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DOE OSTI2025

Tunable and Robust Optical and Structural Properties of a Cooperative Squaraine-Dye Aggregate-DNA DX-DAE Tile System

Molecular excitons, which are excitations delocalized over multiple dyes in a wavelike manner, are of interest for a wide range of applications, including quantum information science. Numerous studies have templated a variety of synthetic dyes via a DNA scaffold to induce dye aggregation to create molecular excitons upon photoexcitation. Dye aggregate optical properties are critically dependent on relative dye geometry and local environment; therefore, an understanding of dye-dye and DNA-dye interactions is critical for advancing toward more complex DNA-dye systems. The extensively studied DNA Holliday junction (HJ) and less-studied double-crossover (DX) tile motif are fundamental test beds for designing complex and ultimately modular DNA-dye architectures. Here, we report the first study of single-linked squaraine dye aggregation and exciton delocalization on a larger and more stable (compared with the HJ) DX tile motif. We first highlight a few DNA-dye constructs that support single dyes and aggregates with distinct optical properties that are both tunable—through sample design, buffer conditions, and heat treatment—and robust to environment changes, including transfer to solid phase. Next, we assess several experimental and design considerations that demonstrate directed dye-driven assembly of a novel double-tile DNA configuration. Our results demonstrate that single-linked squaraine dyes templated to DX tiles provide a viable research path to design and evaluate dye aggregate networks that support exciton delocalization. We include herein the first report of exciton delocalization in the solid phase in a DNA-dye construct. Additionally, our findings indicate that dye aggregation impacts the assembly of the DNA-dye construct, and, in some cases, thereby cooperates with the DNA to determine a final robust system configuration. Finally, we show that a controlled annealing schedule can be employed to promote the homogeneous assembly of DNA-dye constructs. The findings in this study contribute to the understanding of DNA-dye systems and the relevant factors involved in their directed assembly to achieve specific constructs with desirable properties.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Irradiation of an enriched uranium (NaCl-UCl 3 ) fuel salt capsule, summary of nondestructive post-irradiation examinations, and solidification modeling

Molten salt reactors (MSRs) are gaining attention due to their potential for safe, carbon-free nuclear energy with reduced waste. However, licensing these reactors is hindered by limited experimental data on fueled salts, both pre- and post-irradiation. Here, the novel Molten-salt Research Temperature-controlled Irradiation (MRTI) vehicle was designed to address knowledge gaps in irradiating enriched‑uranium-bearing salts. The MRTI experiment irradiated 13 cm 3 of UCl₃-NaCl (93 % U-235) salt in the Neutron Radiography (NRAD) Reactor, achieving a burnup of 0.196 GWd/MTU over 390 h. Despite a heater failure, the thermocouple data suggested fission heat kept the salt molten. The MRTI assembly was remotely disassembled for nondestructive post-irradiation examination (PIE), which included precision gamma-ray scanning (PGS) and neutron radiography. Radiograph images showed the location of the salt and the solidification pattern. PGS results provided an early indication that activated materials of construction did not increase in relative intensity in the region of the capsule where the salt was in contact with the material of construction. Additionally, PGS data showed the presence of several gamma emitting fission products, such as Nb-95, Zr-95, Ru-103, Ce-141, and La-140, where Ru-103 had the highest counts at the bottom of the capsule. Computational fluid dynamics modeling supported observations of salt solidification patterns and proved to be a valuable tool to inform PIE activities. The MRTI experiment has thus far provided critical data and lessons learned for fuel salt PIE activities, essential for advancing the technical readiness of MSRs.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2024

Automated Calibration for Rapid Optical Spectroscopy Sensor Development for Online Monitoring

