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All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Insights into Preceramic Polymer-Based Additive Manufacturing Inks via Rheological and Scattering Studies of Preceramic Polymer-Grafted Nanoparticles Suspended in Polycarbosilane

Preceramic polymers (PCPs) offer advantages in producing ceramics due to their processability and ability to tailor the final chemistry of the produced material. However, challenges such as volumetric shrinkage and mass loss during pyrolysis often result in polymer-derived ceramics containing pores and cracks. PCP-grafted ceramic nanoparticles (PCPGNPs) have been proposed and studied as a route to mitigate the shrinkage issues associated with neat PCPs. Prior studies on PCPGNPs have principally focused on the synthesis and characterization of neat materials. Dispersing PCPGNPs in commercial preceramic polymer is another attractive, but underexplored, route to control the rheological and char yield properties of PCP systems. In this work, a systematic rheological study of commercial PCP (SMP-877) and PCPGNP (silica with poly(1,1-dimethylpropylsilane) corona) mixtures was executed to develop design rules for the processing of such systems. A rheological study demonstrated the effect of increasing particle concentration on network formation with percolation occurring between 50 and 60 wt %. Samples above the percolation threshold exhibited higher viscosities and rapid shear thinning thus demonstrating their direct-write printability. X-ray photon correlation spectroscopy (XPCS) corroborated the rheology and showed two diffusive modes when the material was above percolation. Mixtures of PCPGNPs and SMP-877 had synergistically higher char yields upon thermal treatment and pyrolysis. XPCS and rheological measurements during thermal treatment identified thermal jamming of the polymer grafts as a key factor in improving the char yield. In conclusion, with the insights gained here, we expect these mixed systems to provide attractive feedstocks for polymer-derived ceramics, with proof-of-principal application as feedstocks for direct ink write (DIW) additive manufacturing.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Interflow Is Not Binary: A Continuous Shallow Perched Layer Does Not Imply Continuous Connectivity

Hillslopes exert critical controls on the quality and quantity of downstream waters. To understand and model dominant headwater catchment processes, we need to estimate the relative importance of different runoff generation processes. In this work we analyze published data from studies of 17 hillslopes from a range of landscapes to better understand the relative role of interflow, that is, shallow lateral subsurface flow moving over a layer impeding percolation, in streamflow generation. For each slope, we calculated downslope interflow travel distances, that is, the potential distance a water parcel travels downslope above an impeding layer until it percolates into the impeding layer. The downslope travel distances for the 17 hillslopes ranged from around 1 m to several hundred meters. The vector analysis of downslope travel distances revealed that all but three hillslopes had slope lengths that were much longer than downslope travel distances. For the remaining 14 cases we could show that most water perched above a shallow impeding layer percolates through the impeding layer before reaching the valley or the stream channel. Thus, interflow usually contributes directly to valley water or streamflow only from the lower portions of the hillslope in most landscapes. A critical finding of our analysis is that a continuously perched saturated zone with downslope flow does not imply continuous connectivity to the stream. Such a continuous connectivity is the exception rather than the rule in most landscapes. Future hillslope and headwater processes and modeling studies will need to account for this.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2017

Reducing Cascading Failure Risk by Increasing Infrastructure Network Interdependence

Increased coupling between critical infrastructure networks, such as power and communication systems, has important implications for the reliability and security of these systems. To understand the effects of power-communication coupling, several researchers have studied models of interdependent networks and reported that increased coupling can increase vulnerability. However, these conclusions come largely from models that have substantially different mechanisms of cascading failure, relative to those found in actual power and communication networks, and that do not capture the benefits of connecting systems with complementary capabilities. In order to understand the importance of these details, this paper compares network vulnerability in simple topological models and in models that more accurately capture the dynamics of cascading in power systems. First, we compare a simple model of topological contagion to a model of cascading in power systems and find that the power grid model shows a higher level of vulnerability, relative to the contagion model. Second, we compare a percolation model of topological cascading in coupled networks to three different models of power networks coupled to communication systems. Again, the more accurate models suggest very different conclusions than the percolation model. In all but the most extreme case, the physics-based power grid models indicate that increased power-communication coupling decreases vulnerability. This is opposite from what one would conclude from the percolation model, in which zero coupling is optimal. Only in an extreme case, in which communication failures immediately cause grid failures, did we find that increased coupling can be harmful. Together, these results suggest design strategies for reducing the risk of cascades in interdependent infrastructure systems.

