angle; (iv) A stronger background density gradient causes earlier emission; (v) The beam electron distribution function in phase space shows harmonic oscillation in the perpendicular components at the relativistic gyrofrequency; (vi) The requirement for cyclotron maser emission, ({partial_derivative}f/{partial_derivative}v{sub Up-Tack })>0, is fulfilled; (vii) The degree of linear polarization of the emission is strongly dependent on the beam injection angle; (viii) The generated electromagnetic emission is left-hand elliptically polarized as the pitch angle tends to 90 Degree-Sign ; and (ix) The generated electromagnetic energy is of the order of 0.1% of the initial beam kinetic energy.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Spatio-temporal ablation dynamics and plasma chemistry of aluminum induced by temporally modulated ytterbium fiber laser

Here, in this work, we studied single-pulse ablation dynamics of a temporally modulated continuous wave laser-material interaction with Al using in situ multimodal time-resolved diagnostics that describe in detail the associated physical and chemical processes. Time-resolved scattering, emission imaging, and optical emission spectroscopy unveiled a sequence of events spread out across three distinct phases: (i) early phase ablation process, associated with particle generation and liquid Al column formation (<20 μs), (ii) secondary detonation when sufficient ejected material is accumulated over the surface (20-50 μs), and (iii) molten liquid Al pool oscillation on the surface, followed by large droplet ejection from the liquid pool (100-500 μs). Atomic Al and AlO were observed with optical emission spectroscopy at different ratios during the entire lifetime of the event, verifying the formation of oxidized Al vapor upon its interaction with air. Morphological and compositional characterization confirmed surface oxidation and material re-solidification in the form of protrusions produced during the irradiation process. This work provides insights into the complex physical and chemical mechanisms of single-pulse ablation in the sub-millisecond laser pulse regime, which are critically important for parameter optimization in a variety of laser processing, microfabrication, and deposition applications.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