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DOE OSTI2025

Direct measurement of thermal Knudsen forces in rarefied gas environments

At micro- and nanoscales, momentum transfer between surfaces is influenced by various physical mechanisms, including quantum fluctuations, electromagnetic interactions, electric charges, and the dynamics of (rarefied) gases. Under non-isothermal conditions, rarefied gases give rise to thermal Knudsen forces whose magnitudes strongly depend on the gas species and surface characteristics. Knudsen forces are particularly relevant in nanotechnology, optical manipulation, and aerospace systems, where gas rarefaction occurs due to highly confined geometries, sub-micrometer length scales, and reduced particle densities. Despite their significance, predictive modeling of Knudsen forces is limited by a lack of comprehensive experimental data across diverse materials and surface morphologies. Here, in this work, we present a highly sensitive and adaptable measurement platform capable of directly quantifying Knudsen forces using a suspended, interchangeable micro-cantilever within controlled rarefied helium and nitrogen environments. The system integrates optical fiber interferometry to precisely capture out-of-plane displacements at sub-micrometer resolution, driven by Knudsen forces. From the empirical data, we derive a robust correlation linking the magnitudes of Knudsen forces to energy accommodation coefficients, offering deeper insights into the underlying gas–surface interaction mechanisms.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Microstructure, Thermal, and Mechanical Properties Relationships in U and UZr Alloys (Final Report)

Uranium-zirconium (U-Zr) alloys are candidate fuel systems for transmutation based reactors that can be used to burn long-lived minor actinides and fission products in fast spectrum reactors. Metallic fuels have also been gaining more recent attention for applications as accident tolerant fuels, as well as for use in small modular reactors. This research focused on a “science-based” approach to capture the connections between U and U-Zr alloys’ three-dimensional (3-D) microstructure, thermal properties, and mechanical properties through closely coordinated experiments and modeling efforts from the unirradiated to the irradiated fuels. Advanced characterization and modeling techniques were used to understand irradiation-induced microstructural evolution and its direct impact on the thermal and mechanical properties of U and U-Zr fuel. Closely coordinated experiments and modeling were performed to provide crucial data that does not currently exist. Overall, this research spanned multiple length and time scales within the models and experiments. The scope of the research encompassed the understanding of the irradiation effects in U and various U-Zr alloys with particular attention paid to three task areas: (1) microstructural evolution, (2) in-situ/ex-situ thermal and mechanical properties, and (3) multiscale modeling connections to microstructure, thermal, and mechanical properties. This research resulted in (1) the 3-D characterization of neutron irradiated U-Zr fuel in multiple phase regions to better understand fission gas swelling and constituent redistribution, (2) development of a microstructural model linking thermal and mechanical properties via in situ Raman and nanoindentation, (3) and mesoscale phase field modeling was coupled with the AEH method in the MOOSE framework was used to calculate the effective thermal conductivities of U-Zr fuels consisting of α-U and δ-UZr 2 heterogeneous microstructures.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2020

Flow Channeling in Fracture Networks: Characterizing the Effect of Density on Preferential Flow Path Formation

Flow channelization is a commonly observed phenomenon in fractured subsurface media where the flow of fluids is restricted primarily to highly transmissive fracture networks surrounded by a low-permeability rock matrix. The multiscale structural heterogeneity of these networks results in multiscale flow channelization where preferential flow paths form at length scales ranging from the entire system down to the subfracture size. We present an analysis of how one of the largest scales in fractured media, the network density, influences the degree of flow channeling that occurs using an ensemble of semigeneric three-dimensional discrete fracture network (DFN) simulations. We construct 10 DFNs, whose fracture lengths follow a power law distribution, at four densities for a total of 40 networks. We characterize their structure in terms of the network topology and geometry. Eulerian and Lagrangian observations of the steady-state flow fields obtained within the networks are used to quantify the degree of flow channelization at the network scale. We introduce a measure for the importance-ranking/hierarchy of different flow paths in the network using graph-based analysis of Lagrangian transport by which the degree of flow channeling between networks is compared. These flow observations are then linked to the structural properties of the networks. In general, network-scale flow channeling decreases as the network density increases. However, at low densities, there is more uniform flow within the entire connected network than in high-density networks. We also demonstrate how standard transport observables can be used to infer the degree of flow channelization occurring within a fracture network.