24 POWER TRANSMISSION AND DISTRIBUTION↗
DOE OSTI2013

The dynamical crossover in attractive colloidal systems

We study the dynamical arrest in an adhesive hard-sphere colloidal system. We examine a micellar suspension of the Pluronic-L64 surfactant in the temperature (T) and volume fraction (ϕ) phase diagram. According to mode-coupling theory (MCT), this system is characterized by a cusp-like singularity and two glassy phases: an attractive glass (AG) phase and a repulsive glass (RG) phase. The T − ϕ phase diagram of this system as confirmed by a previous series of scattering data also exhibits a Percolation Threshold (PT) line, a reentrant behavior (AG-liquid-RG), and a glass-to-glass transition. The AG phase can be generated out of the liquid phase by using T and ϕ as control parameters. We utilize viscosity and nuclear magnetic resonance (NMR) techniques. NMR data confirm all the characteristic properties of the colloidal system phase diagram and give evidence of the onset of a fractal-like percolating structure at a precise threshold. The MCT scaling laws used to study the shear viscosity as a function of ϕ and T show in both cases a fragile-to-strong liquid glass-forming dynamic crossover (FSC) located near the percolation threshold where the clustering process is fully developed. These results suggest a larger thermodynamic generality for this phenomenon, which is usually studied only as a function of the temperature. We also find that the critical values of the control parameters, coincident with the PT line, define the locus of the FSC. In the region between the FSC and the glass transition lines the system dynamics are dominated by clustering effects. We thus demonstrate that it is possible, using the conceptual framework provided by extended mode-coupling theory, to describe the way a system approaches dynamic arrest, taking into account both cage and hopping effects.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Negative permittivity and permeability spectra of Cu/yttrium iron garnet hybrid granular composite materials in the microwave frequency range

The relative complex permittivity and permeability spectra of the coagulated copper and yttrium iron garnet (Cu/YIG) hybrid granular composite materials have been studied in the microwave range. The insulator to metal transition was observed at the percolation threshold of Cu particle content (φ{sub Cu} = 16.0 vol. %) in the electrical conductivity. In the percolation threshold, the low frequency plasmonic state caused by the metallic Cu particle networks was observed. The percolated Cu/YIG granular composites show simultaneous negative permittivity and permeability spectra under external magnetic fields.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Nanocomposite formed by titanium ion implantation into alumina

Composites of titanium nanoparticles in alumina were formed by ion implantation of titanium into alumina, and the surface electrical conductivity measured in situ as the implantation proceeded, thus generating curves of sheet conductivity as a function of dose. The implanted titanium self-conglomerates into nanoparticles, and the spatial dimensions of the buried nanocomposite layer can thus be estimated from the implantation depth profile. Rutherford backscattering spectrometry was performed to measure the implantation depth profile, and was in good agreement with the calculated profile. Transmission electron microscopy of the titanium-implanted alumina was used for direct visualization of the nanoparticles formed. The measured conductivity of the buried layer is explained by percolation theory. We determine that the saturation dose, φ{sub 0}, the maximum implantation dose for which the nanocomposite material still remains a composite, is φ{sub 0} = 2.2 × 10{sup 16 }cm{sup −2}, and the corresponding saturation conductivity is σ{sub 0} = 480 S/m. The percolation dose φ{sub c}, below which the nanocomposite still has basically the conductivity of the alumina matrix, was found to be φ{sub c} = 0.84 × 10{sup 16 }cm{sup −2}. The experimental results are discussed and compared with a percolation theory model.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Halo exclusion criteria impacts halo statistics

ABSTRACT Every halo-finding algorithm must make a critical yet relatively arbitrary choice: it must decide which structures are parent haloes, and which structures are subhaloes of larger haloes. We refer to this choice as percolation. We demonstrate that the choice of percolation impacts the statistical properties of the resulting halo catalogue. Specifically, we modify the halo-finding algorithm rockstar to construct three different halo catalogues from the same simulation data, each with identical mass definitions, but different choice of percolation. The resulting haloes exhibit significant differences in both halo abundance and clustering properties. Differences in the halo mass function reach 6 per cent for haloes of mass $10^{13}\ h^{-1}\ {\rm {\rm M}_{\odot }}$, larger than the few per cent precision necessary for current cluster abundance experiments such as the Dark Energy Survey. Comparable differences are observed in the large-scale clustering bias, while differences in the halo–matter correlation function reach 30 per cent on translinear scales. These effects can bias weak-lensing estimates of cluster masses at a level comparable to the statistical precision of current state-of-the-art experiments.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Measurement-induced criticality in random quantum circuits

