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At least 1,189 records · Page 66

Radiation Transport in Random Media With Large Fluctuations

Strongly heterogeneous media arise in several applications that include radiation shields, nuclear fuel, BWR moderators, clouds, planetary and stellar atmospheres, turbulent gases and plasmas. Neutral and charged particle transport computations in such media have relied heavily on formulating transport equations with spatially random coefficients (physical data) and developing solution methods to deal with the additional stochastic dimensions. Attempts at developing approximate closures that yield only low order statistical information (e.g., mean and variance of the flux) have proved to be highly restrictive under real physics conditions or rely on techniques that require fluctuation amplitudes to be small for robustness. Recently, stochastic spectral methods such as polynomial chaos and stochastic collocation have been developed for aleatoric uncertainty quantification and sensitivity analysis, and successfully applied in radiation transport work. Advances in UQ techniques have tended to focus on efficiently handling large numbers of uncertain variables but the rigorous stochastic basis of the approach also promotes its use in situations where stochasticity is due to spatial heterogeneity and the associated uncertainty is large. Here we apply these techniques to radiation transport in media with spatially randomly varying cross sections without restriction on fluctuation amplitudes. Specifically, we represent the cross sections as a lognormal spatial random process with specified mean, variance and covariance function and use a Karhunen-Loeve (KL) decomposition to generate cross section realizations that are strictly positive. Woodcock Monte Carlo (WMC) is then used to simulate transport using random sampling of cross sections and deterministic sampling based on a stochastic collocation technique. Numerical results for the mean and variance in the scalar flux and leakage currents are obtained for weak and strong random variations. We focus in this work on demonstrating the approach and defer application to specific problems to a future investigation. We have demonstrated that a combination of stochastic spectral representation and Woodcock Monte Carlo simulation allows efficient computation of radiation transport in strongly random media. The use of a lognormal distribution to represent the fluctuations in medium properties facilitates enforcement of strict positivity of cross section realizations, a condition that has challenged standard approaches that assume Gaussian fluctuations. The fact that the lognormal random process is a memoryless nonlinear transformation of a Gaussian process further enables efficient and accurate reconstruction of the random cross section realizations using a Karhunen-Loeve representation of the cross section. Finally, the robustness of this model enables fluctuations of arbitrarily large amplitude to be studied, using both random sampling Monte Carlo and more efficient stochastic collocation techniques. The present work is being extended to allow reconstruction of probability density functions of output variables using polynomial chaos representation, and to accommodate general cross section covariance functions. Also, techniques are being explored to more judiciously select ceiling cross sections to enhance the efficiency of Woodcock Monte Carlo for transport in random media. (authors)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Interactive Visualization of Multi-Group Cross Sections on High-Fidelity Spatial Meshes

Core simulation tools utilizing Monte Carlo transport methods represent the 'Holy Grail' for nuclear reactor analysis. However, deterministic transport methods pose a number of advantages to Monte Carlo from a computational perspective, which seems likely to make these methods more viable in the near to intermediate term. Deterministic methods almost universally discretize the energy domain in a few to hundreds of energy groups. One of the key challenges for deterministic transport-based methods to be viable is accurate, reactor agnostic multi-group cross section generation. This paper describes tools for data processing and visualization of multigroup cross sections generated on high-fidelity spatial meshes from the OpenMC Monte Carlo code. Next generation deterministic transport reactor core modeling tools will require multi-group cross section (MGXS) generation on high-fidelity spatial meshes. High-fidelity MGXS are necessary for the accurate simulation of neutron physics in nuclear reactors with a high degree of spectral heterogeneity - e.g., large localized neutron flux gradients throughout a reactor core. Although many local (e.g., pin cell) approximations have been developed to model the scalar flux to compute spectral-averaged MGXS, these techniques cannot account for complex intra-pin and intra-assembly spatial self-shielding effects. Monte Carlo presents the most accurate method for reactor agnostic multi-group cross section generation since it does not require the use of local approximations to the flux. Monte Carlo has been proposed as a highly desirable framework for reactor agnostic cross section generation for many years. Monte Carlo methods can effectively embed all of the relevant spectral effects into the MGXS through the random particle tracking and interaction sampling processes. Previous work has applied MCNP and Serpent to compute few-group constants for diffusion calculations, and OpenMC to compute multi-group cross sections for transport-based methods. The primary difficulty with using Monte Carlo for MGXS generation is the tremendous computational resources required to adequately converge multi-group cross sections in each spatial region and energy group. Recent development of the OpenMC Monte Carlo code for high-performance computing platforms has made multigroup cross section generation from Monte Carlo more tractable in the foreseeable future. The recent release of OpenMC v0.7.1 includes a new Python-based module for MGXS generation. The MGXS generation module leverages many of the algorithms and features for 'big data' analysis of large tally datasets on complex spatial meshes. This paper describes the data management workflow and visualization tools which have been developed to explore the plethora of MGXS data generated with OpenMC. It is the authors' hope that the development of the visualization tool described in this paper will ultimately enable the design of machine learning algorithms to accelerate the convergence rate of high-fidelity multi-group cross section generated with Monte Carlo. (authors)

