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DOE OSTI2025

Perspective: Are glasses really frozen?

A glass is obtained by cooling a liquid fast enough to avoid crystallization. It is a solid with elastic constants and density similar to those of a crystal with the same composition. It is customarily assumed that the structure of a glass is frozen, and atoms are largely locked into a random, but specific, structure; while a small number of loosely bound atoms may be mobile, most atoms are frozen at room temperature and below. However, recent simulation studies on metallic glasses present a rather different picture. A very significant fraction (~20%) of atoms are not frozen and locally mobile, even down to T = 0 partly because of quantum effect. Here, we describe these observations and discuss their implications on the nature of the glass structure and the origin of the glass transition.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Local structural investigation of non-crystalline materials at high pressure: the case of GeO 2 glass

Abstract Local structures play a crucial role in the structural polyamorphism and novel electronic properties of amorphous materials, but their accurate measurement at high pressure remains a formidable challenge. In this article, we use the local structure of network-forming GeO 2 glass as an example, to present our recent approaches and advances in high-energy x-ray diffraction, high-pressure x-ray absorption fine structure, and ab initio first-principles density functional theory calculations and simulations. Although GeO 2 glass is one of the best studied materials in the field of high pressure research due to its importance in glass theory and geophysical significance, there are still some long-standing puzzles, such as the existence of appreciable distinct fivefold [5] Ge coordination at low pressure and the sixfold-plus [6+] Ge coordination at ultrahigh pressure. Our work sheds light on the origin of pressure-induced polyamorphism of GeO 2 glass, and the [5] Ge polyhedral units may be the dominant species in the densification mechanism of network-forming glasses from tetrahedral to octahedral amorphous structures.

Physics↗

DOE OSTI2020

Comparative scintillation performance of EJ-309, EJ-276, and a novel organic glass

An organic glass scintillator developed by Sandia National Laboratories was characterized in terms of its light output and pulse shape discrimination (PSD) properties and compared to commercial liquid (EJ-309) and plastic (EJ-276) organic scintillators. The electron light output was determined through relative comparison of the 137 Cs Compton edge location. The proton light yield was measured using a double time-of-flight technique at the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory. Using a tunable broad-spectrum neutron source and an array of pulse-shape-discriminating observation scintillators, a continuous measurement of the proton light yield was performed for EJ-309 (200 keV–3.2 MeV), EJ-276 (170 keV–4.9 MeV), and the organic glass (50 keV–20 MeV) . Finally, the PSD properties of the organic glass, EJ-309, and EJ-276 were evaluated using an AmBe source and compared via a figure-of-merit metric. The organic glass exhibited a higher electron light output than both EJ-309 and EJ-276. Its proton light yield and PSD performance were comparable to EJ-309 and superior to that of EJ-276. Finally, with these performance characteristics, the organic glass scintillator is well poised to replace current state-of-the-art PSD-capable scintillators in a range of fast neutron detection applications.

47 OTHER INSTRUMENTATION↗

DOE OSTI2025

Neutron and Gamma-Ray Imaging of Th-232 and Cm-244 Using Organic Glass Scintillators

Modern nuclear safeguards require detection and characterization capabilities suitable for a wide variety of radiation sources and applications. Field-deployable detection systems have also had to modernize to meet changing needs. Recent developments in organic scintillator technology have resulted in the creation of an organic glass scintillator (OGS) at Sandia National Laboratory which is composed of a 9:1 mixture of glass compounds C42H36Si and C51H44Si. The novel scintillator composition was implemented into the design for a dual-particle capable imaging system at the University of Michigan. This work presents new results from two experiments demonstrating the gamma-ray and fast-neutron imaging capabilities of the organic glass system. Gamma spectroscopy was also performed using CeBr3 scintillators that are part of the imager design. Measurements were performed at Lawrence Livermore National Laboratory using 232Th metal hemishells and an encapsulated 244Cm oxide source. Successful gamma-ray imaging of the 232Th distributed sources is demonstrated with the glass imager, but there were no appreciable neutrons from the 232Th for neutron imaging. Promising neutron and gamma-ray imaging results of 244Cm are demonstrated despite limited imaging event statistics available in this measurement. Gamma-ray spectroscopy results were able to identify 232Th using prominent emissions at 239, 338, 583, and 911 keV. 244Cm was identified from emissions of 43, 99, and 153 keV. These results demonstrate the potential of organic glass imaging for nuclear nonproliferation or characterization efforts.

