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At least 307 records · Page 17

Air separation via two-step solar thermochemical cycles based on SrFeO 3-δ and (Ba,La) 0.15 Sr 0.85 FeO 3-δ perovskite reduction/oxidation reactions to produce N 2 : rate limiting mechanism(s) determination

Two-step solar thermochemical cycles based on reversible reactions of SrFeO 3–δ and (Ba,La) 0.15 Sr 0.85 FeO 3–δ perovskites were considered for air separation. The cycle steps encompass (1) the thermal reduction of SrFeO 3–δ or (Ba,La) 0.15 Sr 0.85 FeO 3–δ perovskites driven by concentrated solar irradiation and (2) oxidation in air to remove O 2 and produce N 2 . Rate limiting mechanisms were examined for both reactions using a combination of isothermal and non-isothermal thermogravimetry for temperature-swings between 673 and 1373 K, heating rates of 10, 20, and 50 K min –1 , and O 2 pressure-swings between 20% O 2 /Ar and 100% Ar at atmospheric pressure. Evolved O 2 and associated lag due to transport behavior were measured with gas chromatography and used with measured sample temperatures to predict equilibrium compositions from a compound energy formalism thermodynamic model. Measured and predicted chemical equilibrium changes in deviation from stoichiometry were compared. Rapid chemical kinetics were observed as the samples equilibrated rapidly for all conditions, indicative that heat and mass transfer were the rate limiting mechanisms. Furthermore, the effects of bulk diffusion (or gas diffusion through the bed or pellet) were examined using pelletized and loose powdered samples and determined to have no discernable impact.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Intermediate time sub-diffusion and stress relaxation in ring polymer melts

The slow dynamics of non-concatenated ring melts remains a frontier problem in polymer science with implications for many soft material environments including cellular biophysics. Here, in this work, we report large-scale simulations of model ring melts that analyze the monomer and center-of-mass (CM) mean square displacements (MSD) and stress relaxation function on intermediate time and length scales. The degree of dynamical slowing down is characterized by the maximally sub-diffusive fractional time scaling exponents. The data span an exceptionally wide range of ring degrees of polymerization and stiffnesses and are not successfully organized based on the classic measure linear chain entanglement, N/N e . Rather, we find that the crossover degree of polymerization, N D , based on ring macromolecular caging that successfully allows master curves to be constructed for the long-time CM self-diffusion constant also collapses these temporal dynamic scaling exponents. Different properties display different exponents and exhibit one or two regimes of linear variation with the logarithm of N D / N . A distinct crossover of the CM-MSD and stress relaxation exponents emerges at sufficiently large N or stiffness that is not found for the monomer MSD, indicating a novel form of dynamic decoupling. This crossover aligns with the predicted critical degree of polymerization for transitioning from a weak to strong caging regime, indicative of activated transport. The latter may reflect the emergence of an intermolecular collective contribution to stress in analogy with dense soft colloidal matter. Suggestions are made for future theoretical work to address the rich patterns of behavior discovered.

Anomalous diffusion↗

Floating dark matter in celestial bodies

Dark matter (DM) can be captured in celestial bodies after scattering and losing sufficient energy to become gravitationally bound. We derive a general framework that describes the current DM distribution inside celestial objects, which self-consistently includes the effects of concentration diffusion, thermal diffusion, gravity, and capture accumulation. For DM with sufficient interactions, we show that a significant DM population can thermalize and sit towards the celestial-body surface. This surface-enhanced DM distribution allows for new phenomenology for DM searches in a wide range of celestial bodies, including the Sun, Earth, Jupiter, Brown Dwarfs, and Exoplanets.