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Pressure and fluid-driven fracture propagation in porous media using an adaptive finite element phase field model

This work presents phase field fracture modeling in heterogeneous porous media. We develop robust and efficient numerical algorithms for pressure-driven and fluid-driven settings in which the focus relies on mesh adaptivity in order to save computational cost for large-scale 3D applications. In the fluid-driven framework, we solve for three unknowns pressure, displacements and phase field that are treated with a fixed-stress iteration in which the pressure and the displacement–phase-field system are decoupled. The latter subsystem is solved with a combined Newton approach employing a primal–dual active set method in order to account for crack irreversibility. Numerical examples for pressurized fractures and fluid filled fracture propagation in heterogeneous porous media demonstrate our developments. Finally in particular, mesh refinement allows us to perform systematic studies with respect to the spatial discretization parameter.

42 ENGINEERING↗

Are upwind techniques in multi-phase flow models necessary?

Two alternatives of primary variables are compared for two-phase flow in heterogeneous media by solving fully established benchmarks. The first combination utilizes pressure of the wetting fluid and saturation of the non-wetting fluid as primary variables, while the second employs capillary pressure of the wetting fluid and pressure of the non-wetting fluid. While the standard Galerkin finite element method (SGFEM) is known to fail in the physical reproduction of two-phase flow in heterogeneous media (unless employing a fully upwind correction), the second scheme with capillary pressure as a primary variable without applying an upwind technique produces correct physical fluid behaviour in heterogeneous media, as observed from experiments.

97 MATHEMATICS AND COMPUTING↗

Low-Overhead In Situ Visualization Using Halo Replay

In situ visualization and analysis is of increasing importance as the compute and I/O gap further widens with the advance to exascale capable computing. Yet, in situ methods impose resource constraints leading to the difficult task of balancing simulation code performance and the quality of analysis. Applications with tightly-coupled in situ visualization often achieve performance through spatial and temporal downsampling, a tradeoff which risks not capturing transient phenomena at sufficient fidelity. Determining a priori visualization parameters such as sampling rate is difficult without time and resource intensive experimentation. We present a method for reducing resource contention between in situ visualization and stencil codes on heterogeneous systems. This method permits full resolution replay through recording halos and the communication-free reconstruction of interior values uncoupled from the main simulation. We apply this method in the computational fluid dynamics (CFD) code HARVEY [1] on the Summit supercomputer. We demonstrate minimal-overhead, in situ visualization relative to simulation alone, and compare the Halo Replay performance to tightly-coupled in situ approaches.

Ames, Jeff↗

High-Resolution Comonomer Sequencing of Blocky Brominated Syndiotactic Polystyrene Copolymers Using 13C NMR Spectroscopy and Computer Simulations

