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DOE OSTI2021

Photoacoustic 3-D imaging of polycrystalline microstructure improved with transverse acoustic waves

Non-invasive fast imaging of grain microstructure of polycrystalline ceria with sub-micrometric spatial resolution is performed via time-domain Brillouin scattering. The propagation of a nanoacoustic pulse is monitored down to 8 µm deep in a 30 × 30 µm2 area. Grains boundaries are reconstructed in three-dimensions via a twostep processing method, relying on the wavelet synchro-squeezed transform and the alpha shape algorithm. Imaging contrast is improved by taking advantage of stronger sensitivity to anisotropy of transverse acoustic waves, compared with longitudinal waves. Utilization of transverse waves in the image processing reveals additional boundaries that are not discerned using longitudinal waves, confirmed by an electron backscattering diffraction pattern. A buried inclined interface between differently oriented grains is identified by monitoring changes in amplitude (phase) of the portion of the signal associated with transverse (longitudinal) waves. Estimates of the inclination angle of this interface prove the sensitivity of our laser ultrasonic method to image inclined boundaries.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Real-time monitoring of trace noble gases using laser-induced breakdown spectroscopy—An investigation of the impact of bulk gas on plasma properties and sensitivity

The impact of Ar and He bulk gases on laser-induced breakdown spectroscopy (LIBS) real-time monitoring of trace Xe and Kr was assessed. LIBS is being developed as a monitoring tool for measuring noble gas transport in molten salt systems, in which traditional sensors may face challenges associated with radiation, corrosive materials, and/or mixed phases. The plasma temperature and electron densities of LIBS plasmas were measured in both static and various flowing Ar and He streams (0–5 L min −1 ). The use of an Ar bulk gas resulted in higher plasma temperature, greater electron densities by an order of magnitude, and extended plasma lifetime compared with when He bulk gas was used. Gas flow rate was found to have little impact on plasma temperature; however, its effect on electron density was significant, indicating the need to consider flow rate–specific models. Matrix effects on emission peaks were reported for both bulk gases. Due to these matrix effects, multivariate models were developed for Xe and Kr ranging from 0 to 700 ppm in both bulk gases. Although the predictive behavior was similar (root mean square error of prediction ranging from 11.1 to 20.6 ppm), the limits of detection were superior in He (Xe: 22.9 ppm, Kr: 30.4 ppm). Furthermore, these models were employed in demonstrative real-time tests (>1 h), which showed strong predictive precision (relative standard deviation <5 %) regardless of the bulk gas. Ultimately, this study provides a guide for the considerations required when developing gaseous LIBS models for real-time monitoring.

Gas flow effects↗

DOE OSTI2022

Electron-Beam Induced Emergence of Mesoscopic Ordering in Layered MnPS 3

Ordered mesoscale structures in 2D materials induced by small misorientations have allowed for a wide variety of electronic, ferroelectric, and quantum phenomena to be explored. Until now, the only mechanism to induce this periodic ordering was via mechanical rotations between the layers, with the periodicity of the resulting moiré pattern being directly related to twist angle. Here we report a fundamentally distinct mechanism for emergence of mesoscopic periodic patterns in multilayer sulfur-containing metal phosphorus trichalcogenide, MnPS3, induced by the electron beam. The formation under the beam of periodic hexagonal patterns with several characteristic length scales, nucleation and transitions between the phases, and local dynamics are demonstrated. The associated mechanisms are attributed to the relative contraction of the layers caused by beam-induced sulfur vacancy formation with subsequent ordering and lattice parameter change. As a result, the plasmonic response of the system is locally altered, suggesting an element of control over plasmon resonances by electron beam patterning. To conclude, we pose that harnessing this phenomenon provides both insight into fundamental physics of quantum materials and enables device applications by enabling controlled periodic potentials on the atomic scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Scaling behavior of low-temperature orthorhombic domains in the prototypical high-temperature superconductor La 1.875 Ba 0.125 CuO 4

