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Detection and Characterization of Underground Facilities by Stochastic Inversion and Modeling of Data from the New Generation of Synthetic Aperture Satellites (Final Report)

Many clandestine development and production activities can be conducted underground to evade surveillance. The purpose of the study reported here was to develop a technique to detect underground facilities by broad-area search and then to characterize the facilities by inversion of the collected data. This would enable constraints to be placed on the types of activities that would be feasible at each underground site, providing a basis the design of targeted surveillance and analysis for more complete characterization. Excavation of underground cavities causes deformation in the host material and overburden that produces displacements at the ground surface. Such displacements are often measurable by a variety of surveying or geodetic techniques. One measurement technique, Interferometric Synthetic Aperture Radar (InSAR), uses data from satellite-borne (or airborne) synthetic aperture radars (SARs) and so is ideal for detecting and measuring surface displacements in denied access regions. Depending on the radar frequency and the acquisition mode and the surface conditions, displacement maps derived from SAR interferograms can provide millimeter- to centimeter-level measurement accuracy on regional and local scales at spatial resolution of {approx}1-10 m. Relatively low-resolution ({approx}20 m, say) maps covering large regions can be used for broad-area detection, while finer resolutions ({approx}1 m) can be used to image details of displacement fields over targeted small areas. Surface displacements are generally expected to be largest during or a relatively short time after active excavation, but, depending on the material properties, measurable displacement may continue at a decreasing rate for a considerable time after completion. For a given excavated volume in a given geological setting, the amplitude of the surface displacements decreases as the depth of excavation increases, while the area of the discernable displacement pattern increases. Therefore, the ability to detect evidence for an underground facility using InSAR depends on the displacement sensitivity and spatial resolution of the interferogram, as well as on the size and depth of the facility and the time since its completion. The methodology development described in this report focuses on the exploitation of synthetic aperture radar data that are available commercially from a number of satellite missions. Development of the method involves three components: (1) Evaluation of the capability of InSAR to detect and characterize underground facilities ; (2) inversion of InSAR data to infer the location, depth, shape and volume of a subsurface facility; and (3) evaluation and selection of suitable geomechanical forward models to use in the inversion. We adapted LLNL's general-purpose Bayesian Markov Chain-Monte Carlo procedure, the 'Stochastic Engine' (SE), to carry out inversions to characterize subsurface void geometries. The SE performs forward simulations for a large number of trial source models to identify the set of models that are consistent with the observations and prior constraints. The inverse solution produced by this kind of stochastic method is a posterior probability density function (pdf) over alternative models, which forms an appropriate input to risk-based decision analyses to evaluate subsequent response strategies. One major advantage of a stochastic inversion approach is its ability to deal with complex, non-linear forward models employing empirical, analytical or numerical methods. However, while a geomechanical model must incorporate adequate physics to enable sufficiently accurate prediction of surface displacements, it must also be computationally fast enough to render the large number of forward realizations needed in stochastic inversion feasible. This latter requirement prompted us first to investigate computationally efficient empirical relations and closed-form analytical solutions. However, our evaluation revealed severe limitations in the ability of existing empirical and analytical forms to predict deformations from underground cavities with an accuracy consistent with the potential resolution and precision of InSAR data. We followed two approaches to overcoming these limitations. The first was to develop a new analytical solution for a 3D cavity excavated in an elastic half-space. The second was to adapt a fast parallelized finite element method to the SE and evaluate the feasibility of using in the stochastic inversion. To date we have demonstrated the ability of InSAR to detect underground facilities and measure the associated surface displacements by mapping surface deformations that track the excavation of the Los Angeles Metro system. The Stochastic Engine implementation has been completed and undergone functional testing.

