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At least 109 records · Page 6

FInal Report: First Principles Modeling of Mechanisms Underlying Scintillator Non-Proportionality

This final report presents work carried out on the project “First Principles Modeling of Mechanisms Underlying Scintillator Non-Proportionality” at Lawrence Livermore National Laboratory during 2013-2015. The scope of the work was to further the physical understanding of the microscopic mechanisms behind scintillator nonproportionality that effectively limits the achievable detector resolution. Thereby, crucial quantitative data for these processes as input to large-scale simulation codes has been provided. In particular, this project was divided into three tasks: (i) Quantum mechanical rates of non-radiative quenching, (ii) The thermodynamics of point defects and dopants, and (iii) Formation and migration of self-trapped polarons. The progress and results of each of these subtasks are detailed.

36 MATERIALS SCIENCE↗

LL13-MatModelRadDetect-PD2Jf Final Report: Materials Modeling for High-Performance Radiation Detectors

The aims of this project are to enable rational materials design for select high-payoff challenges in radiation detection materials by using state-of-the-art predictive atomistic modeling techniques. Three specific high-impact challenges are addressed: (i) design and optimization of electrical contact stacks for TlBr detectors to stabilize temporal response at room-temperature; (ii) identification of chemical design principles of host glass materials for large-volume, low-cost, highperformance glass scintillators; and (iii) determination of the electrical impacts of dislocation networks in Cd 1-x Zn x Te (CZT) that limit its performance and usable single-crystal volume. The specific goals are to establish design and process strategies to achieve improved materials for high performance detectors. Each of the major tasks is discussed below in three sections, which include the goals for the task and a summary of the major results, followed by a listing of publications that contain the full details, including details of the methodologies used. The appendix lists 12 conference presentations given for this project, including 1 invited talk and 1 invited poster.

36 MATERIALS SCIENCE↗

Progress Summary: Solid-state NMR spectroscopic methods are being used to deduce the molecular structure of degradation products in Material 2

Detrimental outgassing occurs due to the radiolitic and thermal degradation of Materials 2. The specific degradation pathway is yet unknown but thought to involve the formation of long lived radical species in addition to stable products. The task in this project is to use a combination of NMR and EPR spectroscopic methods to identify the major degradation products. The end goal is to develop reaction pathways that better inform models of outgassing from Material 2.

36 MATERIALS SCIENCE↗

University of Minnesota, Twin Cities Final Scientific/Technical Report Small Scale Ammonia Synthesis Using Stranded Wind Energy

Ammonia absorber columns offer an alternative separation unit to replace condensation in the Haber-Bosch synthesis loop. Metal halide salts can selectively separate ammonia from the reactor outlet gas mixture and incorporate it into their crystal lattice with remarkably high thermodynamic capacity. While the salts’ working capacity can be limited and unstable when they are in their pure form, the capacity is stable and can be high when using a porous ceramic support. In this project, we found optimal conditions for sorbent fabrication, we demonstrated benchmark levels of uptake and release of ammonia, and we fabricated and demonstrated a prototype at a scale of 1 kg/day ammonia. This task allowed us to assess improvement in the techno-economic prospects for this new separation approach, making viable more distributed production of green ammonia from geographically dispersed renewable energy sources.

08 HYDROGEN↗

Light Water Reactor Sustainability: Program Materials Research Pathway (FY22 Technical Program Plan)