Structural symmetry breaking and recovery in condensed-matter systems are closely related to exotic physical properties such as superconductivity (SC), magnetism, spin density waves, and charge density waves (CDWs). The interplay between different order parameters is intricate and often subject to intense debate, as in the case of CDW order and superconductivity. In La 1.875 Ba 0.125 CuO 4 (LBCO), the low-temperature structural domain walls are hypothesized as nanometer-scale pinning sites for the CDWs. Coherent x-ray diffraction techniques have been employed here to visualize the domain structures associated with these symmetry changes directly during phase transition. We have pushed Bragg coherent diffractive imaging (BCDI) into the cryogenic regime where most phase transitions in quantum materials reside. Utilizing BCDI, we image the structural evolution of LBCO microcrystal samples during the high-temperature tetragonal to low-temperature orthorhombic (LTO) phase transition. Our results show the formation of LTO domains close to the transition temperature and how the domain size decreases with temperature. In conclusion, the number of domains follows the secondary order parameter (or orthorhombic strain) measurement with a critical exponent that is consistent with the three-dimensional universality class.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Model Intercomparison of the Impacts of Varying Cloud Droplet–Nucleating Aerosols on the Life Cycle and Microphysics of Isolated Deep Convection

The microphysical impacts of aerosol particles on scattered isolated deep convective cells near Houston, Texas, on 19 June 2013, are examined using multiple cloud-resolving model (CRM) simulations initialized with vertical profiles of low and high concentrations of cloud droplet–nucleating aerosols. These simulations formed part of the Model Intercomparison Project (MIP) conducted by the Deep Convective Working Group of the Aerosol, Cloud, Precipitation and Climate (ACPC) initiative. Each CRM generated a field of convective cells representing those observed during the case study with varying degrees of accuracy. The Tracking and Object-Based Analysis of Clouds (tobac) cell-tracking algorithm was applied to each MIP CRM simulation to track relatively long-lived convective cells (20–60 min). Most of the CRMs produced similar aerosol loading impacts on the warm phase of tracked cell properties with reduced autoconversion and accretion growth of rain, increased cloud water, reduced rainfall, and reduced near-surface evaporation of rain. The sign of aerosol impacts on the warm-phase properties of the convective cells was also quite consistent over cell lifetimes with the greatest magnitude of influence in the first half of the life cycle in most CRMs. In contrast, the ice-phase response to aerosol loading was highly variable among CRMs and included increases or decreases in ice amounts at inconsistent stages of the cell life cycle and midlevel versus upper-level changes in ice. This intermodel variability in ice is indicative both of the complex indirect interactions between aerosols and ice-phase processes in deep convection and their associated parameterizations.

Aerosol-cloud interaction↗

DOE OSTI2022

Extended Modeling of DOE Sealed Canisters with Updated Chemistry Models

Road-ready and final disposition packaging configurations for the advanced test reactor (ATR) fuel currently specifies storage within helium backfilled DOE sealed standard canisters. The aluminum cladding of the ATR fuel contains an oxyhydroxide layer of boehmite/bayerite that generates hydrogen when subjected to irradiation. Understanding the effect of this hydrogen buildup over time to important for long term storage considerations. Previous modeling efforts have built a coupled CFD-chemical model to simulate the temperature gas phase concentrations within the DOE sealed standard canisters. These models have coupled the temperature conditions to both the gas phase radiolysis chemistry and the surface chemistry associated with the oxyhydroxide layer. The previous iteration of the model utilized constant G-values for the hydrogen generation a 50-year period. This new iteration of the model utilizes new experimental data to update the hydrogen generation rate, as well as increase the simulated time to a 200-year period. Given the half-life assumed for the primary Cs-137 isotope responsible for gamma radiation in the ATR spent fuel, the 200-year period decreases the decay heat and dose rate of the spent fuel by a factor of 100, which combined with the updated chemistry substantially decreases new hydrogen generation. Continued experimental work has identified trends for aluminum surrogate samples with oxyhydroxide layers for tests done at higher dose rates. At low initial doses a fast generation rate of hydrogen occurs which starts to roll over to a lower generation as the total dose applied increase. A small-scale chemical model was built to replicate as mini-canister surrogate system at SRNL as well as for the smaller capsule tests performed at INL. A variety of chemical models to capture this effect were tested, and a back reaction of H radical absorbing onto the surface, or inhibition of the reaction by significant H 2 cover gas were both able to fit both the mini-canister and the small capsule test data. Both kinetic fits were used to generate data from the new 200-year simulation. As additional experiments continue, the kinetic fits may be adjusted to adapt to new data. However, updated data shows that hydrogen atmosphere has little effect on actual generation data, so the model was reverted to use a star-stepped G-value for low-dose and high-dose regions. For the undried fuel case, the three models differ significantly with an end concentration of 1% for back reaction, 4.2% for inhibition, and 13.1% for constant G-value for the nominal scenario. For the dried fuel case, the nominal cases showed end concentrations of 0.23% for back reaction, 1.9% for inhibition, and 4.2% for const G-value for the nominal scenario. For the constant G-value case that is less conservative than the other two, the pressure for undried fuel increases to 1.94 atm over 200 years for the nominal case and 2.11 atm for the high decay heat case. The total hydrogen concentration after 200 years is 4.92% for the low decay heat case and 27.4% for the high decay heat case for undried fuel and is 1.4% and 9.6% for low and high decay heat fuel for the dried fuel case. If small amount of residual air is present, the potential for nitric acid formation of 595, 1568, and 2816 ppm for the lower, nominal, and upper fuel decay heat can occur. At long-term timeframes no significant shift in major species present occurs, so no appreciable amount of oxygen is present in the system. The continued rate of hydrogen generation in the canister occurs at an increase of 0.04% by mole over the final 10 years. Increasing the model range out to 1000 years continues to drop the hydrogen generation rate through decreasing dose rate.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2023