An automated platform has been developed to assist researchers in the rapid development of optical spectroscopy sensors to quantify species from spectral data. This platform performs calibration and validation measurements simultaneously. Real-time, in situ monitoring of complex systems through optical spectroscopy has been shown to be a useful tool; however, building calibration models requires development time, which can be a limiting factor in the case of radiological or otherwise hazardous systems. While calibration time can be reduced through optimized design of experiments, this study approached the challenge differently through automation. The ATLAS (Automated Transient Learning for Applied Sensors) platform used pneumatic control of stock solutions to cycle flow profiles through desired calibration concentrations for multivariate model construction. Additionally, the transients between desired concentrations based on flow calculations were used as validation measurements to understand model predictive capabilities. This automated approach yielded an incredible 76% reduction in model development time and a 60% reduction in sample volume versus estimated manual sample preparation and static measurements. The ATLAS system was demonstrated on two systems: a three-lanthanide system with Pr/Nd/Ho representing a use case with significant overlap or interference between analyte signatures and an alternate system containing Pr/Nd/Ni to demonstrate a use case in which broad-band corrosion species signatures interfered with more distinct lanthanide absorbance profiles. Both systems resulted in strong model prediction performance (RMSEP < 9%). Lastly, ATLAS was demonstrated as a tool to simulate process monitoring scenarios (e.g., column separation) in which models can be further optimized to account for day-to-day changes as necessary (e.g., baseline correction). Ultimately, ATLAS offers a vital tool to rapidly screen monitoring methods, investigate sensor fusion, and explore more complex systems (i.e., larger numbers of species).

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Experimental Investigations into the Corrosion of Alloy 625 Using NaCl-PuCl3 Molten Salt in a Natural Circulation Microloop

Molten salt reactors (MSRs) can potentially revolutionize the nuclear industry by providing a path to a near-zero nuclear waste fuel cycle, contributing to more sustainable energy sources. As a plethora of MSR developers in the United States work toward an aggressive commercialization timeline, many of their fueled-salts—notably, chloride-based compositions—have limited operational testing with nuclear material. Licensing and operating these reactors require an understanding of corrosion effects on reactor materials of construction under operational conditions. The TerraPower Molten Chloride Fast Reactor (MCFR) is a liquid-fueled chloride-salt fast reactor which has received notable interest from the utility sector based on its desirable economic characteristics. The reactor operates at low pressure but does not require the use of highly reactive chemicals, leading to a reduced use of concrete and steel during construction. Additionally, liquid fuel allows for inherently stable behavior and natural circulation during a loss-of-site-power scenario. MCFR can be refueled while operating which makes it compatible with variable generation sources such as wind and solar. MCFR is a breed-and-burn in-situ reactor that does not implement any chemical processing or separations in the fuel cycle. Only mechanical filtration of noble metals and off-gassing of noble gases are utilized while the actinides stay mixed with the fuel at all times. The MCFR will require technology development to reach commercialization. With a breed-and-burn in-situ reactor like MCFR, the transmutation of fertile U-238 to fissile Pu-239 allows for much greater fuel utilization.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2025

Future Opportunities for LWR Irradiations in US Test Reactors

After several years of relatively low activity in the field of Light Water Reactor (LWR) fuel development, the Department of Energy again began to engage in developing new fuel technologies and irradiation performance data prompted by the Fukushima Daichi nuclear accidents. New competencies for irradiation testing in material test reactors in the United States began to be developed at this time using the Advanced Test Reactor (ATR), High Flux Isotope Reactor (HFIR), Massachusetts Institute of Technology Reactor (MITR), and the Transient Reactor Test Facility (TREAT). Capsules for testing fuel and cladding materials in ATR and HFIR were deployed, a Pressurized Water Reactor (PWR) condition loop for testing fuel rods was established in ATR, cladding corrosion studies were performed using a water loop in MITR, and TREAT pulse testing capabilities were commissioned for fuel rods in water capsules. The more recent and unexpected closure of the Halden Boiling Water Reactor (HBWR) also prompted further investments in Loss of Coolant Accident (LOCA) testing capabilities at TREAT. New configurations of these test devices show further potential in enhanced steam condition control and other investigations are building toward a flowing water loop for testing transient to dryout conditions. The closure of HBWR also prompted a major project currently underway to construct additional water loops in ATR where a novel approach is being pursued to enable Boiling Water Reactor (BWR) conditions. A meaningful collaborative project was awarded to MITR which, amidst an unexpected major overhaul of the reactor, has expanded cladding corrosion test capabilities at MITR. New explorations have led to methods for unique experiments at HFIR including channel box irradiations. New device developments are also bridging toward future potential for instrumented capsule irradiation tests in ATR and HFIR. Finally, a new project referred to as the System Physics Advanced Reactor Critical facility (SPARC) is gaining traction towards a large zero-power reactor able to produce physics validation data for LWR fuel bundle designs with increased enrichment and enhanced absorbers for 24-month operation cycles. This paper provides a brief summary of the status of these irradiation testbed capabilities with an emphasis on current efforts toward future capabilities to obtain new data and maximize the performance potential of LWR fuel technologies.