This work demonstrates the first high-resolution comonomer sequencing of Blocky brominated syndiotactic polystyrene (sPS-co-sPS-Br) copolymers based on pentad assign- ments of the quaternary carbon region of the nuclear magnetic resonance spectrum. Copolymers containing p-bromostyrene (Br-Sty) units were prepared in matched sets using postpolymerization bromination methods carried out in the heterogeneous gel state (Blocky) and homogeneous solution state (Random). Quantitative information from the quaternary carbon spectra, heteronuclear multiple bond correlation spectroscopy, electronic structure calculations, and simulated statistically random copolymers was correlated to confirm the carbon resonance assignments for all 20 possible pentad comonomer sequences. Using the experimental pentad sequence prevalences, a computer code was developed to simulate chains with microstructures typical of each sample as a means to visually represent the copolymer blockiness with quantitative precision. Based on the microstructure and distribution of run lengths in these chains, the simulations revealed that the Blocky copolymers contain a high degree of blockiness. By comparing the run lengths in the simulated chains to the average number of styrene units in a crystalline segment of sPS (found by small-angle X-ray scattering), copolymer crystallizability was predicted. For the simulated Blocky B-21% (21 mol % Br-Sty) chain, the probability of randomly selecting a styrene unit in a crystallizable block was 25.8%, while that in the simulated Random R-18% was zero, in excellent agreement with the experimental crystallization behavior measured by differential scanning calorimetry. Additionally, these predictions confirmed that the simulated chains accurately represent the ensemble of chains in their respective copolymer samples. Furthermore, each simulated Blocky chain contained one or more long sPS blocks that paralleled the measured 38-40 styrene units spanning a crystalline segment within the sPS/CCl4 gel. This finding affirmed that the long sPS segments originated from the precise lamellar structure within the heterogeneous gel morphology (i.e., block length is correlated with lamellar thickness). Overall, the ability to tailor the copolymer microstructure through control of the semicrystalline gel morphology opens the door to synthesizing ordered copolymers by postpolymerization functionalization processes with unprecedented levels of compositional control.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Probing the Role of Multi-scale Heterogeneity in Graphite Electrodes for Extreme Fast Charging

Electrode-scale heterogeneity can combine with complex electrochemical interactions to impede lithium-ion battery performance, particularly during fast charging. This research investigates the influence of electrode heterogeneity at different scales on the lithium-ion battery electrochemical performance under operational extremes. We employ image-based mesoscale simulation in conjunction with a three-dimensional electrochemical model to predict performance variability in 14 graphite electrode X-ray computed tomography data sets. Our analysis reveals that the tortuous anisotropy stemming from the variable particle morphology has a dominating influence on the overall cell performance. Cells with platelet morphology achieve lower capacity, higher heat generation rates, and severe plating under extreme fast charge conditions. On the contrary, the heterogeneity due to the active material clustering alone has minimal impact. Our work suggests that manufacturing electrodes with more homogeneous and isotropic particle morphology will improve electrochemical performance and improve safety, enabling electromobility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

MO-A-BRD-05: Evaluation of Composed Lung Ventilation with 4DCT and Image Registration

Purpose: Regional pulmonary function can be derived using fourdimensional computed tomography (4DCT) combined with deformable image registration. However, only peak inhale and exhale phases have been used thus far while the lung ventilation during intermediate phases is not considered. In our previous work, we have investigated the spatiotemporal heterogeneity of lung ventilation and its dependence on respiration effort. In this study, composed ventilation is introduced using all inspiration phases and compared to direct ventilation. Both methods are evaluated against Xe-CT derived ventilation. Methods: Using an in-house tissue volume preserving deformable image registration, unlike the direct ventilation method, which computes from end expiration to end inspiration, Jacobian ventilation maps were computed from one inhale phase to the next and then composed from all inspiration steps. The two methods were compared in both patients prior to RT and mechanically ventilated sheep subjects. In addition, they wereassessed for the correlation with Xe-CT derived ventilation in sheep subjects. Annotated lung landmarks were used to evaluate the accuracy of original and composed deformation field. Results: After registration, the landmark distance for composed deformation field was always higher than that for direct deformation field (0IN to 100IN average in human: 1.03 vs 1.53, p=0.001, and in sheep: 0.80 vs0.94, p=0.009), and both increased with longer phase interval. Direct and composed ventilation maps were similar in both sheep (gamma pass rate 87.6) and human subjects (gamma pass rate 71.9),and showed consistent pattern from ventral to dorsal when compared to Xe-CT derived ventilation. Correlation coefficient between Xe-CT and composed ventilation was slightly better than the direct method but not significant (average 0.89 vs 0.85, p=0.135). Conclusion: More strict breathing control in sheep subjects may explain higher similarity between direct and composed ventilation. When compared to Xe-CT ventilation, no significant difference was found for the composed method. NIH Grant: R01 CA166703.