58 GEOSCIENCES↗

Elimination of the Characterization of DWPF Pour Stream Sample and the Glass Fabrication and Testing of the DWPF Sludge Batch Qualification Sample

A recommendation to eliminate all characterization of pour stream glass samples and the glass fabrication and Product Consistency Test (PCT) of the sludge batch qualification sample was made by a Six-Sigma team chartered to eliminate non-value-added activities for the Defense Waste Processing Facility (DWPF) sludge batch qualification program and is documented in the report SS-PIP-2006-00030. That recommendation was supported through a technical data review by the Savannah River National Laboratory (SRNL) and is documented in the memorandums SRNL-PSE-2007-00079 and SRNL-PSE-2007-00080. At the time of writing those memorandums, the DWPF was processing sludge-only waste but, has since transitioned to a coupled operation (sludge and salt). The SRNL was recently tasked to perform a similar data review relevant to coupled operations and re-evaluate the previous recommendations. This report evaluates the validity of eliminating the characterization of pour stream glass samples and the glass fabrication and Product Consistency Test (PCT) of the sludge batch qualification samples based on sludge-only and coupled operations. The pour stream sample has confirmed the DWPF's ability to produce an acceptable waste form from Slurry Mix Evaporator (SME) blending and product composition/durability predictions for the previous sixteen years but, ultimately the pour stream analysis has added minimal value to the DWPF's waste qualification strategy. Similarly, the information gained from the glass fabrication and PCT of the sludge batch qualification sample was determined to add minimal value to the waste qualification strategy since that sample is routinely not representative of the waste composition ultimately processed at the DWPF due to blending and salt processing considerations. Moreover, the qualification process has repeatedly confirmed minimal differences in glass behavior from actual radioactive waste to glasses fabricated from simulants or batch chemicals. In contrast, the variability study has significantly added value to the DWPF's qualification strategy. The variability study has evolved to become the primary aspect of the DWPF's compliance strategy as it has been shown to be versatile and capable of adapting to the DWPF's various and diverse waste streams and blending strategies. The variability study, which aims to ensure durability requirements and the PCT and chemical composition correlations are valid for the compositional region to be processed at the DWPF, must continue to be performed. Due to the importance of the variability study and its place in the DWPF's qualification strategy, it will also be discussed in this report. An analysis of historical data and Production Records indicated that the recommendation of the Six Sigma team to eliminate all characterization of pour stream glass samples and the glass fabrication and PCT performed with the qualification glass does not compromise the DWPF's current compliance plan. Furthermore, the DWPF should continue to produce an acceptable waste form following the remaining elements of the Glass Product Control Program; regardless of a sludge-only or coupled operations strategy. If the DWPF does decide to eliminate the characterization of pour stream samples, pour stream samples should continue to be collected for archival reasons, which would allow testing to be performed should any issues arise or new repository test methods be developed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Robustness of RISMC Insights under Alternative Aleatory/Epistemic Uncertainty Classifications: Draft Report under the Risk-Informed Safety Margin Characterization (RISMC) Pathway of the DOE Light Water Reactor Sustainability Program

The Risk-Informed Safety Margin Characterization (RISMC) pathway is a set of activities defined under the U.S. Department of Energy (DOE) Light Water Reactor Sustainability Program. The overarching objective of RISMC is to support plant life-extension decision-making by providing a state-of-knowledge characterization of safety margins in key systems, structures, and components (SSCs). A technical challenge at the core of this effort is to establish the conceptual and technical feasibility of analyzing safety margin in a risk-informed way, which, unlike conventionally defined deterministic margin analysis, would be founded on probabilistic characterizations of uncertainty in SSC performance. In the context of probabilistic risk assessment (PRA) technology, there has arisen a general consensus about the distinctive roles of two types of uncertainty: aleatory and epistemic, where the former represents irreducible, random variability inherent in a system, whereas the latter represents a state of knowledge uncertainty on the part of the analyst about the system which is, in principle, reducible through further research. While there is often some ambiguity about how any one contributing uncertainty in an analysis should be classified, there has nevertheless emerged a broad consensus on the meanings of these uncertainty types in the PRA setting. However, while RISMC methodology shares some features with conventional PRA, it will nevertheless be a distinctive methodology set. Therefore, the paradigms for classification of uncertainty in the PRA setting may not fully port to the RISMC environment. Yet the notion of risk-informed margin is based on the characterization of uncertainty, and it is therefore critical to establish a common understanding of uncertainty in the RISMC setting.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Analysis of the Tank 6F Final Characterization Samples-2012 (U)