Woolstenhulme, Nicolas [Idaho National Laboratory ↗

DOE OSTI2025

Constructing synthetic organosulfur additive for high voltage lithium-ion batteries

Despite its high anodic stability, common organosulfur solvents such as ethyl methyl sulfone and sulfolane typically exhibit poor solid-electrolyte interphase (SEI) formation capability. Here, to address this, the fluorinated organic sulfate 4-(trifluoromethyl)-1,3,2-dioxathiolane 2,2-dioxide (TFDTD) was developed as an effective additive for tailoring organosulfur-based electrolytes in lithium-ion batteries. This development was guided by the functionality selection principle and careful evaluation of feasibility in organic synthesis. TFDTD can be readily synthesized through the reaction between trifluoropropylene glycol and sulfuryl chloride. The ring structure of the organic sulfate enables the formation of a stable SEI on the anode, while the fluorination of the sulfate not only enhances its chemical stability and oxidation potential, but also its effectiveness to protect the anode by increasing its reduction potential, rendering it preferentially reduced on the anode surface before the decomposition of other electrolyte components. Introducing TFDTD facilitates the generation of a robust solidelectrolyte interphase on the graphite anode, significantly enhancing cell performance. Moreover, coupling the use of TFDTD with vinylene carbonate provides further protection on the cathode surface, enabling exceptionally stable, high-voltage, long-term cycling of Gr||NMC full cells.

Functionality selection principle↗

DOE OSTI2024

Improved digital construction binder solution utilizing calcium aluminate additive for Infrastructure Scale Additive Manufacturing

Oak Ridge National Laboratory (ORNL) worked with Kerneos Inc., a Division of Imerys USA, Inc. to develop an improved digital construction binder using calcium aluminate additives produced by Kerneos along with locally available concrete materials. When the two-stage (2K) binder formulation was added to commercially available Portland Limestone Cement and sand to form a digital construction mortar, its strength exceeded a number of commercially available digital construction binders both at early and later ages. At the same time, the developed formulation showed precise control of setting time after addition and showed very low shrinkage making it a strong, reliable, and easily customizable alternative to fixed proprietary digital construction binders.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Improved digital construction binder solution utilizing calcium aluminate additive for Infrastructure Scale Additive Manufacturing

36 MATERIALS SCIENCE↗

DOE OSTI2024

Dynamic Binary Complexes (DBC) as Super-Adjustable Viscosity Modifiers for Hydraulic Fracturing Fluids

In the preceding project year two, we refined three DBC formulations from a selection of over 50 different chemistries. The optimization study primarily encompassed testing for (i) reversibility extent, (ii) performance in the presence of chemical additives, (iii) adhesion and friction behavior during displacement in wellbores and pipelines, (iv) corrosion protection performance, and (v) injection performance with model fracture systems at the laboratory scale. Highly promising results obtained from all these tests signify the significant potential of DBCs in enhancing hydrocarbon recovery from unconventional reservoirs. The primary activities in the third project year included publishing experimental findings across multiple articles and conducting outreach initiatives. Throughout the year, we undertook tasks such as replicating experimental results, further optimizing various formulations and their associated experimental sets, and conducting additional tests to address missing components based on reviewer feedback and suggestions. We also explored the surfactant and friction-reduction aspects of selected formulations through drag reduction tests. In addition, we constructed an improved fracturing performance setup and performed flow injection tests. The specific DBC formulations focused on during this project period were A8/B1, A12/B5, and A10/B12. We also obtained results for additional DBC formulations and a select few commercial fracturing fluids for the purpose of comparison. Within the project's scope, we aim to enhance the experimental findings with the development of various models. The first two years focused on two key aspects: (i) the creation of a high-fidelity hydraulic fracturing model for non-Newtonian fluids to gain insights into the implementation of DBC fluids in fracking environments, and (ii) the development of a multiphase flow simulator for estimating total production, fluid saturation in the reservoir, and the creation of a fracture propagation model and kinetic Monte Carlo (kMC) models for diverse applications. In the third year, we delved into the fundamental nanostructural properties of DBCs, exploring aspects such as material chemistry, pH tunability, and control of DBC formation and stability. Subsequently, in the extension year, we conducted a systematic investigation of various building blocks containing primary, secondary, and tertiary amine functional groups to understand their impact on rheological and viscoelastic properties. Furthermore, we explored a Dissipative Particle Dynamics (DPD) model to simulate self-assembly processes with precision, creating a high-fidelity representation of relevant nanostructures. The tasks performed this year with the significant results obtained have been discussed in Section 2.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Instability of steady-state mixed-state symmetry-protected topological order to strong-to-weak spontaneous symmetry breaking