The Materials Research (MR) Pathway within the Light Water Reactor Sustainability (LWRS) program is charged with performing R&D to develop the scientific basis for understanding and predicting the long-term environmental degradation behavior of materials in nuclear reactors. Furthermore, the mechanistic understanding of degradation phenomena in materials must be leveraged to develop mitigation and repair strategies and new material alternatives for existing components. This research will provide data and methods to assess the performance of systems, structures, and components essential to safe and sustained reactor operations. The R&D products developed from the LWRS program will be used by stakeholders—including utilities, industry groups, and regulators—to inform operational and regulatory requirements for materials in reactor systems, structures, and components subjected to long-term operation conditions, providing key inputs to regulators and industry. Therefore, the intent of this research is to provide options to reduce the operating costs, which may be in the form of offset maintenance costs due to better predictive models for component lifetimes, improved analyses of materials through nondestructive evaluation, reduced costs for repairs, or extended performance of plants through the selection of improved replacement materials. To provide the best options, industry experience and guidance are important because of their role in coordinated or collaborative research projects. The objectives of this report are to describe the motivation and organization of the MR Pathway within the LWRS program; provide details on the individual research tasks within the MR Pathway; describe the outcomes and deliverables of the MR Pathway, including recent technical highlights and progress; and describe the requirements for performing this critically important research.

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Multi-Task with Procter and Gamble (CRADA No. NFE-10-02672)

The purpose of this Cooperative Research and Development Agreement (CRADA) between UT-Battelle, LLC (the “Contractor) and Procter & Gamble Company (the “Participant”) is the development of a research partnership to create new tools, tests and analytical methods to improve the performance, safety and/or environmental quality of chemicals, advanced materials, food products and manufacturing processes. The Participant operates in three global business units: Beauty, Health and Well-Being and Household Care. Some of its worldwide products include Head and Shoulders®, Pantene®, Gillette® razors and personal care products, Crest®, Dawn®, Tide®, Bounty®, Duracell® batteries; and Iams® pet food among others. At its core, however, the Participant is a science driven company. It supports one of the most robust industrial research and development (R&D) programs in the world. The Participant uses this rich foundation of science to drive innovation across all of its product lines. But the innovation process is not confined in-house The Participant pursues an “open innovation” policy, seeking partnerships with scientists and researchers in universities and national laboratories where it can contribute its extensive knowledge assets and collaborate to advance scientific understanding. The research under this multi-task CRADA was directed under the following general task areas and, throughout the duration of this CRADA the work statement was modified to match the needs of the Parties and the direction of the research. (1) Software modeling, simulation and development; (2) Manufacturing Technologies; (3) Supply Chain Optimization, (4) Advanced Materials.

36 MATERIALS SCIENCE↗

Code interoperability extends the scope of quantum simulations

The functionality of many materials is critically dependent on the integration of dissimilar components and on the interfaces that arise between them. The description of such heterogeneous components requires the development and deployment of first principles methods, coupled to appropriate dynamical descriptions of matter and advanced sampling techniques, in order to capture all the relevant length and time scales of importance to the materials’ performance. It is thus essential to build simple, streamlined computational schemes for the prediction and design of multiple properties of broad classes of materials, by developing interoperable codes which can be efficiently coupled to each other to perform complex tasks. We discuss the use of interoperable codes to simulate the structural and spectroscopic characterization of materials, including chemical reactions for catalysis, the description of defects for quantum information science, and heat and charge transport.

36 MATERIALS SCIENCE↗

Epitaxial intergrowths and local oxide relaxations in natural bixbyite Fe 2– x Mn x O 3

The scattering pattern of a crystal obeys the symmetry of the crystal structure through the corresponding Laue group. This is usually also true for the diffuse scattering, containing information about disorder, but here a case is reported where the diffuse scattering is of lower symmetry than the parent crystal structure. The mineral bixbyite has been studied by X-ray and neutron scattering techniques since 1928 with some of the most recent studies characterizing the low-temperature transition to a magnetically disordered spin-glass state. However, bixbyite also exhibits structural disorder, and here single-crystal X-ray and neutron scattering is used to characterize the different modes of disorder present. One-dimensional rods of diffuse scattering are observed in the cubic mineral bixbyite, which break the expected symmetry of the scattering pattern. It is shown that this scattering arises from epitaxial intergrowths of the related mineral, braunite. The presence of this disorder mode is found to be directly observable as well-defined residuals in the average structure refined against the Bragg diffraction. An additional three-dimensional diffuse scattering component is observed in neutron scattering data, which is shown to originate from the substitutional disorder on the Fe/Mn sites. This occupational disorder gives rise to local relaxations of the oxide sublattice, and the pattern of oxide displacements can be rationalized based on crystal-field theory. The combined use of neutron and X-ray single-crystal scattering techniques highlights their great complementarity. In particular, the large sample requirements for neutron scattering experiments prove to be an obstacle in solving the intergrowth disorder due to several growth orientations, whereas for X-ray scattering the one-dimensional nature of the intergrowth disorder renders solving this a more tractable task. On the other hand, the oxide relaxations cannot be resolved using X-rays due to the low Mn/Fe contrast. By combining the two approaches both types of disorder have been characterized.