The Savannah River National Laboratory (SRNL) was requested by Savannah River Remediation (SRR) to provide sample preparation and analysis of the Tank 6F final characterization samples to determine the residual tank inventory prior to grouting. Fourteen residual Tank 6F solid samples from three areas on the floor of the tank were collected and delivered to SRNL between May and August 2011. These Tank 6F samples were homogenized and combined into three composite samples based on a proportion compositing scheme and the resulting composite samples were analyzed for radiological, chemical and elemental components. Additional measurements performed on the Tank 6F composite samples include bulk density and water leaching of the solids to account for water soluble components. The composite Tank 6F samples were analyzed and the data reported in triplicate. Sufficient quality assurance standards and blanks were utilized to demonstrate adequate characterization of the Tank 6F samples. The main evaluation criteria were target detection limits specified in the technical task request document. While many of the target detection limits were met for the species characterized for Tank 6F some were not met. In a few cases, the relatively high levels of radioactive species of the same element or a chemically similar element precluded the ability to measure some isotopes to low levels. The isotopes whose detection limits were not met in all cases included Sn-126, Sb-126, Sb-126m, Eu-152, Cm-243 and Cf-249. SRNL, in conjunction with the customer, reviewed all of these cases and determined that the impacts of not meeting the target detection limits were acceptable. Based on the analyses of variance (ANOVA) for the inorganic constituents of Tank 6F, all the inorganic constituents displayed heterogeneity. The inorganic results demonstrated consistent differences across the composite samples: lowest concentrations for Composite Sample 1, intermediate-valued concentrations for Composite Sample 2, and highest concentrations for Composite Sample 3. The Hg and Mo results suggest possible measurement outliers. However, the magnitudes of the differences between the Hg 95% upper confidence limit (UCL95) results with and without the outlier and the magnitudes of the differences between the Mo UCL95 results with and without the outlier do not appear to have practical significance. It is recommended to remove the potential measurement outliers. Doing so is conservative in the sense of producing a higher UCL95 for Hg and Mo than if the potential outliers were included in the calculations. In contrast to the inorganic results, most of the radionuclides did not demonstrate heterogeneity among the three Tank 6F composite sample characterization results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Analysis of the Tank 6F Final Characterization Samples-2012

The Savannah River National Laboratory (SRNL) was requested by Savannah River Remediation (SRR) to provide sample preparation and analysis of the Tank 6F final characterization samples to determine the residual tank inventory prior to grouting. Fourteen residual Tank 6F solid samples from three areas on the floor of the tank were collected and delivered to SRNL between May and August 2011. These Tank 6F samples were homogenized and combined into three composite samples based on a proportion compositing scheme and the resulting composite samples were analyzed for radiological, chemical and elemental components. Additional measurements performed on the Tank 6F composite samples include bulk density and water leaching of the solids to account for water soluble components. The composite Tank 6F samples were analyzed and the data reported in triplicate. Sufficient quality assurance standards and blanks were utilized to demonstrate adequate characterization of the Tank 6F samples. The main evaluation criteria were target detection limits specified in the technical task request document. While many of the target detection limits were met for the species characterized for Tank 6F some were not met. In a few cases, the relatively high levels of radioactive species of the same element or a chemically similar element precluded the ability to measure some isotopes to low levels. The isotopes whose detection limits were not met in all cases included Sn-126, Sb-126, Sb-126m, Eu-152, Cm- 243 and Cf-249. SRNL, in conjunction with the customer, reviewed all of these cases and determined that the impacts of not meeting the target detection limits were acceptable. Based on the analyses of variance (ANOVA) for the inorganic constituents of Tank 6F, all the inorganic constituents displayed heterogeneity. The inorganic results demonstrated consistent differences across the composite samples: lowest concentrations for Composite Sample 1, intermediate-valued concentrations for Composite Sample 2, and highest concentrations for Composite Sample 3. The Hg and Mo results suggest possible measurement outliers. However, the magnitudes of the differences between the Hg 95% upper confidence limit (UCL95) results with and without the outlier and the magnitudes of the differences between the Mo UCL95 results with and without the outlier do not appear to have practical significance. It is recommended to remove the potential measurement outliers. Doing so is conservative in the sense of producing a higher UCL95 for Hg and Mo than if the potential outliers were included in the calculations. In contrast to the inorganic results, most of the radionuclides did not demonstrate heterogeneity among the three Tank 6F composite sample characterization results.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characterization of U-Mo Foils for AFIP-7