79 ASTRONOMY AND ASTROPHYSICS↗

Global gyrokinetic simulations of electrostatic microturbulent transport using kinetic electrons in LHD stellarator

Global gyrokinetic simulations of ion temperature gradient (ITG) and trapped electron mode (TEM) in the LHD stellarator are carried out using the gyrokinetic toroidal code (GTC) with kinetic electrons. ITG simulations show that kinetic electron effects increase the growth rate by more than 50% and more than double the turbulent transport levels compared with simulations using adiabatic electrons. Zonal flow dominates the saturation mechanism in the ITG turbulence. Nonlinear simulations of the TEM turbulence show that the main saturation mechanism is not the zonal flow but the inverse cascade of high to low toroidal harmonics. Further nonlinear simulations with various pressure profiles indicate that the ITG turbulence is more effective in driving heat conductivity whereas the TEM turbulence is more effective for particle diffusivity.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Modelling and simulation of brinicle formation

Below the Arctic sea ice, under the right conditions, a flux of icy brine flows down into the sea. The icy brine has a much lower fusion point and is denser than normal seawater. As a result, it sinks while freezing everything around it, forming an ice channel called a brinicle (also known as ice stalactite). In this paper, we develop a mathematical model for this phenomenon, assuming cylindrical symmetry. The fluid is considered to be viscous and quasi-stationary. The heat and salt transport are weakly coupled to the fluid motion and are modelled with the corresponding conservation equations, accounting for diffusive and convective effects. Finite-element discretization is employed to solve the coupled system of partial differential equations. We find that the model can capture the general behaviour of the physical system and generate brinicle-like structures while also recovering dendrite composition, which is a physically expected feature aligned with previous experimental results. This represents, to our knowledge, the first complete model proposed that captures the global structure of the physical phenomenon even though it has some discrepancies, such as brine accumulation.

97 MATHEMATICS AND COMPUTING↗

Quasi-one-dimensional uniform spin- 1 2 Heisenberg antiferromagnet KNaCuP 2 O 7 probed by P 31 and Na 23 NMR

Here we present the structural and magnetic properties of KNaCuP 2 O 7 investigated via x-ray diffraction, magnetization, specific heat, and P 31 and Na 23 NMR measurements and complementary electronic structure calculations. The temperature-dependent magnetic susceptibility and P 31 NMR shift could be modeled very well by the uniform spin- 1 2 Heisenberg antiferromagnetic chain model with a nearest-neighbor interaction J / k B ≃ 58.7 K . The corresponding mapping using first-principles electronic structure calculations leads to J DFT / k B ≃ 59 K with negligibly small interchain couplings, further confirming that the system is indeed a one-dimensional uniform spin- 1 2 Heisenberg antiferromagnet. The diverging trend of NMR spin-lattice relaxation rates ( 1 / T 1 31 and 1 / T 1 23 ) implies the onset of a magnetic long-range ordering at around T N ≃ 1 K . From the value of T N , the average interchain coupling is estimated to be J ' / k B ≃ 0.28 K . Moreover, the NMR spin-lattice relaxation rates show the dominant contributions from uniform ( q = 0 ) and staggered ( q = ± π / a ) spin fluctuations in the high- and low-temperature regimes, respectively, mimicking one-dimensionality of the spin lattice. We have also demonstrated that 1 / T 1 31 in high temperatures varies linearly with 1 / H , reflecting the effect of spin diffusion on the dynamic susceptibility. The temperature-dependent unit cell volume could be described well using the Debye approximation with a Debye temperature of Θ D ≃ 294 K , consistent with the heat capacity data.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Comparison of momentum transport models for numerical relativity

The main problems of nonvacuum numerical relativity, compact binary mergers and stellar collapse, involve hydromagnetic instabilities and turbulent flows, so that kinetic energy at small scales leads to mean effects at large scale that drive the secular evolution. Notable among these effects is momentum transport. We investigate two models of this transport effect, a relativistic Navier-Stokes system and a turbulent mean stress model, that are similar to all of the prescriptions that have been attempted to date for treating subgrid effects on binary neutron star mergers and their aftermath. Our investigation involves both stability analysis and numerical experimentation on star and disk systems. We also begin the investigation of the effects of particle and heat transport on postmerger simulations. Here, we find that correct handling of turbulent heating is crucial for avoiding unphysical instabilities. Given such appropriate handling, the evolution of a differentially rotating star and the accretion rate of a disk are reassuringly insensitive to the choice of prescription. However, disk outflows can be sensitive to the choice of method, even for the same effective viscous strength. We also consider the effects of eddy diffusion in the evolution of an accretion disk and show that it can interestingly affect the composition of outflows.