Recent experimental progress in controlling open quantum systems enables the pursuit of mixed-state nonequilibrium quantum phases. We investigate whether open quantum systems hosting mixed-state symmetry-protected topological states as steady states retain this property under symmetric perturbations. Focusing on the decohered cluster state – a mixed-state symmetry-protected topological state protected by a combined strong and weak symmetry – we construct a parent Lindbladian that hosts it as a steady state. This Lindbladian can be mapped onto exactly solvable reaction-diffusion dynamics, even in the presence of certain perturbations, allowing us to solve the parent Lindbladian in detail and reveal previously-unknown steady states. Using both analytical and numerical methods, we find that typical symmetric perturbations cause strong-to-weak spontaneous symmetry breaking at arbitrarily small perturbations, destabilize the steady-state mixed-state symmetry-protected topological order. However, when perturbations introduce only weak symmetry defects, the steady-state mixed-state symmetry-protected topological order remains stable. Additionally, we construct a quantum channel which replicates the essential physics of the Lindbladian and can be efficiently simulated using only Clifford gates, Pauli measurements, and feedback.

Shah, Jeet [University of Maryland, College Park, ↗

DOE OSTI2025

Light, High Performance and Scalable Coal-Derived Composites for Construction: Precast and Cast-in-Place Applications

The overall objective of this project was to produce a coal-based construction material that has up to ~95 weight percent (wt. %) coal with physical, chemical, and thermal properties exceeding those of ordinary Portland cement (OPC)-based construction materials. Additionally, the project aimed to minimize external binders by implementing novel mixing techniques, while exceeding the performance/cost ratio of OPC. Finally, the project was to demonstrate production of precast products via the design and fabrication of products via a bench scale process. Consistent with some of these objectives, the project successfully fabricated samples of coal-based composite materials with >80 wt% coal with physical, chemical and thermal properties on par with cement-based concrete. Select samples demonstrated compressive strengths with >7,000 psi and flexural strength of >420 psi. The composite materials minimized external binders and also demonstrated durability, as evidenced by resistance to acidic and basic solutions. Finally, larger slab and beam type samples were produced using a process developed by the Recipient, although, the process was not semicontinuous in nature. Taken together, the results of this project suggest that domestic coal has potential to serve as a replacement for cementitious materials utilized in incumbent construction technologies, which could significantly reduce the energy and emissions of the construction industry