58 GEOSCIENCES↗

DOE OSTI2022

Actinides and Correlated Electron Materials

The Actinides and Correlated Electron Materials area of leadership spans Los Alamos National Laboratory competency in actinide materials research dating to the Manhattan Project as articulated in the Integrated Plutonium Science and Research Strategy and competency in strongly correlated electron systems dating back to at least the early 1980s. This area of leadership focuses on the goals of discovering, understanding, and controlling emergent electronic states and predictive performance of actinide materials. They are quintessentially linked by the fact that the physics of actinides—and plutonium in particular—are governed by strong electronic correlations. Not only is the electronic structure of actinides dictated by fine details of electron correlations, but chemical bonding and physical structure are as well. Hence, by addressing the first goal of this leadership area we can significantly accelerate progress on the second goal. To understand such matter requires probing the intertwined spin, charge, orbital, and lattice degrees of freedom with greater precision and developing models that accurately predict the consequences of these coupled degrees of freedom, on multiple length and time scales and including acute reactivity and effects of self-irradiation phenomena in these materials.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Efficient Routing of Quantum LDPC Codes on Programmable 2D Toric Architectures

Quantum low-density parity-check codes are promising candidates towards scalable fault-tolerant quantum computation. Among these, bivariate bicycle (BB) codes offer superior encoding rates and large code distance compared to surface codes. However, their requirement on long-range stabilizer measurements poses significant challenges for implementation on realistic hardware with limited connectivity, such as superconducting circuit platforms. In this work, we introduce a novel hardware-software co-design that leverages a programmable communication network architecture to address these limitations. Our approach utilizes a 2D toric network of oscillators as a flexible communication fabric linking qubits at each site. Such architecture significantly reduces the number of long-range couplers required from O ( n ) to O (√ n ). Dual-rail qubits, along with native gates including Swap-Wait-Swap gates and beamsplitter SWAPs, ensure that long-range two-qubit gates can be executed with high fidelity and low latency. To further enhance performance, our qubit layout and routing algorithm utilize symmetries of the codes and enable maximum parallelism for long-range two-qubit gates, maintaining a low syndrome extraction cycle duration and scalability over the code length. We perform circuit-level simulation with realistic noise modeling based on experimental hardware parameters, observing an logical error rate per logical qubit per cycle of 3.06% for [[18,4,4]] BB code, 2.6× less than the existing experimental result. These findings provide a practical roadmap and identify key technological advancements needed to achieve low-overhead fault-tolerant quantum computing at scale.

Liu, Kun [Yale Univ., New Haven, CT (United States↗

DOE OSTI2021

Isotope Effects in Thermal Neutron Scattering [Slides]

AMPX links Thermal Scattering Law (TSL) libraries to isotopes in the resolved resonance region. No guidance is given in the TSL files or the ENDF format if this is acceptable or advised, which can lead to issues for researchers.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2023

A first principles analysis of potential-dependent structural evolution of active sites in Fe-N-C catalysts