Lopez, Ricardo [Univ. of Michigan, Ann Arbor, MI (↗

DOE OSTI2023

Effect of material properties on batch‐to‐glass conversion kinetics

Abstract A recently developed model of the cold cap—the reacting glass batch (melter feeds) floating on molten glass in an electric glass melter—couples heat transfer with the feed‐to‐glass conversion kinetics. The model allows for determining the distributions of temperature and various properties within the cold cap. In the present study, this model is applied to four melter feeds designed for high‐level and low‐activity nuclear wastes. Profiles of temperature, conversion degree, cold cap porosity and density, condensed matter velocity, and heating rate were determined using the material properties of the cold cap. Effects of vigorous foaming at the cold cap bottom were considered. Density, thermal conductivity, and glass production rate strongly affect the cold cap thickness and the fraction of undissolved silica entering the melt under the cold cap. The heating rate profile in the cold cap is highly nonlinear, with high heating rates observed in the foam layer.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2020

Topological controls on aluminosilicate glass dissolution: Complexities induced in hyperalkaline aqueous environments

Abstract Fly ash, an aluminosilicate composite consisting of disordered (major) and crystalline (minor) compounds, is a low‐carbon alternative that can partially replace ordinary portland cement (OPC) in the binder fraction of concrete. Therefore, understanding the reactivity of fly ash in the hyperalkaline conditions prevalent in concrete is critical to predicting concrete's performance; including setting and strength gain. Herein, temporal measurements of the solution composition (using inductively coupled plasma‐optical emission spectrometry: ICP‐OES) are used to assess the aqueous dissolution rate of monophasic synthetic aluminosilicate glasses analogous to those present in technical fly ashes, under hyperalkaline conditions (10 ≤ pH ≤ 13) across a range of temperatures (25°C ≤ T≤45°C). The dissolution rate is shown to depend on the average number of topological constraints per atom within the glass network (n c , unitless), but this dependence weakens with increasing pH (>10). This is postulated to be on account of: (a) time‐dependent changes in the glass’ surface structure, that is, the number of topological constraints; and/or (b) a change in the dissolution mechanism (eg from network hydrolysis to transport control). The results indicate that the topological description of glass dissolution is most rigorously valid only at very short reaction times (ie at high undersaturations), especially under conditions of hyperalkalinity. These findings provide an improved basis to understand the underlying factors that affect the initial and ongoing reactivity of aluminosilicate glasses such as fly ash in changing chemical environments, for example, when such materials are utilized in cementitious composites.

Oey, Tandré↗

DOE OSTI2023

Emergent Halperin–Saslow mode, gauge glass and quenched disorders in quantum Ising magnet TmMgGaO 4

Quenched disorders could bring novel quantum excitations and models to certain quantum magnets. Motivated by recent experiments on the quantum Ising magnet TmMgGaO 4 , we explore the effects of the quenched disorder and the interlayer coupling in this triangular lattice Ising antiferromagnet. It is pointed out that the weak quenched (nonmagnetic) disorder would convert the emergent 2D Berezinskii–Kosterlitz–Thouless (BKT) phase and the critical region into a U(1) gauge glass. There will be an emergent Halperin–Saslow mode associated with this gauge glass. Using the Imry-Ma’s renormalization group result, we explain the fate of the finite-field [Formula: see text] symmetry breaking transition at the low temperatures. The ferromagnetic interlayer coupling would suppress the BKT phase and generate a tiny ferromagnetism. With quenched disorders, this interlayer coupling changes the 2D gauge glass into a 3D gauge glass, and the Halperin–Saslow mode persists. This work merely focuses on addressing a phase regime in terms of emergent U(1) gauge glass behaviors and hope to inspire future works and thoughts in weakly disordered frustrated magnets in general.