79 ASTRONOMY AND ASTROPHYSICS↗

Equilibrium solute segregation to matrix- θ' precipitate interfaces in Al-Cu alloys from first principles

Particular combinations of solute atoms segregated to the interface of the Al and θ ' - Al 2 Cu in Al-Cu alloys can help stabilize θ ' precipitates at high temperatures. Stabilization of such precipitates is determined by a combination of thermodynamics (including driving forces for coarsening and transformation and solute segregation tendencies) and kinetic effects (including solute diffusion and interfacial mobility in the presence of interfacial solute segregation). For some alloys such as recent Al-Cu-based alloys, multiple solutes segregate in significant quantities to interfaces, and solute-solute interactions at the interface are important, with multiple types of solutes competing for similar interfacial sites. To treat this situation, we develop and apply a statistical mechanics approach to calculate the temperature-dependent equilibrium solute atoms distribution near the coherent and semicoherent interfaces between the Al matrix and the θ ' - Al 2 Cu precipitates. The developed approach is applied to the investigation of Si, Mn, and Zr segregation at the interface, as particular combinations of these elements affect the thermal stability of the θ ' precipitates. We demonstrate that because Si and Mn atoms segregate on the same semicoherent interface, the presence of Si reduces the concentration of Mn solutes at the interface. Si atoms preferably occupy the first layer of the interface and compete with Mn atoms for one type of particular sites in the layer. Mn atoms preferably occupy the second layer of the semicoherent interface, and the Mn-Mn interaction plays an important role in their distribution. Zr atoms mostly segregate on one of the two nonequivalent sites of the second layer of the coherent interface. Due to symmetry properties of the coherent interface, the calculations show that the segregation Zr of atoms to this interface will likely lead to the formation of L 1 2 ordered Al 3 Zr layer.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Predictive Large-Eddy Simulation of Supercritical-Pressure Reactive Flows in the Cold Ignition Regime

This report describes a one-year study performed under DOE sponsorship, continuing the investigation of high-pressure turbulent reactive flows. The interest is in the effect of the chemical species distribution in high-pressure turbulent flows in the presence of strong temperature gradients as would occur during reactions in realistic flows. The prime example of such flows are boundary layers in which the wall is at a lower temperature than that of the fluid, as would be the case in Diesel engines. Previous DOE BES work in the program further highlighted the importance of the boundary layer as a configuration for fundamental studies: soot formation in boundary layers is still a problem poorly understood and depends on the availability of particular chemical species at that location, and when boundary layer Large Eddy Simulations results were compared with measurements, the agreement was unfavorable, showing that this important ‘unit’ problem is not well understood. To understand this unit problem, modeling and Direct Numerical Simulations of this unit problem were conducted for the simplest possible multispecies system, that is a binary-species system. The results discovered a new phenomenon, that is, Soret effect induced uphill diffusion. The far-reaching implication is that through an imposed wall/fluid temperature difference it is possible to control the distribution of the species in the boundary layer. Because the results have been documented in one paper published in the refereed literature, and also in conference papers, this final report is in the form of an Executive Summary succinctly describing the results and putting them in perspective with respect to existing information. The refereed and conference papers published are individually listed as Appendices and attached to this report. One manuscript is still in progress and is thus not listed.

74 ATOMIC AND MOLECULAR PHYSICS↗

A PDE Model of Breast Tumor Progression in MMTV-PyMT Mice

The evolution of breast tumors greatly depends on the interaction network among different cell types, including immune cells and cancer cells in the tumor. This study takes advantage of newly collected rich spatio-temporal mouse data to develop a data-driven mathematical model of breast tumors that considers cells’ location and key interactions in the tumor. The results show that cancer cells have a minor presence in the area with the most overall immune cells, and the number of activated immune cells in the tumor is depleted over time when there is no influx of immune cells. Interestingly, in the case of the influx of immune cells, the highest concentrations of both T cells and cancer cells are in the boundary of the tumor, as we use the Robin boundary condition to model the influx of immune cells. In other words, the influx of immune cells causes a dominant outward advection for cancer cells. We also investigate the effect of cells’ diffusion and immune cells’ influx rates in the dynamics of cells in the tumor micro-environment. Sensitivity analyses indicate that cancer cells and adipocytes’ diffusion rates are the most sensitive parameters, followed by influx and diffusion rates of cytotoxic T cells, implying that targeting them is a possible treatment strategy for breast cancer.