Fe-N-C (iron–nitrogen–carbon) electrocatalysts have emerged as potential alternatives to precious metal-based materials for the oxygen reduction reaction (ORR). However, the structure of these materials under electrochemical conditions is not well understood, and their poor stability in acidic environments poses a formidable challenge for successful adoption in commercial fuel cells. To provide molecular-level insights into these complex phenomena, we combine periodic density functional theory (DFT) calculations, exhaustive treatment of coadsorption effects for ORR reaction intermediates, including O and OH, and comprehensive analysis of solvation stabilization effects to construct voltage-dependent ab initio thermodynamic phase diagrams that describe the in situ structure of the active sites. These structures are further linked to activity and stability descriptors that can be compared with experimental parameters such as the half-wave potential for ORR and the onset potential for carbon corrosion and CO 2 evolution. The results indicate that pyridinic Fe sites at zigzag carbon edges, as well as other edge sites, exhibit high activity for ORR compared to sites in the bulk. However, edges neighboring the active sites are prone to instability via overoxidation and consequent site loss. The results suggest that it could be beneficial to synthesize Fe-N-C catalysts with small sizes and large perimeter edge lengths to enhance ORR activity, while voltage fluctuations should be limited during fuel cell operation to prevent carbon corrosion of overoxidized edges.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

A correlation between seasonally changing photoperiod, whole body lipid, and condition factor in juvenile spring Chinook salmon (Oncorhynchus tshawytscha)

The regulation of lipid stores is a central process for the physiology and ecology of fishes. Seasonal variation in lipid stores has been directly linked to survival of fishes across periods of food deprivation. We assessed whether a seasonally changing photoperiod was correlated to seasonal changes in energetic status to help better understand these important processes. Groups of first feeding Chinook salmon fry were introduced to a seasonal photoperiod cycle, but the point of entrance into the seasonal cycle varied from near the winter solstice (December), to either side of the spring equinox (February & May). Temperature and feeding rate were similar for all treatments. Subsequently, condition factor and whole body lipid content were assessed through a seasonal progression. Throughout most of the experiment, length and weight did not differ between the different photoperiod treatments, however whole body lipid and Fulton’s condition factor did. Furthermore, changes in both whole body lipid and Fulton’s condition factor in all treatment groups followed a similar seasonal pattern that was inversely related to day length (highest K and lipid levels found during days with the least light). These results suggest that regardless of age or size, there is a correlation between seasonal changes in photoperiod and changes in body composition in juvenile Chinook salmonids.

Spangenberg, Dina K. (ORCID:000000018861395X)↗

DOE OSTI2022

Isotope Effects in Thermal Neutron Scattering [Slides]

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2023

Linking water quality, fouling layer composition, and performance of reverse osmosis membranes

Fouling of polyamide membranes during reverse osmosis (RO) is a major challenge for adopting membrane technologies to treat highly contaminated waters, especially those containing organic foulants (e.g., natural organic matter (NOM), polysaccharides) and dominant cations (e.g., sodium, magnesium, calcium). Here, this work combines bench-scale membrane fouling experiments with detailed characterization of feedwater chemistry and fouling layer composition/morphology to reveal fundamental mechanisms of (in)organic fouling during RO. Divalent cations are shown to promote fouling by hydrophobic NOM containing aromatic and carboxyl groups, while NOM fouling in the presence of a monovalent cation, sodium, occurs by smaller fulvic acids containing larger fractions of carboxyl groups and other oxygen-rich moieties. Calcium-carboxyl bridging occurs in solution and near the membrane surface to induce NOM aggregation on nanometer length scales. In complex waters containing foulant mixtures, co-fouling by calcium-carboxyl bridging and CaCO 3 precipitation influence membrane performance at longer timeframes. However, the flux decline observed for the co-fouling mechanism was less significant than the sum of its parts, suggesting both synergistic and antagonistic fouling mechanisms should be considered in membrane design/operation. These results encourage the design of pretreatment processes to reduce concentrations of multivalent ions and hydrophobic NOM in RO feedwaters, and of membrane materials to limit attachment/deposition of aggregates to/on polyamide surfaces.