We investigate the critical behavior of the entanglement transition induced by projective measurements in (Haar) random unitary quantum circuits. Using a replica approach, we map the calculation of the entanglement entropies in such circuits onto a two-dimensional statistical-mechanics model. In this language, the area- to volume-law entanglement transition can be interpreted as an ordering transition in the statistical-mechanics model. We derive the general scaling properties of the entanglement entropies and mutual information near the transition using conformal invariance. We analyze in detail the limit of infinite on-site Hilbert space dimension in which the statistical-mechanics model maps onto percolation. In particular, we compute the exact value of the universal coefficient of the logarithm of subsystem size in the n th Rényi entropies for n ≥ 1 in this limit using relatively recent results for the conformal field theory describing the critical theory of two-dimensional (2D) percolation, and we discuss how to access the generic transition at finite on-site Hilbert space dimension from this limit, which is in a universality class different from 2D percolation. Here, we also comment on the relation to the entanglement transition in random tensor networks, studied previously in Vasseur et al. [Phys. Rev. B 100, 134203 (2019)].

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Scrambling Transition in a Radiative Random Unitary Circuit

Here we study quantum information scrambling in a random unitary circuit that exchanges qubits with an environment at a rate p. As a result, initially localized quantum information not only spreads within the system, but also spills into the environment. Using the out-of-time-order correlator (OTOC) to characterize scrambling, we find a nonequilibrium phase transition in the directed percolation universality class at a critical swap rate p c : for p < p c the ensemble-averaged OTOC exhibits ballistic growth with a tunable light cone velocity, while for p > p c the OTOC fails to percolate within the system and vanishes uniformly within a finite timescale, indicating that all local operators are rapidly swapped into the environment. To elucidate its information-theoretic consequences, we demonstrate that the transition in operator spreading coincides with a transition in an observer’s ability to decode the system’s initial quantum information from the swapped-out, or “radiated,” qubits. We present a simple decoding scheme which recovers the system’s initial information with perfect fidelity in the nonpercolating phase, and with continuously decreasing fidelity with decreasing swap rate in the percolating phase. Depending on the initial state of the swapped-in qubits, we further observe a corresponding entanglement transition in the coherent information from the system into the radiated qubits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Application of the Environmentally Non-Aggressive Dissolvents to Mobilize Metals in Tailings in the Norilsk Region

Under analysis is on-site extractability of nonferrous and noble metals from tailings by leaching with natural reagents (humus acids, water, lignin). Redistribution of nonferrous and noble metals in a percolation bed made of old tailings in the Norilsk copper–nickel ore field is studied. Kinetics of dissolving of nonferrous and noble metals under capillary ascensional percolation is investigated. It is shown that directional capillary percolation of solutions is applicable to extraction of nonferrous and noble metals under long-term mining waste storage.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Phase-field simulations of fission gas bubble growth and interconnection in U-(Pu)-Zr nuclear fuel

Abstract The growth and interconnection of fission gas bubbles in the hotter central regions of U-(Pu)-Zr nuclear fuel has been simulated with a phase-field model. The Cahn-Hilliard equation was used to represent the two-phase microstructure, with a single defect species. The volume fraction of the bubble phase and surface area of the bubble-matrix interface were determined during growth and interconnection. Surface area increased rapidly during the initial stages of growth, then slowed and finally decreased as bubble interconnection began and coarsening acted to reduce surface area. The fraction of the bubbles vented to a simulation domain boundary, f V , was quantified as a measure of the microstructure’s interconnectivity and plotted as a function of porosity p . The defect species diffusivity was varied; although changes in diffusivity significantly affected the microstructure, the plots of f V vs. p did not change significantly. The percolation threshold p c was calculated to be approximately 0.26, depending on the assumed diffusivity and using an initial bubble number density based on experimental observations. This is slightly smaller than the percolation threshold for continuum percolation of overlapping 3D spheres. The simulation results were used to parameterize two different engineering-scale swelling models for U-(Pu)-Zr in the nuclear fuel performance code BISON.

Aagesen, Larry K. (ORCID:000000034936676X)↗
DOE OSTI2018

Challenging Geostatistical Methods To Represent Heterogeneity in CO2 Reservoirs Under Residual Trapping