60 APPLIED LIFE SCIENCES↗

BETO 2021 Peer Review - Cell Free and Immobilization Technologies (CFIT)

Today, several key factors negatively impact the production of fuels and chemicals from renewable sources. Common hindrances in the biological production of biochemicals are: (1) end-product or intermediate toxicity to the microbial biocatalyst, (2) the diversion of carbon to biomass formation, and (3) co-production of undesired byproducts. A particularly attractive alternative is to eliminate the biocatalyst entirely and instead operate the desired metabolic pathways in isolation, thus circumventing the roadblocks of biological toxicity, lower yields, and lack of specificity. However, cell-free enzyme systems still suffer from low productivities owing in part to the effects of free diffusion of intermediates, lack of long term enzyme stability, cofactor cost or inefficient recycling rates, and finally, the cost of enzyme production/purification. This project represents a new effort to propose innovative and cost competitive routes to producing biochemicals from a variety of feedstocks using cell free approaches. These routes will help reduce the current risk and cost associated with classical cell free production. Cell free technologies show promise for application to the production of toxic/inhibitory products or products difficult to separate from microbial growth media and can help reduce the production barriers in multiple areas of biological conversion of feedstocks to biochemicals.

29 ENERGY PLANNING, POLICY, AND ECONOMY↗

Reduced diffusion and enhanced retention of multiple radionuclides from pore structure characterization of barrier materials for enhanced repository performance

Fluid flow and chemical transport in porous media are the macroscopic consequences of pore structure, which integrates geometry (e.g., pore size and surface area, pore-size distribution) and topology (e.g., pore connectivity). Low-permeability geological media whose pores are poorly interconnected will exhibit the characteristics of anomalous diffusion and sample size-dependent effective porosity, which will strongly impact long-term net diffusion and retention of radionuclides in geological repository settings involving different host rocks and barrier materials. A suite of innovative and complementary experimental approaches is utilized to study the microscopic pore structure and macroscopic fluid flow & chemical transport for a range of host rocks and barrier materials, in addition to standard clay minerals and reference rocks. With a particular focus on quantifying the presence and magnitude of “isolated” pores for a reduced effective porosity in low-permeability geomedia, the integrated methodologies for basic properties and pore structure characterization of these geomedia include X-ray diffraction, thin section petrography, grain size distribution, water immersion porosimetry after vacuum-pulling for full saturation, mercury intrusion porosimetry, nitrogen physisorption, scanning electron microscopy, X-ray computed tomography, and (ultra-)small angle neutron (X-ray) scattering. In addition, custom-designed gas diffusion, tracer recipe involving a range of anionic and cationic chemicals with subsequent analyses by laser ablation and inductively coupled plasma-mass spectrometry, along with batch sorption, column transport, and imbibition tests were conducted for coupled effects of pore structure and chemical retention/transport. From the perspectives of pore structure in conjunction with multiple and complementary approaches to examining a range of sample sizes under different observational scales, we find that the poor pore connectivity is prevalent in low-permeability media (mudstone and crystalline rock) that is related to geological processes (e.g., compaction, diagenesis and thermal maturation). For example, the deep and organic matter-rich mudstones have a much smaller effective porosity than the total porosity (as a result of poor pore connectivity) and associated diffusion coefficient, and the effective porosity & diffusion coefficients are also dependent upon the sample sizes used in the measurement. Similarly, most of the pore space in the shallow mudstone is also controlled by pore-throat diameters in the 5-50 nm range of intergranular pore types from its fine-grained nature, but with an overall good pore connectivity. However, the nm-sized pore space (physically pore-network architecture) and strong sorption capacities (chemical retention from clay minerals) of both shallow and deep mudstones lead to the synergistic retention of cationic radionuclides and their utilities as effective host rocks and barrier materials. Our unique approaches of studying how the micro-scale pore structure affect macro-scale fluid flow, diffusion & retention, and chemical transport produce improved mechanistic understanding, and realistic quantification, of diffusion and retention of typical radionuclides in a range of generic host rocks and barrier materials (clay/shale, salt, crystalline rock, and tuff), with the overall results leading to scientifically-based understanding of enhanced isolation (from both diffusion and retention) of radionuclides and improved confidence on the long-term performance of geological repository to store high-level radioactive wastes. In addition to the training of 25 undergraduates, graduates, and postdocs of UTA, the scientists (organizations) involved in performing this work (e.g., discussion, sample sharing, and operation of SANS and SAXS instruments) include Ed Matteo, Yifeng Wang, and Kristopher Kuhlman (Sandia National Laboratories), Jens Birkholzer, Liange Zheng, Tim Kneafsey, and Sharon Borglin (Lawrence Berkeley National Laboratory), Mavrik Zavarin (Lawrence Livermore National Laboratory), Yukio Tachi and Yuta Fukatsu (Japan Atomic Energy Agency), Mieke de Craen (Euridice, Belgium), Markus Bleuel (NIST), Wei-Ren Chen, Gergely Nagy, Changwoo Do, William Heller, Larry Anovitz, and Kenneth Littrell (ORNL), as well as Jan Illvsky, Ivan Kuzmenko, Ju-Sang Park and Jon Almers (ANL). Key deliverables include a total of 13 peer-reviewed journal articles (nine published and three under review), 23 presentations at scientific conferences (AAPG, AAPG Southwest Section, AGU, Asian Clay Conference, GSA, GSA South-Central Section, IHLRWM, InterPore, International Conference on Chemistry and Migration Behavior of Actinides and Fission Products in the Geosphere, International Conference on Coupled Processes in Fractured Geological Media: Observation, Modeling and Application), and academic institutions (UTA, New Mexico State University; University of Poitiers, France; University of Helsinki, Finland; Uppsala University, Sweden; Istanbul Technical University, Turkey) and other organizations (Andra, France; Posiva Oy, Finland).