42 ENGINEERING↗

DOE OSTI2020

Population Dynamics and Temporal Trends of Bull Trout in the East Fork Salmon River, Idaho

Abstract Because of their long-term listing under the Endangered Species Act, much interest has been placed on estimating population vital rates for Bull Trout Salvelinus confluentus, but the biotic and abiotic factors that influence the interannual variability in those vital rates have rarely been evaluated. We used mark–recapture data to estimate fish growth, survival, and trends in abundance for fluvial adult Bull Trout in the East Fork Salmon River, Idaho. Over an 8-year period, a total of 1,205 individual Bull Trout were collected at a weir on the East Fork Salmon River (29 km upstream of its confluence with the Salmon River) during June–September, of which 420 were recaptures from prior years. Bull Trout varied in length from 215 to 756 mm and achieved a slightly larger asymptotic length and a slightly lower rate of growth relative to other fluvial and adfluvial Bull Trout populations. Apparent survival averaged 0.42 across all years, which was similar to previous studies estimating apparent survival for Bull Trout. The number of emigrating anadromous salmonid smolts in the upper Salmon River basin positively influenced East Fork Salmon River Bull Trout growth and survival, and survival was higher in years with lower annual discharge. Assessment of population growth via linear regression analysis indicated that the Bull Trout population was increasing during the study period (λ = 1.08; 95% confidence interval = 1.03–1.14). Our findings highlight the ecological link between the abundance of wild and hatchery Chinook Salmon Oncorhynchus tshawytscha, Sockeye Salmon O. nerka, and steelhead O. mykiss smolts and growth and survival of adult Bull Trout in systems where these species occur in sympatry.

Roth, Curtis J.↗

DOE OSTI2024

Response of hypoxia to future climate change is sensitive to methodological assumptions

Climate-induced changes in hypoxia are among the most serious threats facing estuaries, which are among the most productive ecosystems on Earth. Future projections of estuarine hypoxia typically involve long-term multi-decadal continuous simulations or more computationally efficient time slice and delta methods that are restricted to short historical and future periods. We make a first comparison of these three methods by applying a linked terrestrial–estuarine model to the Chesapeake Bay, a large coastal-plain estuary in the eastern United States. Results show that the time slice approach accurately captures the behavior of the continuous approach, indicating a minimal impact of model memory. However, increases in mean annual hypoxic volume by the mid-twenty-first century simulated by the delta approach (+ 19%) are approximately twice as large as the time slice and continuous experiments (+ 9% and + 11%, respectively), indicating an important impact of changes in climate variability. Our findings suggest that system memory and projected changes in climate variability, as well as simulation length and natural variability of system hypoxia, should be considered when deciding to apply the more computationally efficient delta and time slice methods.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

On the relation between active-region lifetimes and the autocorrelation function of light curves

ABSTRACT Rotational modulation of stellar light curves due to dark spots encloses information on spot properties and, thus, on magnetic activity. In particular, the decay of the autocorrelation function (ACF) of light curves is presumed to be linked to spot/active-region lifetimes, given that some coherence of the signal is expected throughout their lifetime. In the literature, an exponential decay has been adopted to describe the ACF. Here, we investigate the relation between the ACF and the active-region lifetimes. For this purpose, we produce artificial light curves of rotating spotted stars with different observation, stellar, and spot properties. We find that a linear decay and respective time-scale better represent the ACF than the exponential decay. We therefore adopt a linear decay. The spot/active-region time-scale inferred from the ACF is strongly restricted by the observation length of the light curves. For 1-yr light curves our results are consistent with no correlation between the inferred and the input time-scales. The ACF decay is also significantly affected by differential rotation and spot evolution: strong differential rotation and fast spot evolution contribute to a more severe underestimation of the active-region lifetimes. Nevertheless, in both circumstances the observed time-scale is still correlated with the input lifetimes. Therefore, our analysis suggests that the ACF decay can be used to obtain a lower limit of the active-region lifetimes for relatively long-term observations. However, strategies to avoid or flag targets with fast active-region evolution or displaying stable beating patterns associated with differential rotation should be employed.