36 MATERIALS SCIENCE↗

Evaluating Corrosion Effects on the Stainless Steel Components of the SAVY-4000/Hagan Nuclear Material Storage Containers: FY2022 Update

This report summarizes the work completed and underway for the Corrosion Working Group (CWG) for FY2022 in support of evaluating a greater than a 15 year design life for the SAVY4000. The CWG meets on an as needed basis to review new work, results or information regarding the corrosion of SAVY-4000 and Hagan nuclear material storage containers. The goal when analyzing corrosion is to develop a design life appropriate for the containers and to identify when a container should be removed from service. There are many parallel efforts associated with identifying and extending the service life of nuclear material storage containers. This report includes information from research and development efforts to address the lifetime. The CWG is closely related to surveillance activities and continues to play a role in identification of issues and paths forward for analysis of surveillance containers. This work summarizes the completed tasks for FY22 of the CWG while keeping in mind that some efforts continue into future years. Brief summaries of identified new avenues of work have been identified for FY23.

36 MATERIALS SCIENCE↗

Community-Driven Methods for Open and Reproducible Software Tools for Analyzing Datasets from Atom Probe Microscopy

Atom probe tomography, and related methods, probe the three-dimensional architecture of a material. The software tools that microscopists use, and how these tools are connected into workflows, makes a substantial contribution to the accuracy and precision of such a material characterization experiment. Typically, we adapt methods from other communities like mathematics, data science, computational geometry, artificial intelligence, or scientific computing. We also realize that improving on research data management is a challenge when it comes to align with the FAIR data stewardship principles. Faced with this global challenge, we are convinced that collaborating is useful. Here, we report the results and challenges with an inter-laboratory call for developing test cases for several types of atom probe software tools. The results support why defining detailed recipes of software workflows and sharing these recipes is necessary and rewarding: Open source tools and (meta)data exchange can help to make our day-to-day data processing tasks become more efficient, the training of new users and knowledge transfer become easier, and assist us with automated quantification of uncertainties to gain access to substantiated results.

36 MATERIALS SCIENCE↗

Development and Characterization of High Performance and Robust Mixed Conducting Cathodes Supportive of Lower Cost Solid Oxide Fuel Cells (Final Report)