Abstract Geostatistical methods based on two-point spatial-bivariate statistics have been used to model heterogeneity within computational studies of the dispersion of contaminants in groundwater reservoirs and the trapping of CO2 in geosequestration reservoirs. The ability of these methods to represent fluvial architecture, commonly occurring in such reservoirs, has been questioned. We challenged a widely used two-point spatial-bivariate statistical method to represent fluvial heterogeneity in the context of representing how reservoir heterogeneity affects residual trapping of CO2 injected for geosequestration. A more rigorous model for fluvial architecture was used as the benchmark in these studies. Both the geostatistically generated model and the benchmark model were interrogated, and metrics for the connectivity of high-permeability preferential flow pathways were quantified. Computational simulations of CO2 injection were performed, and metrics for CO2 dynamics and trapping were quantified. All metrics were similar between the two models. The percentage of high-permeability cells in spanning connected clusters (percolating clusters) was similar because percolation is strongly dependent upon proportions, and the same proportion of higher permeability cross-strata was specified in generating both models. The CO2 plume dynamics and residual trapping metrics were similar because they are largely controlled by the occurrence of percolating clusters. The benchmark model represented more features of the fluvial architecture and, depending on context, representing those features may be quite important, but the simpler geostatistical model was able to adequately represent fluvial reservoir architecture within the context and within the scope of the parameters represented here.

defects, mechanical behavior, carbon sequestration↗
DOE OSTI2020

Nevada National Security Site 2019 Waste Management Monitoring Report Area 3 and Area 5 Radioactive Waste Management Sites

Environmental monitoring data are collected at and around the Area 3 and Area 5 Radioactive Waste Management Sites (RWMSs) within the Nevada National Security Site (NNSS). This report summarizes the 2019 environmental data to provide an overall evaluation of RWMS performance and to support environmental compliance and performance assessment (PA) activities. Some of these data (e.g., radiation exposure, air, and groundwater) are presented in other reports (Mission Support and Test Services, LLC 2019, 2020a, 2020b). Direct radiation monitoring data indicate exposure levels at the Area 3 and Area 5 RWMSs are within the range of background levels measured at the NNSS. Slightly elevated exposure levels outside the Area 3 RWMS are attributed to nearby historical aboveground nuclear weapons tests. Air monitoring data at the Area 3 and Area 5 RWMSs show that tritium concentrations in water vapor and americium and plutonium concentrations in air particles are below Derived Concentration Standards for these radionuclides. Groundwater monitoring data indicate the groundwater in the uppermost aquifer beneath the Area 5 RWMS is not impacted by RWMS operations. Results of groundwater analysis from wells around the Area 5 RWMS are below established investigation levels. Leachate samples collected from the leachate collection systems at the Area 5 mixed low-level waste disposal unit are below established contaminant regulatory limits. During 2019, precipitation at the Area 3 RWMS was 77 percent above average, and precipitation at the Area 5 RWMS was 69 percent above average. Water balance measurements indicate that evapotranspiration from the vegetated weighing lysimeter at the Area 5 RWMS dries the soil and prevents downward percolation of precipitation more effectively than evaporation as measured from the bare-soil weighing lysimeter. Vadose zone monitoring in the Area 3 and Area 5 RWMS soil covers shows no evidence of precipitation percolating through the covers to the waste. Moisture from precipitation did not percolate below 120 centimeters (3.9 feet [ft]) in the vegetated final cover on the U-3ax/bl disposal unit at the Area 3 RWMS during 2019. There was no drainage through 2.4 meters (8 ft) of soil as indicated from the Area 3 drainage lysimeters that received only natural precipitation. At the Area 3 RWMS, which received three times the natural precipitation, 57 percent of the applied precipitation and irrigation drained from the bare-soil drainage lysimeter. All 2019 monitoring data indicate that the Area 3 and Area 5 RWMSs are performing within expectations of the model and parameter assumptions for the facilities’ PAs.

2019↗
DOE OSTI2022

Strategies to Recover Easily-Extractable Rare Earth Elements and Other Critical Metals from Coal Waste Streams and Adjacent Rock Strata Using Citric Acid

Maximum rare earth element (REE) extractability from a sample of Middle Kittanning coal seam underclay was previously demonstrated at ~30% of the total REE content with a citric acid solution (Montross et al., 2020). This report further refines the mechanisms of citrate application for leaching of coal seam underclays using an organic acid lixiviant and evaluates strategies to begin to scale this process to industrially relevant volumes. This study evaluates the suitability of citrate leaching solutions for downstream recovery and separation of the REEs via oxalic acid precipitation. The applicability of citric acid solutions to recover ion-adsorbed metals from clay surfaces was evaluated by leaching a prepared sample of kaolinite with known amounts of ion-adsorbed lanthanum. Citrate systematics was further defined through experiments varying the solution pH. Up-scaling investigations proceeded with percolation leaching columns and stirred tank reactors. Two embodiments were run in percolation leaching: a continuous flow-through process and a multi-stage saturated process. The results showed that in certain limited scenarios, low pH citrate solutions could be used to target REEs mineralized within secondary calcium phosphate minerals. Results from the upscaling attempts encountered difficulties in extraction efficiencies. For the percolation columns, hydrodynamic flow was insufficient to recover the extractable REE content fully. For the stirred barrels, mixing inefficiencies likely inhibited the extractability of the REEs. Oxalic acid precipitation experiments also highlighted difficulties in downstream operations. The REEs were removed from the citrate solution with high efficiency, but were accompanied by equally efficient removal of calcium in orders of magnitude of greater amounts. Overall, for citrate leaching to be effective, future studies will have to: 1) carefully consider the feedstock application (i.e., likely better suited for secondary mineralization of calcium phosphate minerals), and 2) overcome the technical barriers of large-scale processing, such as inefficient hydrodynamic regimes due to small crush sizes needed and difficulties in downstream separation and purification. Alternatively, citrate solutions may be better recommended as leaching amendments to other leaching solutions to enhance REE complexation in the solution.