Santos, A. R. G. (ORCID:0000000171956542)↗

DOE OSTI2022

Implementation of a Model Predictive Control Strategy to Regulate Temperature Inside Plug-Flow Solar Reactor With Countercurrent Flow

Abstract Solar-driven thermochemical energy storage systems are proven to be promising energy carriers (solar fuels) to utilize solar energy by using reactive solid-state pellets. However, the production of solar fuel requires a quasi-steady-state process temperature, which represents the main challenge due to the transient nature of solar power. In this work, an adaptive model predictive controller (MPC) is presented to regulate the temperature inside a tubular solar reactor to produce solid-state solar fuel for long-term thermal storage systems. The solar reactor system consists of a vertical tube heated circumferentially over a segment of its length by concentrated solar power, and the reactive pellets (MgMn2O4) are fed from the top end and flow downwards through the heated tube. A countercurrent flowing gas supplied from the lower end interacts with flowing pellets to reduce it thermochemically at a temperature range of 1000—1500 °C. A low-order physical model was developed to simulate the dynamics of the solar reactor including the reaction kinetics, and the proposed model was validated numerically by using a 7-kW electric furnace. The numerical model then was utilized to design the MPC controller, where the control system consists of an MPC code linked to an adaptive system identification code that updates system parameters online to ensure system robustness against external disturbances (sudden change in the flow inside the reactor), model mismatches, and uncertainty. The MPC controller parameters are tuned to enhance the system performance with minimum steady-state error and overshoot. The controller is tested to track different temperature ranges between 500 °C and 1400 °C with different particles/gas mass flowrates and ramping temperature profiles. Results show that the MPC controller successfully regulated the reactor temperature within ± 1 °C of its setpoint and maintained robust performance with minimum input effort when subjected to sudden changes in the amount of flowing media and the presence of chemical reaction.

Engineering↗

DOE OSTI2023

Micro‐ and Nanoscale Heterogeneities in Zeolite Beta as Measured by Atom Probe Tomography and Confocal Fluorescence Microscopy

Micro- and nanoscale information on the activating and deactivating coking behaviour of zeolite catalyst materials increases our current understanding of many industrially applied processes, such as the methanol-to-hydrocarbon (MTH) reaction. Atom probe tomography (APT) was used to reveal the link between framework and coke elemental distributions in 3D with sub-nanometre resolution. APT revealed 10–20 nanometre-sized Al-rich regions and short-range ordering (within nanometres) between Al atoms. With confocal fluorescence microscopy, it was found that the morphology of the zeolite crystal as well as the secondary mesoporous structures have a great effect on the microscale coke distribution throughout individual zeolite crystals over time. Additionally, a nanoscale heterogeneous distribution of carbon as residue from the MTH reaction was determined with carbon-rich areas of tens of nanometres within the zeolite crystals. Finally, a short length-scale affinity between C and Al atoms, as revealed by APT, indicates the formation of carbon-containing molecules next to the acidic sites in the zeolite.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Review and meta-analysis of electron temperatures from high-intensity laser–solid interactions

The accelerated electron spectrum from high-intensity laser–solid interaction is often conveniently described using a Boltzmann distribution, whose temperature is known within the field as the hot-electron temperature. The importance of the electron temperature is highlighted by the sheer number of experimental and simulation studies on the subject over the past three decades. Recently, multi-kJ, multi-ps pulses have yielded electron spectra with temperatures far beyond the expected ponderomotive result. Expressions that predict the electron temperature considering laser parameters beyond intensity and wavelength have been developed, albeit using small datasets. In this review, we present what is, to the best of our knowledge, the largest dataset of electron temperatures gathered from experimental measurements and particle-in-cell simulations. This dataset allows us to compare existing analytical and empirical hot-electron temperature scaling models over a wide parameter range. We also develop new scaling models that incorporate the laser pulse duration of the laser and the plasma scale length. Three models that include pulse-duration and scale length dependence are especially successful at predicting both simulated and experimental data. The dataset will soon be made publicly available to encourage further investigation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2024