The objective of the proposed research is to advance an existing partnership between the University of South Carolina (USC) and LG Fuel Cell Systems, Inc. (LGFCS) to research and develop mixed electronic and ionic conducting cathode materials for durable and robust low-cost solid oxide fuel cells (SOFCs). The first task is to develop mixed ionic and electronic conducting doped (Pr,Nd)NiO 4 (PNNO)-based cathodes. This task is built on a prior collaborative work with LG Fuel Cell System, which showed that doped PNNO could exhibit phase stability at high temperatures. The initial focus will be on investigating the durability and endurance of its electrochemical performance and the temporal evolution of microstructures. In-situ high temperature neutron diffraction and x-ray diffraction will be used to study the structures of these phase stable compounds. PNNO doped with Ca and transition metal elements will be synthesized. Physical properties of these materials with respect to coefficient of thermal expansion, electrical conductivity, diffusion coefficient, and nonstoichiometry will be measured. The benefits of dense versus porous barriers will be studied and the role of barrier layer will be identified and a guideline will be provided to choose the maximum porosity for durable and robust cathode performance with co-doped PNNO as the cathodes. LSCF6428 will be used to compare its power density with that of co-doped PNNO in the absence of Cr, but some studies comparing Cr tolerance will be performed towards the end of the project. The conditions at which preferred nickelate phases are stable will be defined, including sintering temperature, operating temperature, and composition range. The second task will focus on the investigation of the location of degradation by using differential relaxation time (DRT) analysis, coupled with least squares fitting and systematical post analyses. DRT analysis can provide (1) a direct access to the kinetic parameters of the underlying processes in both cathode and anode, and (2) a clearer picture of SOFC operation, which allows loss factors to the changes of microstructures or activities of either electrode to be distinguished, and a better target fuel cell development to be enabled. The third task aims at applying the accelerated testing protocol to investigate the microstructural evolution of the cathode candidates identified in this research. Technical approaches will be developed to mitigate and improve the durability of cathode materials by choosing the right chemistry and tuning cathode microstructures.

36 MATERIALS SCIENCE↗

Low-Cost Preform and Molding Processes

The entry cost for prototyping a composite component for manufacture using automated, high rate processes is prohibitively expensive in many cases, especially for small business, where tooling costs may be several $100k. Discussions with industry also indicate that many small companies, tier 1 and 2 suppliers, have an interest to mold composite parts but do not want to deal with the capital cost, material handling issues, and labor associated with dry fiber preforming operations. While the molders may locate near the end user for logistics reasons, it may be more cost effective for the performer to remain regional and invest in capital equipment to support preform automation, thus keeping costs to a minimum. This project was designed to explore and demonstrate several options to meet these industry needs. Dry fiber preforming approaches were evaluated which allow for low pressure resin infusion, single sided tooling options such a vacuum assisted resin transfer molding (VARTM) or low pressure resin transfer molding (RTM-light). Unlike sheet molding compound, SMC compression molding where typical molding pressures of 1000 psi are required to push material into the desired location; positioning of a dry fiber preform into the desired location on the tool allows for low molding pressures of 10-50 psi. Lower molding pressures allow for use of low cost, additive fabrication of polymeric tooling. Polymeric tooling is suitable for rapid part prototyping and limited production. Dry fiber preforming approaches evaluated included use of commercial chopped strand mat, robotic chopper gun deposition, and continuous fiber preform augmentation using tailored fiber placement (TFP). Use of chopped strand mat does not require a robotic deposition method, however a cutting table is generally required and there is typically 20-30% scrap generation. While various fiber areal weights are available, the preform is not readily optimized for minimal fiber use or weight savings. In contrast, a robotic chopper gun approach allows for localized deposition where fiber is required to meet structural requirements. The robotic method is highly automated and minimizes fiber scrap, however the capital cost of the equipment and engineering labor for programming can result in higher preform cost compared to chopped strand mat in certain cases depending on preform complexity. Dry fiber preforming using the robotic chopper gun method allows for creation of three dimensional forms. This approach may be ideal for molding in-house, or if the preforms stack together densely to allow for efficient shipping. Applications evaluated for this program considered trade-off between fabrication of a fully 3D preform versus production of a flat preform which is designed to readily drape into the final desired shape. Such a preform design greatly simplifies robotic programming and requires no specialized tooling. The flat preforms are easily stacked and shipped to the final molding location. Flat preforms are much easier to augment with TFP continuous fiber to provide local reinforcement. The demonstration and evaluation of these preforming and tooling methods were completed on three component applications. The first application was a battery box cover for an electric vehicle which was highly three dimensional. The second demonstrator article was comprised of complex contours and was used to demonstrate the use of TFP and RTM-light molding process. The third demonstration article was the roof of an operator’s cab for large construction equipment. The roof is relatively flat however it is comprised of complex changes in thickness which clearly demonstrate the advantage of robotic chopper gun approach as compared to using numerous preform layers of chopped strand mat. The cost trades for the various preforming methods are summarized to help guide the reader as to preforming method considerations. Finally, these demonstrations all used glass fiber roving. A fourth, exploratory task was added to evaluate the ability to make preforms using Zoltek’s carbon fiber split tow roving. We were able to adapt the chopper gun to make flat preforms for laminate testing, but further development effort would be required to make suitable preforms.