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Disentangling the effects of non-adiabatic interactions upon ion self-diffusion within warm dense hydrogen

Warm dense matter is a material state in the region of parameter space connecting condensed matter to classical plasma physics. In this intermediate regime, we investigate the significance of non-adiabatic electron-ion interactions upon ion dynamics. To disentangle non-adiabatic from adiabatic electron-ion interactions, we compare the ion self-diffusion coefficient from the non-adiabatic electron force field computational model with an adiabatic, classical molecular dynamics simulation. A classical pair potential developed through a force-matching algorithm ensures the only difference between the models is due to the electronic inertia. Here, we implement this new method to characterize non-adiabatic effects on the self-diffusion of warm dense hydrogen over a wide range of temperatures and densities. Ultimately we show that the impact of non-adiabatic effects is negligible for equilibrium ion dynamics in warm dense hydrogen.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Dust-void evolution driven by turbulent dust flux can induce runaway migration of Earth-mass planets

Torques from asymmetric dust structures (so-called dust-void and filamentary structures) formed around low-mass planets embedded in a nonturbulent dust-gas disk can exceed the torques produced by the gas disk component and then go on to dominate the planet’s orbital dynamics. Here, we investigate how these structures (hence the dust torque) change when the effect of turbulent dust diffusion and dust feedback are included, along with the direct implications on the migration of Earth-like planets. Using the FARGO3D code, we performed 2D and 3D multifluid hydrodynamic simulations, focusing on a non-migrating planet with a mass of M p = 1.5 M ⊕ in 2D and on migrating planets with M p ∈ [1.5, 12] M ⊕ in 3D. We varied the δ-dimensionless diffusivity parameter in the range [0, 3 × 10 −3 ] and considered three different Stokes numbers, St = {0.04, 0.26, 0.55}, which are representative of the gas-dominated, the transitional, and the gravity-dominated regimes, respectively. In our 2D models, we find that turbulent diffusion of dust prevents the formation of the dust-void and filamentary structures when δ > 3 × 10 −4 . Otherwise, dust structures survive turbulent diffusion flow. However, dust and total torques become positive only in transitional and gravity-dominated regimes. In our 3D models, we find that the dust-void is drastically modified and the high-density ring-shaped barrier delineating the dust-void disappears if δ ≳ 10 −4 , due to the effect of dust turbulent diffusion along with the back-reaction of the dust. For all values of δ, the filament in front of the planet is replaced by a low-density trench. Remarkably, as we have allowed the planets to migrate, the evolving dust-void can drive either runaway migration or outward (inward) oscillatory-torque migration. Our study thus suggests that low-mass Earth-like planets can undergo runaway migration in dusty disks.