Twelve AFIP in-process foil samples, fabricated by either Y-12 or LANL, were shipped from LANL to PNNL for potential characterization using optical and scanning electron microscopy techniques. Of these twelve, nine different conditions were examined to one degree or another using both techniques. For this report a complete description of the results are provided for one archive foil from each source of material, and one unirradiated piece of a foil of each source that was irradiated in the Advanced Test Reactor. Additional data from two other LANL conditions are summarized in very brief form in an appendix. The characterization revealed that all four characterized conditions contained a cold worked microstructure to different degrees. The Y-12 foils exhibited a higher degree of cold working compared to the LANL foils, as evidenced by the highly elongated and obscure U-Mo grain structure present in each foil. The longitudinal orientations for both of the Y-12 foils possesses a highly laminar appearance with such a distorted grain structure that it was very difficult to even offer a range of grain sizes. The U-Mo grain structure of the LANL foils, by comparison, consisted of a more easily discernible grain structure with a mix of equiaxed and elongated grains. Both materials have an inhomogenous grain structure in that all of the characterized foils possess abnormally coarse grains.

Edwards, Danny J.↗

Source Characterization and Temporal Variation of Methane Seepage from Thermokarst Lakes on the Alaska North Slope in Response to Arctic Climate Change

The goals of this research were to characterize the source, magnitude and temporal variability of methane seepage from thermokarst lakes (TKL) within the Alaska North Slope gas hydrate province, assess the vulnerability of these areas to ongoing and future arctic climate change and determine if gas hydrate dissociation resulting from permafrost melting is contributing to the current lake emissions. Analyses were focused on four main lake locations referred to in this report: Lake Qalluuraq (referred to as Lake Q) and Lake Teshekpuk (both on Alaska's North Slope) and Lake Killarney and Goldstream Bill Lake (both in Alaska's interior). From analyses of gases coming from lakes in Alaska, we showed that ecological seeps are common in Alaska and they account for a larger source of atmospheric methane today than geologic subcap seeps. Emissions from the geologic source could increase with potential implications for climate warming feedbacks. Our analyses of TKL sites showing gas ebullition were complemented with geophysical surveys, providing important insight about the distribution of shallow gas in the sediments and the lake bottom manifestation of seepage (e.g., pockmarks). In Lake Q, Chirp data were limited in their capacity to image deeper sediments and did not capture the thaw bulb. The failure to capture the thaw bulb at Lake Q may in part be related to the fact that the present day lake is a remnant of an older, larger, and now-partially drained lake. These suggestions are consistent with our analyses of a dated core of sediment from the lake that shows that a wetland has been present at the site of Lake Q since approximately 12,000 thousand years ago. Chemical analyses of the core indicate that the availability of methane at the site has changed during the past and is correlated with past environmental changes (i.e. temperature and hydrology) in the Arctic. Discovery of methane seeps in Lake Teshekpuk in the northernmost part of the lake during 2009 reconnaissance surveys provided a strong impetus to visit this area in 2010. The seismic methods applied in Lake Teshekpuk were able to image pockmarks, widespread shallow gas in the sediments, and the relationship among different sediment packages on the lake's bottom, but even boomer seismics did not detect permafrost beneath the northern part of the lake. By characterizing the biogeochemistry of shallow TKL with methane seeps we showed that the radical seasonal shifts in ice cover and temperature. These seasonal environmental differences result in distinct consumption and production processes of biologically-relevant compounds. The combined effects of temperature, ice-volume and other lithological factors linked to seepage from the lake are manifest in the distribution of sedimentary methane in Lake Q during ice-covered and ice-free conditions. The biogeochemistry results illustrated very active methanotrophy in TKLs. Substantial effort was subsequently made to characterize the nature of methanotrophic communities in TKLs. We applied stable isotope probing approaches to genetically characterize the methanotrophs most active in utilizing methane in TKLs. Our study is the first to identify methane oxidizing organisms active in arctic TKLs, and revealing that type I methanotrophs and type II methanotrophs are abundant and active in assimilating methane in TKLs. These organisms play an important role in limiting the flux of methane from these sites. Our investigations indicate that as temperatures increase in the Arctic, oxidation rates and active methanotrophic populations will also shift. Whether these changes can offset predicted increases in methanogenesis is an important question underlying models of future methane flux and resultant climate change. Overall our findings indicate that TKLs and their ability to act as both source and sink of methane are exceedingly sensitive to environmental change.