Modeling DOE Standard Canister Configurations with Updated Surface Chemistry

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

NASA NTRS1974

Development of polyphenylquinoxaline graphite composites

This exploratory program was divided into four basic tasks. The initial phase was devoted toward investigating processing variables associated with previously developed PPO resins. These polymers were derived from p-bis(phenyl glyoxalyl)benzene reacted with 3,3'-diamino benzidine and/or 3,3',4,4'-tetramino benzophenone. Four new phenyl quinoxaline polymers were synthesized and characterized in Tasks 2 and 3. These consisted of a hydroxyl group containing PPQ synthesized from 3,3'-diamino benzidine (DAB), m-bis(phenyl glyoxal)benzene and m-bis(p'-hydroxy phenyl glyoxalyl) benzene; a cyano group containing PPQ from the reaction of DAB and p-bis(p'-cyano phenoxy phenyl glyoxalyl)benzene; an end-capped block copolymer; and a polymer from the reaction of 3,3',4,4'-tetraamino benzo phenone and m-bis(phenyl glyoxalyl)benzene. The latter two polymers were chosen for composite studies in the latter two tasks of the program. Mechanical properties of the graphite reinforced PPQ composites were determined over the temperature range of +21 C to 316 C. Flexural strengths of the HMS graphite fiber composites were in excess of 8.97 X 10 to the 8th power N/sq m (130,000 psi) at +21 C (70 F) with over 50% strength retention at +316 C.

Hoggatt, J. T.↗

NASA NTRS1976

Injection boundary dynamics during a geomagnetic storm

A series of proton and electron injections were observed by Explorer 45 associated with several substorms during the main phase of the Feb. 24, 1972 geomagnetic storm. The 1- to 290-keV protons and 1- to 560-keV electrons were observed in the evening quadrant up to L of about 5.2. A model distorted dipole magnetic field and McIlwain's E3 convection electric field were used to backtrack the energy-dispersed electron and proton fluxes to their source at the time of injection. The source turns out to be a region extending over several earth radii outside an injection boundary. In the night magnetosphere, the inferred injection boundary is displaced inward with each successive substorm. The energy dispersion plot of the particles injected during orbit 314 indicates that as the energy of the observed particles decreases there is a smooth transition to the position of the plasmapause. This suggests that for that substorm the injection boundary and the plasmapause were one and the same. The proton 'noses' reported by Smith and Hoffman (1974) are discussed.

Konradi, A.↗

NASA NTRS1979

Advanced methods for preparation and characterization of infrared detector materials

Crystal growth of Hg sub 1-x Cd sub x Te and density measurements of ingot slices are discussed. Radial compositional variations are evaluated from the results of infrared transmission edge mapping. The pseudo-binary HgTe-CdTe phase diagram is examined with reference to differential thermal analysis measurements. The phase equilibria calculations, based on the 'regular association solution' theory (R.A.S.) are explained and, using the obtained R.A.S. parameters, the activities of Hg, Cd, and Te vapors and their partial pressures over the pseudo-binary melt are calculated.