60 APPLIED LIFE SCIENCES↗

Site heterogeneity and broad surface-binding isotherms in modern catalysis: Building intuition beyond the Sabatier principle

Learning the science of heterogeneous catalysis and electrocatalysis always starts with the simple case of a flat, uniform surface with an ideal adsorbate. It has of course been recognized for a century that real catalysts are more complicated. For the increasingly complex catalysts of the 21st century, this Perspective argues that surface heterogeneity and non-ideal binding isotherms are central features, and their implications need to be incorporated in current thinking. A variety of systems are described herein where catalyst complexity leads to broad, non-Langmuirian surface isotherms for the binding of hydrogen atoms – and this occurs even for ideal, flat Pt(111) surfaces. Modern catalysis employs nanoscale materials whose surfaces have substantial step, edge, corner, impurity, and other defect sites, and they increasingly have both metallic and non-metallic elements M n X m , including metal oxides, chalcogenides, pnictides, carbides, doped carbons, etc. The surfaces of such catalysts are often not crystal facets of the bulk phase underneath, and they typically have a variety of potential active sites. Catalytic surfaces in operando are often non-stoichiometric, amorphous, dynamic, and impure, and often vary from one part of the surface to another. Understanding of the issues that arise at such nanoscale, multi-element catalysts is just beginning to emerge. Yet these catalysts are widely discussed using Brønsted/Bell-Evans-Polanyi (BEP) relations, volcano plots, Tafel slopes, the Butler-Volmer equation, and other linear free energy relations (LFERs), which all depend on the implicit assumption that the active sites are “similar” and that surface adsorption is close to ideal. These assumptions underly the ubiquitous intuition based on the Sabatier Principle, that the fastest catalysis will occur when key intermediates have free energies of adsorption that are not too strong nor too weak. Current catalysis research often aims to minimize the complexity of non-ideal isotherms through experimental and computational design (e.g., the use of single crystal surfaces), and these studies are the foundation of the field. In contrast, this Perspective argues that the heterogeneity of binding sites and binding energies is an inherent strength of these catalysts. Here, this diversity makes many nanoscale catalysts inherently a high-throughput screen wrapped in a tiny package. Only by making the heterogeneity part of the foundation of catalysis models, sorting the types of active sites and dissecting non-ideal binding isotherms, will modern catalysis learn to harness the inherent diversity of real catalysts. Controlling and exploiting diversity rather than avoiding it will help to optimize complex modern catalysts and catalytic conditions.

Mayer, James M.↗

Establishing a geochemical heterogeneity model for a contaminated vadose zone – Aquifer system

A large set of sediment samples from a 1600 m2 experimental plot within a 2.2 km2 vadose zone and groundwater uranium (VI) plume were subject to physical, chemical, and mineralogic characterization. The plot is being used for field experimentation on U(VI) recharge and transport processes within a persistent groundwater plume that exists in the groundwater-river interaction zone of the Columbia River at the U.S. DOE Hanford site. The samples were obtained during the installation of 35 tightly spaced (10 m separation) groundwater monitoring wells. The characterization measurements for each sample included total contaminant concentrations (U and Cu primarily), bicarbonate extractable U(VI), sequential 238U(VI) contaminant desorption Kd, 233U(VI) adsorption Kd, grain size distribution, surface area, extractable poorly crystalline Fe(III) oxides, and mineralogy. The characterization objective was to inform a conceptual model of coupled processes controlling the anomalous longevity of the plume, and to quantify the spatial heterogeneity of the contaminant inventory and the primary properties effecting reactive transport. Correlations were drawn between chemical, physical, and reaction properties, and Gaussian simulation was used to compute multiple 3-D realizations of extractable U(VI), the 233U(VI) adsorption Kd, and the distribution of the reactive < 2 mm fraction. Adsorbed contaminant U(VI) was highest in the vadose zone and the zone of seasonal water table fluctuation lying at its base. Adsorbed U(VI) was measureable, but low, in the groundwater plume region where very high hydraulic conductivities existed. The distribution of adsorbed U(VI) displayed no apparent correlation with sediment physical or chemical properties. Desorption [238U(IV)] and adsorption [233U(VI)] Kd values showed appreciable differences due to mass transfer controlled surface complexation and the effects of long subsurface residence times. The 233U(VI) adsorption Kd, a combined measure of surface complexation strength and site concentration, was relatively uniform throughout the domain, displaying correlation with fines distribution and surface area. The characterization results revealed U(VI) supplied to the groundwater plume through spatially heterogeneous recharge from residual contamination in the zone of seasonal water table fluctuation, and transport of U(VI) controlled by weak, kinetically-controlled surface complexation in the coarse-textured saturated zone. Geostatistical relationships for the adsorbed contaminant U distribution in the characterization domain allow an extrapolation to inventory at the plume scale, a critical unknown for remedial action.