Comprehensive Dynamics in a Polyelectrolyte Complex Coacervate

The linear viscoelastic response, LVR, of a hydrated polyelectrolyte complex coacervate, PEC, was evaluated over a range of frequencies, temperatures, and salt concentrations. The PEC was a nearly stoichiometric blend of a quaternary ammonium poly([3-(methacrylamido)propyl]trimethylammonium chloride), PMAPTAC, and poly(2-acrylamido-2-methyl-1-propanesulfonic acid sodium salt), PAMPS, an aliphatic sulfonate, selected because they remain fully charged over the conditions of use. Narrow molecular weight distribution polyelectrolytes were prepared using fractionation techniques. A partially deuterated version of PMAPTAC was incorporated to determine its coil radius of gyration, R g , within PECs using small-angle neutron scattering. Chain dimensions were determined to be Gaussian with a Kuhn length of 2.37 nm, which remained constant from 25 to 65 °C. The LVR for a series of matched molecular weight PECs, mostly above the entanglement threshold, exhibited crossovers of modulus versus frequency classically attributed to the reptation time, relaxation between entanglements, and the relaxation of a Kuhn length of units (the “monomer” time). The scaling for zero shear viscosity, η 0 , versus chain length, N, was η 0 ~ N 3.1 , in agreement with “sticky reptation” theory. The lifetime and activation energy, E p , of a pair between polyanion and polycation repeat units, Pol + Pol – , were determined from diffusion coefficients of salt ions within the PEC. The activation energy for LVR of salt-free PECs was 2E p , showing that the key mechanism limiting the dynamics of undoped PECs is pair exchange. An FTIR technique was used to distinguish whether SCN– acts as a counterion or a co-ion within PECs. Doping of PECs with NaSCN breaks Pol + Pol – pairing efficiently, which decreases effective cross-linking and decreases viscosity. Finally, an equation was derived that quantitatively predicts this effect.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Molecular basis of force-pCa relation in MYL2 cardiomyopathy mice: Role of the super-relaxed state of myosin

Here, in this study, we investigated the role of the super-relaxed (SRX) state of myosin in the structure–function relationship of sarcomeres in the hearts of mouse models of cardiomyopathy-bearing mutations in the human ventricular regulatory light chain (RLC, MYL2 gene). Skinned papillary muscles from hypertrophic (HCM–D166V) and dilated (DCM–D94A) cardiomyopathy models were subjected to small-angle X-ray diffraction simultaneously with isometric force measurements to obtain the interfilament lattice spacing and equatorial intensity ratios (I 11 /I 10 ) together with the force-pCa relationship over a full range of [Ca 2+ ] and at a sarcomere length of 2.1 μm. In parallel, we studied the effect of mutations on the ATP-dependent myosin energetic states. Compared with wild-type (WT) and DCM–D94A mice, HCM–D166V significantly increased the Ca 2+ sensitivity of force and left shifted the I 11 /I 10 -pCa relationship, indicating an apparent movement of HCM–D166V cross-bridges closer to actin-containing thin filaments, thereby allowing for their premature Ca 2+ activation. The HCM–D166V model also disrupted the SRX state and promoted an SRX-to-DRX (super-relaxed to disordered relaxed) transition that correlated with an HCM-linked phenotype of hypercontractility. While this dysregulation of SRX ↔ DRX equilibrium was consistent with repositioning of myosin motors closer to the thin filaments and with increased force-pCa dependence for HCM–D166V, the DCM–D94A model favored the energy-conserving SRX state, but the structure/function–pCa data were similar to WT. Our results suggest that the mutation-induced redistribution of myosin energetic states is one of the key mechanisms contributing to the development of complex clinical phenotypes associated with human HCM–D166V and DCM–D94A mutations.

59 BASIC BIOLOGICAL SCIENCES↗