Physics↗

DOE OSTI2023

Enhanced laser-induced damage performance of all-glass metasurfaces for energetic pulsed laser applications

To fabricate optical components with surface layers compatible with high power laser applications that may operate as antireflective coatings, polarization rotators, or harness physical anisotropy for other uses, metasurfaces are becoming an appealing candidate. In this study, a large-beam (1.05 cm diameter) 351-nm laser-induced damage testing was done on an all-glass metasurface structure composed of cone-like features with a subwavelength spacing of adjacent features. These structures were fabricated on untreated fused silica glass and damage tested, as were structures that were fabricated on fused silica glass that experienced a preliminary etching process to remove the surface Beilby layer that is characteristic of polished fused silica. The laser-induced damage onset for structures on untreated fused silica glass was 19.3 J∙cm -2 , while the sample that saw an initial pretreatment etch exhibited an improved damage onset of 20.4 J∙cm -2 , only 6% short of the reference pretreated glass damage onset of 21.7 J∙cm -2 . For perspective, the National Ignition Facility (NIF) operational average fluence at this wavelength and pulse length is about 10 J/cm2. At a fluence of 25.5 J∙cm -2 , the reference (pretreated) fused silica initiated 5.2 damage sites per mm 2 , while the antireflective metasurface sample with a preliminary etching process treatment initiated 9.8 damage sites per mm 2 . In conclusion, these findings demonstrate that substrate-engraved metasurfaces are compatible with high energy and power laser applications, further broadening their application space.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Aluminization Coatings and Glass Seals for High Temperature System: CRADA 536 [Abstract Only]

The proposed work will demonstrate the suitability of PNNL Reactive Air Aluminization (RAA) coatings (US Patent Numbers 10,577,694, 10,378,094, and 9,481,923) for use in high-temperature systems. In particular, the Participant and Contractor will explore applicability of these coatings in Participant’s high-temperature hydrogen reactors where they would be used to prepare the sealing surfaces of the reactor technology. Utility Global will also instruct PNNL regarding their needs relating to the further development of glass seal technologies that are suitable for use in their systems. This effort will entail alkaline earth-based silicate glass development and characterization; evaluation and characterization of reliability and compatibility of the coatings with glass seals, working environments, and substrates; performance demonstrations of representative cells and intermediate cells sealed using the glass seals and/or coatings of interest; and incorporation of the aluminization coatings and glass seals into the reactor for full-scale testing.

08 HYDROGEN↗

DOE OSTI2022

Results of Re-evaluation of FEPs Related to Implementing the ABD Glass Program

The Savannah River Site plans to reprocess defense spent nuclear fuel currently stored in their L-Basin via the Accelerated Basin Deinventory (ABD) Program. The previous plan for the L-Basin spent nuclear fuel was to dispose of it directly in the federal repository without reprocessing. Implementing the ABD Program will result in final disposal of approximately 900 fewer canisters of defense spent nuclear fuel and the production of approximately 521 more canisters of vitrified high-level waste glass with some specific differences from the planned high-level waste glass. Because the 235U in the L-Basin spent nuclear fuel is not intended to be recovered, the fissile mass loading of the vitrified high-level glass waste form to be produced must be increased above the current value of 897 g/m 3 to a maximum of 2,500 g/m 3 . Therefore, implementing the ABD Program would produce a variant of high-level waste glass—the ABD glass—that needs to be evaluated for future repository licensing, which includes both preclosure safety and postclosure performance. This report describes the approach to and summarizes the results of an evaluation of the potential effects of implementing the ABD Program at the Savannah River Site on the technical basis for future repository licensing for a generic repository that is similar to Yucca Mountain and for one that is fully generic. This evaluation includes the effects on preclosure safety analyses and postclosure performance assessment for both repository settings. The license application for the proposed Yucca Mountain repository (DOE 2008), which is serving as a framework for this evaluation, concluded that the proposed Yucca Mountain repository would meet all applicable regulatory requirements. The evaluation documented in this report found that implementing the ABD Program is not expected to change that conclusion for a generic repository similar to Yucca Mountain or for a generic repository with respect to the preclosure safety analyses. With respect to the postclosure performance of a generic repository, no concerns were identified.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Aluminization Coatings and Glass Seals for High Temperature Systems - CRADA 536 (Final Report)