01 COAL, LIGNITE, AND PEAT↗

DOE OSTI2025

Evaluation of Hanford Supernatant Waste Evaporation

Storage space within Hanford’s double shell tanks is running low, with only an approximate 4.1 Mgal of space remaining. Construction of additional storage space is not a pursuable option, but treatment of the waste via vacuum evaporation may be used to reduce the waste volume and increase the available amount of free space. However, without proper care and consideration, concentrating the waste may lead to harmful effects such as excessive solids generation, growth in liquid density and ionic concentration, and development of aggressive properties in the solution. OLI Studio was used to simulate a subset of DSTs using BBI ionic concentrations to generate recipes of every tank’s supernatant layer. Vacuum evaporation was performed by taking each simulated solution and bringing it to 50°C under a pressure of 60 Torr, after which the vapor phase was removed from the simulation, and the solution was brought back to ambient temperature and pressure. Several million gallons of space were created, and only about 100-200 kgal of solids were precipitated during evaporation. Minimal changes to the solution’s pitting factor occurred, and no solution is expected to develop aggressive characteristics due to evaporation. Although a theoretical result is provided, it is unique to the specific temperature and pressure value chosen for the simulation, and future transfers of waste are expected to cause changes in waste properties, which would cause the OLI recipes to lose accuracy. Though the results are not anticipated to be used as a target value or a guide, as an exercise, they show that the extent of volume gains could be equivalent to the construction of new DSTs.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

DOE OSTI2025

Continuum shock mixture models for Ni+Al multilayers: Individual layers and bulk equations of state

Continuum shock mixture models are reviewed and applied to determine the equations of state for five different compositions of Ni x Al y ⁠, as well as bulk Ni+Al reactive multilayers, by combining the fundamental property data for elemental nickel and aluminum. From the literature, we down-select and evaluate two analytical models for the mixture Hugoniot, i.e., the well-known method of kinetic energy averaging (KEA) and a recent model proposed by Jordan and Baer [J. Appl. Phys. 111, 083516 (2012)]. Fundamentally, the former method assumes pressure equilibrium, whereas the latter assumes a common particle velocity and mixture sound speed from compressible two-phase cavitating flows. Additionally, we construct thermodynamically complete equations of state by fitting Einstein oscillator series models for the specific heat at constant volume. Finally, the solid solution approximation is invoked for intermetallic compositions, which are not strictly physical mixtures. Overall, the KEA model provides a better fit to the available Ni x Al y and Ni+Al multilayer shock compression data; however, there are combinations of material properties where the performance of these two models is thought to be reversed. Moreover, the results of this work include the first analytical solution of Jordan–Baer that does not require numerical root finding, as well as proposed modifications to the Einstein oscillator series to incorporate some effects of local pressure–temperature equilibrium and reaction–diffusion. Future work is planned that will use these equations of state in mesoscale simulations to study shock-induced reaction in Ni+Al multilayers, and the intended application is illustrated with a brief 2D hydrocode example.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Fiber-optic bolometers with high-temperature tolerance and reduced time constants for fusion plasma diagnostics

Fiber-optic bolometers (FOBs) designed for plasma radiation measurement in magnetically confined fusion environments have been previously developed and tested at the DIII-D tokamak. These FOBs utilize a silicon Fabry–Perot interferometer at the fiber tip for temperature measurement and a gold disk as a radiation absorber. This paper presents recent advancements in the development of FOBs with reduced cooling time constants and enhanced temperature tolerance. We also demonstrate high-temperature operation and report findings from irradiation tests. By incorporating a copper sensor holder as a thermal sink and integrating two closely packed sensor heads into a compact design, the cooling time constants were reduced to ∼100 ms in vacuum, while minimizing uncertainties caused by temperature gradients. The FOBs were subjected to heating at 400 °C for five hours, with no observed degradation in noise performance post-heating. High-temperature operation tests were conducted at ∼220 °C using a 404 nm square-wave modulated laser to simulate the plasma radiation. In addition, four FOBs constructed from copper-coated pure-silica fibers were fabricated and underwent irradiation testing, enduring a total γ-radiation dose of 15.2 MGy and a neutron fluence of 1.6 × 10 18 n/cm 2 . As a result, the FOBs maintained their physical integrity and the optical signal shows high visibility throughout the test.

42 ENGINEERING↗

DOE OSTI2026

Faster Randomized Dynamical Decoupling

We present a randomized dynamical decoupling (DD) protocol that can substantially improve the performance of any given deterministic DD scheme for suppressing coherent noise by using no more than two additional pulses. Our construction is implemented by probabilistically applying sequences of pulses, which, when combined, effectively eliminate the error terms that scale linearly with the system-environment coupling strength. As a result, we show that a randomized protocol using a few pulses can outperform deterministic DD protocols that require considerably more pulses. Furthermore, we prove that the randomized protocol provides an improvement compared to deterministic DD sequences that aim to reduce the error in the system’s Hilbert space, such as Uhrig DD, which had been previously regarded to be optimal. To rigorously evaluate the performance, we introduce new analytical methods suitable for analyzing higher-order DD protocols that might be of independent interest. Here, we also present numerical simulations confirming the significant advantage of using randomized protocols compared to widely used deterministic protocols.