79 ASTRONOMY AND ASTROPHYSICS↗

Simulations of self- and Xe diffusivity in uranium mononitride including chemistry and irradiation effects

A combination of density functional theory and empirical potential atomic scale simulations have been used to determine a model for defect stability and mobility in uranium mononitride (UN), as a function of temperature (T) and N 2 partial pressure (p N 2 ). Using the model, predictions of hypo-stoichiometry under U-rich conditions compare favorably to CALPHAD calculations using the TAF-ID database. Furthermore, our predictions of U and N self-diffusivity are in good agreement with experiments carried out as a function of T at specific partial pressures under thermal equilibrium. The validated atomic scale data have then been implemented within a cluster dynamics method to simulate irradiation-enhanced defect concentrations. All defects and clusters studied have significantly enhanced concentrations, with respect to thermal equilibrium, as T is lowered. The irradiation-enhanced Xe diffusivity is compared to post-irradiation annealing and in-pile experiments. In conclusion, the contributions of various defects and clusters to non-stoichiometry, self-diffusivity, and Xe diffusivity are discussed.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗

Tackling the curse of dimensionality in fractional and tempered fractional PDEs with physics-informed neural networks

Fractional and tempered fractional partial differential equations (PDEs) are effective models of long-range interactions, anomalous diffusion, and non-local effects. Traditional numerical methods for these problems are mesh-based, thus struggling with the curse of dimensionality (CoD). Physics-informed neural networks (PINNs) offer a promising solution due to their universal approximation, generalization ability, and mesh-free training. In principle, Monte Carlo fractional PINN (MC-fPINN) estimates fractional derivatives using Monte Carlo methods and thus could lift CoD. However, this may cause significant variance and errors, hence affecting convergence; in addition, MC-fPINN is sensitive to hyperparameters. In general, numerical methods and specifically PINNs for tempered fractional PDEs are under-developed. Herein, we extend MC-fPINN to tempered fractional PDEs to address these issues, resulting in the Monte Carlo tempered fractional PINN (MC-tfPINN). To reduce possible high variance and errors from Monte Carlo sampling, we replace the one-dimensional (1D) Monte Carlo with 1D Gaussian quadrature, applicable to both MC-fPINN and MC-tfPINN. We validate our methods on various forward and inverse problems of fractional and tempered fractional PDEs, scaling up to 100,000 dimensions. Our improved MC-fPINN/MC-tfPINN using quadrature consistently outperforms the original versions in accuracy and convergence speed in very high dimensions.

42 ENGINEERING↗

Thermal diffusivity and thermal conductivity of SiC composite tubes: the effects of microstructure and irradiation

Cladding thermal conductivity is an important physical property in assessing the performance of silicon carbide (SiC)-cladded fuels for nuclear reactors. However, there is a significant lack of reliable data, particularly for irradiated materials, because the geometry complicates the measurement. This study investigates the thermal diffusivity of coupons with a curvature, machined from SiC fiber–reinforced SiC matrix composite tubes, with and without neutron irradiation under light water reactor–relevant temperature and dose conditions. The tested materials included full composite and duplex SiC composite tubes. The measurements were conducted using a modern flash diffusivity apparatus. The analyzed area on the specimen during diffusivity testing was reduced for improved measurement accuracy due to sample curvature. Post-irradiation measurements showed that the effects of neutron irradiation on thermal conductivity (e.g. thermal defect resistivity) are different between SiC composite plates versus tubes. The difference was explained by higher matrix density of the tube than the plate. This study provides reliable thermal properties of prototypic SiC composite tubes useful for fuel performance modeling of SiC-based cladding.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