Lehoczy, S. L.↗

NASA NTRS1986

Spatial and temporal characteristics of flare energy release determined from X-ray and radio imaging observations

Using the Hard X-ray Imaging Spectrometer (HXIS) from the Solar Maximum Mission Satellite, the morphological aspects and temporal evolution of three major flares which occurred on June 29, 1980 are studied. One of these events, observed at 10:40 UT, is analyzed in particular detail, including Hard X-ray Burst Spectrometer (HXRBS) data and metric wavelength data from the Nancay radioheliograph. The flares occurred during the interaction of two distinct magnetic structures. There is an early onset phase during which there is a weak level of particle acceleration, perhaps accompanied by strong heating within the magnetic interaction region. The impulsive phase of high power energy release is associated with a major interaction between the two structures and accompanied by strong acceleration and heating.

Hernandez, A. M.↗

NASA NTRS1989

Wide swath ocean topography mapping with interferometric altimeters

An interferometric radar altimeter is proposed to provide wide-swath high-resolution ocean topography. Several system design issues of such an interferometric altimeter are presented. Tradeoffs between processing of the interferometric signal using the so-called amplitude approach and the so-called phase approach are shown. The systematic errors associated with uncertainties in the interferometer baseline and the attitude of interferometer orientation are also discussed. Described is an approach using the measurements at orbit cross-over regions, together with the topography measurements from a traditional nadir-looking altimeter that are not contaminated by the baseline and attitude noises. Preliminary simulation results show that such an approach can generate an acceptable error level if the ocean surface does not change appreciably between the observations.

Rodriguez, E.↗

NASA NTRS1991

Formation of the protosolar nebula

Theoretical models are discussed of the collapse of a dense molecular cloud core to form the protosolar nebula that produce the sun and the planet. The theoretical models use the equations of hydrodynamics, gravitation, and radiative transfer to follow the time evolution of a cloud collapsing under its own self-gravity. Both semi-analytical and fully numerical solutions (in two and three spatial dimensions) were calculated by several workers, One challenge is to find a set of initial conditions that will lead to the formation of a suitable protosolar nebula. Detailed results are shown for 2-D models, both with and without turbulent viscosity for redistributing angular momentum, and for 3-D models investigating the strength of gravitational torques associated with nonaxisymmetry produced during the collapse phase.

Tscharnuter, Werner M.↗

NASA NTRS1991

Collision avoidance for CTV: Requirements and capabilities

Cargo transfer vehicle (CTV) operations near Space Station Freedom will require positive collision avoidance maneuver (CAM) capability to preclude any change of collision, even in the event of CTV failures. The requirements for CAM are discussed, and the CAM design approach and design of the Orbiting Maneuvering Vehicle (OMV) are reviewed; this design met requirements for OMV operation near the Space Station, provided a redundant collision avoidance maneuver capability. Significant portions of the OMV CAM design should be applicable to CTV. The key features of the OMV design are summarized and related to the CTV mission design to that of OMV's. CAM is a defined sequence of events executed by the CTV to place the vehicle in a safe position relative to a target such as the Space Station. CAM can be performed through software commands to the propulsion system, or through commands pre-stored in hardware. Various techniques for triggering CAM are considered, and the risks associated with CAM enable and execution in phases are considered. OMV CAM design features both hardware and software CAM capability, with analyses conducted to assess the ability to meet the collision-free requirement during all phases of the mission.

Nosek, Thomas P.↗

NASA NTRS1993

C/O atomic ratios in micrometer-size crushed grains from Antarctic micrometeorites and two carbonaceous meteorites

Antarctic micrometeorites (AMM's) have similarities (but also differences) with primitive meteorites, such as unequilibrated mineral assemblages. To further assess such similarities, we have measured the carbon content of micrometeorites and meteorites (Orgueil and Murchison), as determined in a random selection of micrometer-size crushed grain, with an analytical transmission electron microscope. Such analyses yield the C/O atomic ratio, the major and minor elements contents, and the textural features of the grains on a scale of approx. equal to 100 nanometers. An important proportion of micrometeorites from both the 100-400 micron and the 50-100 micron size fractions contains much more carbon than CI chondrite Orgueil. The average C-content of all micrometeorites in these two size fractions amount to approximately 1.8 x CI, and approximately 0.8 x CI, respectively (CI refers to the bulk C-content of Orgueil, of about 3.5 percent by weight). Carbon is usually not homogeneously distributed in the micrometeorite but is concentrated in C-rich grains. So far, most of these grains are amorphous, and seem to be associated with an oxidized Fe-rich phase (possibly a variety of 'dirty' magnetite). About 5 percent of them have the composition of 'COPS', a phase additionally enriched in O, P, and S.