03 NATURAL GAS↗

Treated Wood Waste Identification and Characterization

At LLNL different program areas may encounter treated wood waste and need to determine the appropriate disposal method. Disposal option decisions are to be made by the generator, environmental analyst (EA) and, if needed, support from RHWM. If the generator decides to use the Treated Wood exemption, the regulatory guidance and characterization support is provided in this paper. For additional support RHWM can be contacted through the assigned area Field Technician. Otherwise if the generator and the EA decide to opt for the exemption path then the regulations and controls referenced in this paper have to be initiated and followed. Pressure treated wood presents an issue for identification and waste processing. It has the potential to be in construction waste in facility structures and in outside construction, such as porches, steps, landscaping borders. The difficulty is in easy identification and characterization without costly analytical support and obtaining information in the post D&D phase of an operation. The following guidance presents an easy solution to this characterization issue. This paper is limited to Chromated Copper Arsenate (CCA) and other related metal treated wood. The local availability and the lack of an alternative to direct chemical analysis for identification and characterization prevented the inclusion of organic wood preservatives in this study.

54 ENVIRONMENTAL SCIENCES↗

Cf-252 Characterization Documents

Six documents were written by Vance and Associates under contract to the Off-Site Source Recovery Project of Los Alamos National Laboratory. These Six documents provided the basis for characterization of Californium-252 sealed sources and for the packaging and manifesting of this material for disposal at the Waste Isolation Pilot Project. The Six documents are: 1. VA-OSR-10, Development of radionuclide distributions for Cf-252 sealed sources. 2. VA-OSR-11, Uncertainty analysis for Cf-252 sealed sources. 3. VA-OSR-12, To determine the radionuclides in the waste drums containing Cf-252 sealed source waste that are required to be reported under the requirements of the WIPP WAC and the TRAMPAC. 4. VA-OSR-13, Development of the spreadsheet for the radiological calculations for the characterization of Cf-252 sources. 5. VA-OSR-14, Relative importance of neutron-induced fission in Cf-252 sources. 6. VA-OSR-15, Determine upper bound of decay product inventories from a drum of Cf-252 sources. These six documents provide the technical basis for the characterization of Cf-252 sources and will be part of the AK documentation required for submittal to the Central Characterization Project (CCP) of WIPP.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characterization of Bond Strength of U-Mo Fuel Plates Using the Laser Shockwave Technique: Capabilities and Preliminary Results

This report summarizes work conducted to-date on the implementation of new laser-based capabilities for characterization of bond strength in nuclear fuel plates, and presents preliminary results obtained from fresh fuel studies on as-fabricated monolithic fuel consisting of uranium-10 wt.% molybdenum alloys clad in 6061 aluminum by hot isostatic pressing. Characterization involves application of two complementary experimental methods, laser-shock testing and laser-ultrasonic imaging, collectively referred to as the Laser Shockwave Technique (LST), that allows the integrity, physical properties and interfacial bond strength in fuel plates to be evaluated. Example characterization results are provided, including measurement of layer thicknesses, elastic properties of the constituents, and the location and nature of generated debonds (including kissing bonds). LST provides spatially localized, non-contacting measurements with minimum specimen preparation, and is ideally suited for applications involving radioactive materials, including irradiated materials. The theoretical principles and experimental approaches employed in characterizing nuclear fuel plates are described, and preliminary bond strength measurement results are discussed, with emphasis on demonstrating the capabilities and limitations of these methods. These preliminary results demonstrate the ability to distinguish bond strength variations between different fuel plates. Although additional development work is necessary to validate and qualify the test methods, these results suggest LST is viable as a method to meet fuel qualification requirements to demonstrate acceptable bonding integrity.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterization of Tri-lab Tantalum Plate

This report provides a detailed characterization Tri-lab Tantalum (Ta) plate jointly purchased from HCStark Inc. by Sandia, Los Alamos and Lawrence Livermore National Laboratories. Data in this report was compiled from series of material and properties characterization experiments carried out at Sandia (SNL) and Los Alamos (LANL) Laboratories through a leveraged effort funded by the C2 campaign. Results include microstructure characterization detailing the crystallographic texture of the material and an increase in grain size near the end of the rolled plate. Mechanical properties evaluations include, compression cylinder, sub-scale tension specimen, micohardness and instrumented indentation testing. The plate was found to have vastly superior uniformity when compare with previously characterized wrought Ta material. Small but measurable variations in microstructure and properties were noted at the end, and at the top and bottom edges of the plate.