contaminant heterogeniety, uranium groundwater plu↗

Solution and Interface Structure and Dynamics in Geochemistry: Gateway to Link Elementary Processes to Mineral Nucleation and Growth

Our understanding of the process of mineral nucleation is starting to evolve from the solely thermodynamical aspects in classical nucleation theory toward a mechanistic study of reactions influenced by solvation structures of ions and their dynamics. A knowledge of how these atomic and molecular interactions respond to changing solution composition and/or the nature of an interface will form a fundamental foundation to understand rate-limiting reactions and processes for nucleation and growth. Here, we review recent advances from multidisciplinary experimental and computational approaches of the structure and dynamics of aqueous solutions and mineral–liquid interfaces that will influence rates of nucleation (and growth behavior) both homogeneously in aqueous solutions and heterogeneously at mineral–liquid interfaces. Furthermore, these processes include structure (and extent) of solute clustering, solvent degrees of freedom, and the presence of noninnocent charge-balancing ions, all of which can drive the selectivity and exert control over nucleation mechanisms. Similar controlling reactions can also occur at interfaces with the added complexities of how solute ions interact with and assemble on surface sites and use different mechanisms from bulk solutes, such as lateral solvent exchanges between distinct surface sites. To gain a predictive understanding of nucleation chemistry, we emphasize several key knowledge gaps that will need to be addressed in this field and highlight the importance of combining computations and experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Shaping the Future of Self-Driving Autonomous Laboratories Workshop

The "Shaping the Future of Self-Driving Autonomous Laboratories" workshop, held in Denver on November 7-8, 2024, brought together leading experts from materials science and computing to address the growing need to revolutionize scientific research through AI-driven autonomous laboratories. The workshop identified critical challenges, including the integration of heterogeneous data, development of AI systems that understand fundamental physical principles, and comprehensive safety protocols. Key recommendations emerged around developing universal laboratory equipment interfaces, implementing automated metadata collection systems, and creating hybrid AI approaches that combine data-driven learning with scientific principles. The workshop emphasized maintaining human oversight while leveraging automation, transforming scientific education to prepare the next generation of researchers, and establishing a national consortium leveraging DOE facilities as anchors for broader collaboration with academia and industry. Participants stressed the urgency of addressing the growing disconnect between human decision-making timescales and modern instrumentation capabilities, highlighting the need for strategic automation while preserving essential human insight and oversight in the research process.

36 MATERIALS SCIENCE↗

On data-driven energy flexibility quantification: A framework and case study

Building energy flexibility is an important resource for a sustainable and resilient power grid, and an important measure to reduce utility costs for building owners. Quantifying energy flexibility for existing buildings can provide critical insights in optimizing their operation. Data-driven methods for building energy modeling and analytics are gaining popularity due to the increasingly available sensor and meter infrastructure, affordable computational resources, and advanced modeling algorithms. However, their application in quantifying the energy flexibility of real buildings is still limited due to the heterogeneous data types and limited data availability. Here, this study proposes a framework for building-level data-driven energy flexibility quantification that considers different levels of data availability and use cases. Two case studies with real building data collected at different scales were conducted to demonstrate the proposed framework for different purposes.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗

Privacy-Preserving Federated Learning for Science: Challenges and Research Directions

This paper discusses the key challenges and future research directions for privacy-preserving federated learning (PPFL), with a focus on its application to large-scale scientific AI models, in particular, foundation models~(FMs). PPFL enables collaborative model training across distributed datasets while preserving privacy-- an important collaborative approach for science. We discuss the need for efficient and scalable algorithms to address the increasing complexity of FMs, particularly when dealing with heterogeneous clients. In addition, we underscore the need for developing advance privacy-preserving techniques, such as differential privacy, to balance privacy and utility in large FMs emphasizing fairness and incentive mechanisms to ensure equitable participation among heterogeneous clients. Finally, we emphasize the need for a robust software stack supporting scalable and secure PPFL deployments across multiple high-performance computing facilities. We envision that PPFL would play a crucial role to advance scientific discovery and enable large-scale, privacy-aware collaborations across science domains.

Kim, Kibaek [Argonne National Laboratory (ANL)]↗