Perreau, M.↗

NASA NTRS1994

Aubrite basalt vitrophyres: High sulfur silicate melts and a snapshot of aubrite formation

Two aubrite basalt vitrophyre clasts have been found within AMNH thin sections from the Parsa EH3 chondrite and the Khor Temiki aubrite. Polished sections of the Parsa Aubrite Inclusion (PAI) and the Khor Temiki Inclusion (KTI) were studied by optical, electron probe microanalysis (EPMA), and scanning electron microscopy (SEM) techniques with broad-beam and low absorbed EPMA currents used to minimize glass volatile loss. Some data have previously been reported for PAI and KTI may possibly correlate to a previously reported inclusion in Khor Tiimiki. In polished sections, PAI and KTI are approximately equal 4 mm in diameter and contain a large volume of glass. The clasts have similar textural characteristics and are akin to lunar vitrophyre textures. The glasses have high alkali rhyodacitic compositions Al-though PAI is peraluminous, KTI is significantly peralkaline. Additionally, the glasses have elevated sulfur concentrations that are extremely high by geochemical standards. SEM examination for beam overlap of microscopic CaS, FeS, and (Mg, Mn, Fe) S inclusions showed no such contamination. Furthermore, homogeneity of glass S content and low FeO contents help rule out contamination. Materials research data show that under reducing conditions alumino-silicate melts can dissolve up to several weight percent sulfur in the absence of Fe. The high S and alkali contents, the lack of associated high shock features, and the rationalized phase equilibria suggest that PAI and KTI are igneous melting products of an E-chondrite-like source material. Although large-scale impact melting cannot totally be ruled out, the above observations eliminate the possibility of in-situ shock melting.

Fogel, R. A.↗

NASA NTRS1997

Nucleation and Convection Effects in Protein Crystal Growth

Work during the second year under this grant (NAG8-1161) resulted in several major achievements. We have characterized protein impurities as well as microheterogeneities in the proteins hen egg white lysozyme and horse spleen apoferritin, and demonstrated the effects of these impurities on nucleation and crystallization. In particular, the purification of apoferritin resulted in crystals with an X-ray diffraction resolution of better than 1.8 A, i.e. a 1 A improvement over earlier work on the cubic form. Furthermore, we have shown, in association with studies of liquid-liquid phase separation, that depending on the growth conditions, lysozyme can produce all growth morphologies that have been observed with other proteins. Finally, in connection with our experimental and simulation work on growth step bunching, we have developed a system-dependent criterion for advantages and disadvantages of crystallization from solution under reduced gravity. In the following, these efforts are described in some detail.

Rosenberger, Franz↗

NASA NTRS1995

Gravity Waves Near 300 km Over the Polar Caps

Distinctive wave forms in the distributions of vertical velocity and temperature of both neutral particles and ions are frequently observed from Dynamics Explorer 2 at altitudes above 250 km over the polar caps. These are interpreted as being due to internal gravity waves propagating in the neutral atmosphere. The disturbances characterized by vertical velocity perturbations of the order of 100 m/s and horizontal wave lengths along the satellite path of about 500 km. They often extend across the entire polar cap. The associated temperature perturbations indicate that the horizontal phase progression is from the nightside to the dayside. Vertical displacements are inferred to be of the order of 10 km and the periods to be of the order of 10(exp 3) s. The waves must propagate in the neutral atmosphere, but they usually are most clearly recognizable in the observations of ion vertical velocity and ion temperature. By combining the neutral pressure calculated from the observed neutral concentration and temperature with the vertical component of the neutral velocity, an upward energy flux of the order of 0.04 erg/sq cm-s at 250 km has been calculated, which is about equal to the maximum total solar ultraviolet heat input above that altitude. Upward energy fluxes calculated from observations on orbital passes at altitudes from 250 to 560 km indicate relatively little attenuation with altitude.

Johnson, F. S.↗