Buchheit, Thomas E.↗

A Ten Step Protocol and Plan for CCS Site Characterization, Based on an Analysis of the Rocky Mountain Region, USA

This report expresses a Ten-Step Protocol for CO2 Storage Site Characterization, the final outcome of an extensive Site Characterization analysis of the Rocky Mountain region, USA. These ten steps include: (1) regional assessment and data gathering; (2) identification and analysis of appropriate local sites for characterization; (3) public engagement; (4) geologic and geophysical analysis of local site(s); (5) stratigraphic well drilling and coring; (6) core analysis and interpretation with other data; (7) database assembly and static model development; (8) storage capacity assessment; (9) simulation and uncertainty assessment; (10) risk assessment. While the results detailed here are primarily germane to the Rocky Mountain region, the intent of this protocol is to be portable or generally applicable for CO2 storage site characterization.

McPherson, Brian↗

Milestones for Selection, Characterization, and Analysis of the Performance of a Repository for Spent Nuclear Fuel and High-Level Radioactive Waste at Yucca Mountain

This report presents a concise history in tabular form of events leading up to site identification in 1978, site selection in 1987, subsequent characterization, and ongoing analysis through 2008 of the performance of a repository for spent nuclear fuel and high-level radioactive waste at Yucca Mountain in southern Nevada. The tabulated events generally occurred in five periods: (1) commitment to mined geologic disposal and identification of sites; (2) site selection and analysis, based on regional geologic characterization through literature and analogous data; (3) feasibility analysis demonstrating calculation procedures and importance of system components, based on rough measures of performance using surface exploration, waste process knowledge, and general laboratory experiments; (4) suitability analysis demonstrating viability of disposal system, based on environment-specific laboratory experiments, in-situ experiments, and underground disposal system characterization; and (5) compliance analysis, based on completed site-specific characterization. Because the relationship is important to understanding the evolution of the Yucca Mountain Project, the tabulation also shows the interaction between four broad categories of political bodies and government agencies/institutions: (a) technical milestones of the implementing institutions, (b) development of the regulatory requirements and related federal policy in laws and court decisions, (c) Presidential and agency directives and decisions, and (d) critiques of the Yucca Mountain Project and pertinent national and world events related to nuclear energy and radioactive waste.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Characterization of Ceramic Material Produced From a Cold Crucible Induction Melter Test

This report summarizes the results from characterization of samples from a melt processed surrogate ceramic waste form. Completed in October of 2014, the first scaled proof of principle cold crucible induction melter (CCIM) test was conducted to process a Fe-hollandite-rich titanate ceramic for treatment of high level nuclear waste. X-ray diffraction, electron microscopy, inductively coupled plasma-atomic emission spectroscopy (and inductively coupled plasma-mass spectroscopy for Cs), and product consistency tests were used to characterize the CCIM material produced. Core samples at various radial locations from the center of the CCIM were taken. These samples were also sectioned and analyzed vertically. Together, the various samples were intended to provide an indication of the homogeneity throughout the CCIM with respect to phase assemblage, chemical composition, and chemical durability. Characterization analyses confirmed that a crystalline ceramic with desirable phase assemblage was produced from a melt using a CCIM. Hollandite and zirconolite were identified in addition to possible highly-substituted pyrochlore and perovskite. Minor phases rich in Fe, Al, or Cs were also identified. Remarkably only minor differences were observed vertically or radially in the CCIM material with respect to chemical composition, phase assemblage, and durability. This recent CCIM test and the resulting characterization in conjunction with demonstrated compositional improvements support continuation of CCIM testing with an improved feed composition and improved melter system.