The objective of this project was to demonstrate the suitability of PNNL’s Reactive Air Aluminization (RAA) coatings (US Patent Numbers 10,577,694, 10,378,094, and 9,481,923) for use in high-temperature systems. In particular, PNNL and Utility Global undertook a collaborative effort to explore the applicability of these coatings in Utility Global’s high-temperature hydrogen reactors where they would be used to prepare the sealing surfaces of the reactor technology. Utility Global instructed PNNL regarding their needs relating to further development of glass seal technologies suitable for use in their systems. This effort entailed alkaline earth-based silicate glass development and characterization; evaluation and characterization of reliability and compatibility of the coatings with glass seals, working environments, and substrates; performance demonstrations of representative cells and intermediate cells sealed using the glass seals and/or coatings of interest; and incorporation of the aluminization coatings and glass seals into Utility Global reactors for testing.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Machine-Learned Structure-Property Relationship in Metallic Glasses (Final Report)

The goal of the proposed work was to gain the ability to predict properties from the known coordinates (relative positions) of atoms in a metallic glass, presuming that information about which regions of the glass are fertile for rearrangment (defects) are encoded in this structural information. This goal is important to the science of metallic glasses. This research of applied machine learning methods to automate the development of a relationship between structural measures and thermally and stress-activated events in the metallic glass. In this way, the work aimed to building a bridge between structure and properties for this class of materials. The work is expected to have timely impact on guiding the tuning of internal structures of metallic glasses for desired properties. It also represents an advance in applying machine learning techniques to discerning the properties of materials.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Chemical durability assessment of enhanced low-activity waste glasses through EPA method 1313

In this work, we report the progress of the Glass Leaching Assessment for Durability (GLAD) program on the implementation of the United States Environmental Protection Agency (EPA) Leaching Environmental Assessment Framework pH-dependent leach test (EPA Method 1313) to low-activity nuclear waste (LAW) glasses. The GLAD program seeks to develop new strategies to understand the chemical durability of nuclear waste glasses for the disposal in near-surface conditions. A series of 16 high-waste loading LAW glasses, currently under development, were selected using machine learning methods to study the corrosion behavior using EPA Method 1313. Reacted glass powders were examined using scanning electron microscopy and the eluate compositions were examined using inductively coupled plasma-optical emission spectroscopy. Compositional modeling was used to fit the measured elemental releases from EPA Method 1313. The compositional models demonstrated that elements such as Si reduce elemental release while B can increase elemental release (consistent with elemental modeling of the Product Consistency Test and Vapor Hydration Test) while other elements, such as Fe, exhibit pH-dependent behavior. The amount of acid added during the EPA testing was found to significantly impact the observed result, which was only apparent after preforming the present matrix study. The overall titration curves were able to be compositionally modeled for future process optimization.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2023