01 COAL, LIGNITE, AND PEAT↗
NASA NTRS1993

Unusual radar echoes from the Greenland ice sheet

In June 1991, the NASA/Jet Propulsion Laboratory airborne synthetic-aperture radar (AIRSAR) instrument collected the first calibrated data set of multifrequency, polarimetric, radar observations of the Greenland ice sheet. At the time of the AIRSAR overflight, ground teams recorded the snow and firn (old snow) stratigraphy, grain size, density, and temperature at ice camps in three of the four snow zones identified by glaciologists to characterize four different degrees of summer melting of the Greenland ice sheet. The four snow zones are: (1) the dry-snow zone, at high elevation, where melting rarely occurs; (2) the percolation zone, where summer melting generates water that percolates down through the cold, porous, dry snow and then refreezes in place to form massive layers and pipes of solid ice; (3) the soaked-snow zone where melting saturates the snow with liquid water and forms standing lakes; and (4) the ablation zone, at the lowest elevations, where melting is vigorous enough to remove the seasonal snow cover and ablate the glacier ice. There is interest in mapping the spatial extent and temporal variability of these different snow zones repeatedly by using remote sensing techniques. The objectives of the 1991 experiment were to study changes in radar scattering properties across the different melting zones of the Greenland ice sheet, and relate the radar properties of the ice sheet to the snow and firn physical properties via relevant scattering mechanisms. Here, we present an analysis of the unusual radar echoes measured from the percolation zone.

Rignot, E. J.↗
DOE OSTI2014

Invariant soil water potential at zero microbial respiration explained by hydrological discontinuity in dry soils

We report that soil microbial respiration rates decrease with soil drying, ceasing below water potentials around -15 MPa. A proposed mechanism for this pattern is that under dry conditions, microbes are substrate limited because solute diffusivity is halted due to breaking of water film continuity. However, pore connectivity estimated from hydraulic conductivity and solute diffusivity (at Darcy's scale) is typically interrupted at much less negative water potentials than microbial respiration (-0.1 to -1 MPa). It is hypothesized here that the more negative respiration thresholds than at the Darcy's scale emerge because microbial activity is restricted to microscale soil patches that retain some hydrological connectivity even when it is lost at the macroscale. This hypothesis is explored using results from percolation theory and meta-analyses of respiration-water potential curves and hydrological percolation points. Lastly, when reducing the spatial scale from macroscale to microscale, hydrological and respiration thresholds become consistent, supporting the proposed hypothesis.

58 GEOSCIENCES↗
DOE OSTI2020

Effect of Fluorination on Lithium Transport and Short-Range Order in Disordered-Rocksalt-Type Lithium-Ion Battery Cathodes

Fluorine substitution is a critical enabler for improving the cycle life and energy density of disordered rocksalt (DRX) Li-ion battery cathode materials which offer prospects for high energy density cathodes, without the reliance on limited mineral resources. Due to the strong Li–F interaction, fluorine also is expected to modify the short-range cation order in these materials which is critical for Li-ion transport. In this work, density functional theory and Monte Carlo simulations are combined to investigate the impact of Li–F short-range ordering on the formation of Li percolation and diffusion in DRX materials. Additionally, the modeling reveals that F substitution is always beneficial at sufficiently high concentrations and can, surprisingly, even facilitate percolation in compounds without Li excess, giving them the ability to incorporate more transition metal redox capacity and thereby higher energy density. It is found that for F levels below 15%, its effect can be beneficial or disadvantageous depending on the intrinsic short-range order in the unfluorinated oxide, while for high fluorination levels the effects are always beneficial. Using extensive simulations, a map is also presented showing the trade-off between transition-metal capacity, Li-transport, and synthetic accessibility, and two of the more extreme predictions are experimentally confirmed.

25 ENERGY STORAGE↗