36 MATERIALS SCIENCE↗

Establishing the World Reference for Measuring the Atmospheric Longwave Irradiance with Traceability to the International System of Units

Advancing climate change research requires accurate and traceable measurement of atmospheric longwave irradiance. Measurement capabilities are limited to an estimated uncertainty of larger than +/- 6 W/m2 using the interim World Infrared Standard Group (WISG). Two independently designed and calibrated absolute radiometers measuring downwelling longwave irradiance were compared during five outdoor comparisons in 2013, 2015, and 2017 at the Physikalisch Meteorologisches Observatorium Davos World Radiation Center (PMOD/WRC) and the U.S. Department of Energy (DOE) Atmospheric Radiation Measurement program (ARM) in the Southern Great Planes (SGP). Two Absolute Cavity Pyrgeometers (ACPs) developed by the National Renewable Energy Laboratory (NREL) and four Integrating Sphere Infrared Radiometers (IRISs) developed by PMOD/WRC took part in these intercomparisons.From the five comparisons, the difference between the irradiance measured by ACPs and IRISs varied from 0.2 W/m2 to 2.5 W/m2 based on atmospheric conditions, which is within the combined stated uncertainties of +/- 3 W/m2. The irradiance measured by the WISG is lower than the average irradiance measured by ACPs and IRISs. The magnitude of difference varied from 0.2 W/m2 to 6.6 W/m2 depending on the integrated water vapor. A concerted effort to establish a world reference for measuring the atmospheric longwave irradiance with lower uncertainty and with traceability to the International System of Units (SI) by using the ACPs and IRISs as the reference started at the World Meteorological Organization (WMO). The Commission for Instruments and Methods of Observation Commission (CIMO) Task Team on Radiation References (TT) meeting was held in 2017 at the National Physical Laboratory (NPL), in Teddington, United Kingdom to discuss specific recommendation on the traceability of the atmospheric longwave irradiance to the International System of units (SI).

14 SOLAR ENERGY↗

Preface to Special Topic: New Physics and Materials for Neuromorphic Computation

Artificial Intelligence is a topic that is pervasive in many modern developments and not just confined to science anymore. Many practical applications are based on performing classification tasks inspired by how the natural brain processes information. This current Special Topic on New Physics and Materials for Neuromorphic Computation looks toward solutions for such computational processes that go beyond the currently well-established semiconducting digital computation paradigm.

36 MATERIALS SCIENCE↗

Quantification of morphological change in materials based on image data utilizing machine learning techniques

Computed tomography (CT) resolution has become high enough to monitor morphological changes due to aging in materials in long-term applications. We explored the utility of the critic of a generative adversarial network (GAN) to automatically detect such changes. The GAN was trained with images of pristine Pharmatose, which is used as a surrogate energetic material. It is important to note that images of the material with altered morphology were only used during the test phase. The GAN-generated images visually reproduced the microstructure of Pharmatose well, although some unrealistic particle fusion was seen. Calculated morphological metrics (volume fraction, interfacial line length, and local thickness) for the synthetic images also showed good agreement with the training data, albeit with signs of mode collapse in the interfacial line length. While the critic exposed changes in particle size, it showed limited ability to distinguish images by particle shape. The detection of shape differences was also a more challenging task for the selected morphological metrics that related to energetic material performance. We further tested the critic with images of aged Pharmatose. Subtle changes due to aging are difficult for the human analyst to detect. Both critic and morphological metrics analysis showed image differentiation.