36 MATERIALS SCIENCE↗

Waste Characterization Methods

This report discusses ways to classify waste as outlined by LANL. Waste Generators must make a waste determination and characterize regulated waste by appropriate analytical testing or use of acceptable knowledge (AK). Use of AK for characterization requires several source documents. Waste characterization documentation must be accurate, sufficient, and current (i.e., updated); relevant and traceable to the waste stream’s generation, characterization, and management; and not merely a list of information sources.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Solid State Characterizations of Long-Term Leached Cast Stone Monoliths

This report describes the results from the solid phase characterization of six Cast Stone monoliths from the extended leach tests recently reported on (Serne et al. 2016),that were selected for characterization using multiple state-of-the-art approaches. The Cast Stone samples investigated were leached for > 590 d in the EPA Method 1315 test then archived for > 390 d in their final leachate. After reporting the long term leach behavior of the monoliths (containing radioactive 99 Tc and stable 127 I spikes and for original Westsik et al. 2013 fabricated monoliths, 238 U), it was suggested that physical changes to the waste forms and a depleting inventory of contaminants of potential concern may mean that effective diffusivity calculations past 63 d should not be used to accurately represent long-term waste form behavior. These novel investigations, in both length of leaching time and application of solid state techniques, provide an initial arsenal of techniques which can be utilized to perform such Cast Stone solid phase characterization work, which in turn can support upcoming performance assessment maintenance. The work was performed at Pacific Northwest National Laboratory (PNNL) for Washington River Protection Solutions (WRPS) to characterize several properties of the long- term leached Cast Stone monolith samples.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

High-Resolution Characterization of UMo Alloy Microstructure

This report highlights the capabilities and procedure for high-resolution characterization of UMo fuels in PNNL. Uranium-molybdenum (UMo) fuel processing steps, from casting to forming final fuel, directly affect the microstructure of the fuel, which in turn dictates the in-reactor performance of the fuel under irradiation. In order to understand the influence of processing on UMo microstructure, microstructure characterization techniques are necessary. Higher-resolution characterization techniques like transmission electron microscopy (TEM) and atom probe tomography (APT) are needed to interrogate the details of the microstructure. The findings from TEM and APT are also directly beneficial for developing predictive multiscale modeling tools that can predict the microstructure as a function of process parameters. This report provides background on focused-ion-beam–based TEM and APT sample preparation, TEM and APT analysis procedures, and the unique information achievable through such advanced characterization capabilities for UMo fuels, from a fuel fabrication capability viewpoint.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Characterizing Organic Aerosol Processes and Climatically Relevant Properties via Advanced and Integrated Analyses of Aerosol Mass Spectrometry Datasets from DOE Campaigns and ACRF Measurements. Final report for DE-SC0007178

Organic aerosols (OA) are an important but poorly characterized component of the earth’s climate system. Enormous complexities commonly associated with OA composition and life cycle processes have significantly complicated the simulation and quantification of aerosol effects. To unravel these complexities and improve understanding of the properties, sources, formation, evolution processes, and radiative properties of atmospheric OA, we propose to perform advanced and integrated analyses of multiple DOE aerosol mass spectrometry datasets, including two high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) datasets from intensive field campaigns on the aerosol life cycle and the Aerosol Chemical Speciation Monitor (ACSM) datasets from long-term routine measurement programs at ACRF sites. In this project, we will focus on 1) characterizing the chemical (i.e., composition, organic elemental ratios), physical (i.e., size distribution and volatility), and radiative (i.e., sub- and super-saturated growth) properties of organic aerosols, 2) examining the correlations of these properties with different source and process regimes (e.g., primary, secondary, urban, biogenic, biomass burning, marine, or mixtures), 3) quantifying the evolutions of these properties as a function of photochemical processing, 4) identifying and characterizing special cases for important processes such as SOA formation and new particle formation and growth, and 5) correlating size-resolved aerosol chemistry with measurements of radiative properties of aerosols to determine the climatically relevant properties of OA and characterize the relationship between these properties and processes of atmospheric aerosol organics. Our primary goal is to improve a process-level understanding of the life cycle of organic aerosols in the Earth’s atmosphere. We will also aim at bridging between observations and models via synthesizing and translating the results and insights generated from this research into data products and formulations that may be directly used to inform, improve, and evaluate regional and global models. In addition, we will continue our current very active collaborations with several modeling groups to enhance the use and interpretation of our data products. Overall, this research will contribute new data to improve quantification of the aerosol’s effects on climate and thus the achievement of ASR’s science goal of – “improving the fidelity and predictive capability of global climate models”.

54 ENVIRONMENTAL SCIENCES↗