Quantum algorithms & computation↗

DOE OSTI2025

Custom Equipment Development for Processing of Surplus Plutonium

Facilities and Material • Location: Savannah River Site K-Area, South Carolina • Plutonium designated as surplus is blended with adulterant material, re-packaged and shipped to WIPP in New Mexico • Currently one operational glovebox for downblending, facility modifications and construction of three additional glovebox lines in progress • Current operations are highly manual requiring full PPE and reader/worker steps

Krementz, Daniel [Savannah River National Laborato↗

DOE OSTI2026

Additive-Induced Morphology Change of Polymer Film Enables Enhanced Charge Mobility and Faster Organic Electrochemical Transistor Switching

Conjugated polymers (CPs) play an important role in organic electrochemical transistors (OECTs) for bioelectronics and related applications, where they serve as channel materials. Currently, most successful polymers for CPs are re-engineered from traditional CPs by replacing hydrophobic alkyl side chains with hydrophilic ethylene glycol or ionic groups. Frustratingly, the enhanced ion transport often compromises the charge mobility of the original CP. In this work, we present an additive-mediated method to construct a modified poly(3-hexylthiophene) (P3HT) film to enable efficient ion migration. The additive is designed with a cleavable diazo group that releases nitrogen and 2-methoxyethanol, a volatile compound, to alter the P3HT film morphology. OECTs based on the film exhibit improved response times. Interestingly, the process also enhances the crystallinity of P3HT, leading to higher hole mobility compared with pristine P3HT. This study proposes an in situ strategy to achieve the functionality of the OMIEC via morphological regulation, offering a promising route to simultaneously enhance both ion accessibility and charge mobility.

Organic polymers↗

DOE OSTI2024

Impacts of Model Building Energy Codes

The Department of Energy (DOE) Building Energy Codes Program (BECP) periodically evaluates national and state-level impacts associated with energy codes in residential and commercial buildings. Pacific Northwest National Laboratory (PNNL), funded by DOE, conducted an assessment of the prospective impacts of national model building energy codes from 2010 through 2040. A previous PNNL study evaluated the impact of the Building Energy Codes Program. A 2016 study looked more broadly at overall code impacts and this report describes the methodology used for the assessment and presents the impacts in terms of energy savings, consumer cost savings, and reduced emissions at the state level and at aggregated levels. In 2021, DOE conducted an interim and limited update to its 2016 study to evaluate potential building code updates using the 2016 methodology. That interim update includes estimated savings resulting from updates to the model energy codes, including the ANSI/ASHRAE/IES Standard 90.1-2016 (ASHRAE 90.1-2016) and 2019 editions, as well as the 2018 and 2021 International Energy Conservation Code (IECC). In 2023, DOE developed a fully updated report that includes code updates (ASHRAE 90.1-2019 and 2021 IECC), as well as additional enhancements and updates, including updated energy prices, annual floorspace additions, state code adoption dates, and emission factors, among others. This current version is another fully updated report that includes code updates (ASHRAE 90.1-2022 and 2024 IECC), as well as additional enhancements and updates, including updated energy prices, state code adoption dates, emission factors, and renewable energy contribution among others. Energy codes follow a three-phase cycle that starts with the development of a new model code, proceeds with the adoption of the new code by states and local jurisdictions, and finishes when the new code is implemented and builders, architects, and engineers are required to comply with the new provisions. The development of new model code editions creates the potential for increased energy savings. After a new model code is adopted, potential savings are realized in the field when new buildings (or additions and alterations) are constructed to comply with the new code. The contributions of all three phases are crucial to the overall impact of codes and are considered in this assessment. Figure ES.1 schematically describes the analysis framework. Energy savings are expressed in terms of energy use intensity (EUI) in the figure.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