Preliminary Enhanced LAW Glass Formulation Algorithm

This report summarizes the Preliminary Enhanced Low-Activity Waste Glass Formulation Algorithm (GFA), its background information, and the calculations it performs. The Preliminary Enhanced Low-Activity Waste GFA is a tool developed in MATLAB to formulate glass for a given waste composition while attempting to maximize waste loading. It is intended for use at the Waste Treatment and Immobilization Plant, where nuclear waste will be vitrified into glass. The formulated glass is required to satisfy several processing and product quality constraints. In addition, calculations must account for associated uncertainties in constraint prediction and measurement. The GFA adheres to Pacific Northwest National Laboratory nuclear quality assurance procedures and has been validated and verified. In this second revision to the report, two constraints: the lithium and zirconia target constraints were amended to Table 3.1 and programmed into the algorithm. Additionally, three sections were added. Section 3.2.1 includes the Enhanced LAW Correlation Rules, an addition to the glass optimality criteria. Section 4.0 discusses a stepped process approach taken to ensure the algorithm can adequately react to differences between its recommended output and the actual measurements and transfers made during plant operation, and calculation of specific radionuclide concentrations. Section 5.2 describes changes to the user interaction with the algorithm program including the addition of a graphical user interface and compilation of the software.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Glass Formulation and Testing with RPP-WTP HLW Simulants (Final Report)

This report presents the results from HLW glass formulation work that was conducted at the Vitreous State Laboratory of The Catholic University of America during Part B1 of the RPP-WTP Project (formally known as TWRS-P) in support of the Privatization contractor, BNFL, Inc. Glass formulation development is required to provide data that are essential for design of the vitrification facility in the near term and for safe and reliable operation of that facility in the longer-term. These data also form the bases from which contractually and technically acceptable immobilized high-level waste (IHLW) products will be devised. Glass formulation therefore impacts many aspects of the vitrification facility design, overall process economics, and contractual compliance. As an integral part of the overall system design, development of glass formulations requires input from many sources including tank waste characterization, pretreatment process definition, flow sheet development, and processing schedules. Accordingly, the glass formulation effort must be responsive to new information as the facility design basis evolves.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2024

Viscosity Measurements of the HLW APPS Glasses

The U.S. Department of Energy is responsible for building the Hanford Waste Treatment and Immobilization Plant (WTP) at the Hanford site in Washington to remediate 56 million gallons of radioactive waste historically stored in 177 underground tanks. The Office of River Protection has requested that the Savannah River National Laboratory (SRNL) contribute in areas of recognized capabilities and expertise for glass waste form development to support successful startup of the WTP. SRNL support of this work is defined in the Task Technical and Quality Assurance Plan.1 This report provides results from viscosity measurements on a series of simulated nuclear waste glasses designed and fabricated at Pacific Northwest National Laboratory (PNNL). The glasses were designated the high-level waste – Aspen Process Performance Simulation (HLW-APPS) study glasses. The data provided in this report is to be used in the development, validation, and implementation of enhanced property/composition models for nuclear waste glasses.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Small Scale Melter Testing of HLW Algorithm Glasses: Matrix 1 Tests

The principal objectives of the DM100 tests were to determine the effects of glass property extremes (glass viscosity, electrical conductivity, and T1%), minimum and maximum concentrations of several major and minor glass components, +/-15% batching errors in the addition of Glass Forming Chemicals (GFCs) to the feed, and variation in the sources of boron and sodium used in the GFCs on processing rates and melter conditions (off-gas characteristics, glass processing, foaming, cold cap, etc.) at constant bubbling rate.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2026

Volumetric Additive Manufacturing of Gradient Composition Glass

Advanced optics, such as lasers or cameras, are currently limited by geometric or compositional restrictions on the silica glass components that act as focusing or refracting lenses. Currently, these glass components must be made of one homogenous material in a range of shapes and sizes limited by a few specialized vendors. However, additional flexibility and customization of these optical components could significantly improve the performance of these devices and expand the design space available to optics engineers, as would the capability to locally change the optical properties of these glass components by changing the composition of the glass as a function of location. To this end, we have developed a method to print and process gradient composition glass, using volumetric additive manufacturing (VAM) and direct ink writing (DIW), on-site at Lawrence Livermore National Lab.

36 MATERIALS SCIENCE↗