36 MATERIALS SCIENCE↗

Contaminant Stabilization Technology Gap Report

After an intentional radiological release or nuclear power plant (NPP) accidental release, there may be a large area that is contaminated. Re-suspension and tracking of contamination may create issues with containing the contaminated area and create additional exposure to responders. There is a need for technologies/methodologies to reduce resuspension and tracking. Current radiological particle containment relies on securing the area, setting up a single egress and ingress route, and minimizing the amount of contaminated equipment and vehicles leaving the contaminated zone. The re-suspension and tracking of contamination greatly hampers the ability to conduct first response activities in that zone therefore technologies that can reduce these spreading mechanisms are needed. In the NPP decommissioning industry, coatings are employed to reduce the spread of contamination. These coatings may not be readily available in the quantities needed for early response. Responders need containment methodologies that can be employed with existing equipment and materials on site using techniques such as fire hosing, street sweepers, and painting. A review by Parra et al. (2009) provided a good overview of fixative/stabilization materials, which formed the basis (in addition to a literature search) for a list of potential technologies presented to stakeholders in the initial stages of this work. Advantages and disadvantages were identified for each of the technologies, which were grouped into tiers based on the time-frame they would be available following a radiological release. Stakeholders then ranked containment technologies in terms of their preference and interest in use and availability. The final part of this task is to gather more information on the stakeholder-selected technologies and identify technical gaps that need to be filled with experimental research before technical procedures can be developed for containment technology use in the field.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Noble gas ion beams in materials science for future applications and devices

Helium ion microscopy (HIM), enabled by a gas field ion source (GFIS), is an emerging imaging and nanofabrication technique compatible with many applications in materials science. The scanning electron microscope (SEM) has become ubiquitous in materials science for high-resolution imaging of materials. However, due to the fundamental limitation in focusing of electron beams, ion-beam microscopy is now being developed (e.g., at 20 kV the SEM beam diameter ranges from 0.5 to 1 nm, whereas the HIM offers 0.35 nm). The key technological advantage of the HIM is in its multipurpose design that excels in a variety of disciplines. The HIM offers higher resolution than the best available SEMs as well as the traditional gallium liquid-metal ion source (LMISs) focused ion beams (FIBs), and is capable of imaging untreated biological or other insulating samples with unprecedented resolution, depth of field, materials contrast, and image quality. GFIS FIBs also offer a direct path to defect engineering via ion implantation, three-dimensional direct write using gaseous and liquid precursors, and chemical-imaging options with secondary ion mass spectrometry. HIM covers a wide range of tasks that otherwise would require multiple tools or specialized sample preparation. In this paper, we describe the underlying technology, present materials, relevant applications, and offer an outlook for the potential of FIB technology in processing materials.

2D materials↗

Utilization of the Critic Subnetwork of a Generative Adversarial Network as Detector of Morphological Material Change in Image Data

The resolution of computed tomography (CT) has become high enough to monitor morphological changes due to aging in materials in long-term applications. For this work, we explored the utility of the critic of a generative adversarial network (GAN) to automatically detect such changes. The GAN was trained with images of pristine Pharmatose, which is used as a surrogate energetic material. It is important to note that images of the material with altered morphology were only used during the test phase. The GAN-generated images reproduced the microstructure of Pharmatose well, although some unrealistic particle fusion was seen. Calculated morphological metrics (volume fraction, interfacial line length, and local thickness) for the synthetic images also showed good agreement with the training data, albeit with signs of mode collapse in the interfacial line length. While the critic exposed changes in particle size, it showed limited ability to distinguish images by particle shape. The detection of shape differences was also a more challenging task for the selected morphological metrics that related to energetic material performance. We further tested the critic with images of aged Pharmatose. Subtle changes due to aging are difficult for the human analyst to detect; but both critic and morphological metrics analysis showed image differentiation.

36 MATERIALS SCIENCE↗