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DOE OSTI2024

Surface-mediated spontaneous emulsification of the acylated peptide, semaglutide

Acylated peptides composed of glucagon-like peptide-1 receptor agonists modified with a fatty acid side chain are an important class of therapeutics for type 2 diabetes and obesity but are susceptible to an unusual physical instability in the presence of hydrophobic surfaces, i.e., spontaneous emulsification, also known as ouzo formation in practice. In this work, light scattering, small-angle X-ray scattering, and circular dichroism measurements are used to characterize the physical properties of the semaglutide colloidal phase, including size distribution, shape, secondary structure, internal structure, and internal composition, as a function of solution physico-chemical conditions. The existence and size of the colloids formed are successfully predicted by a classical Rayleigh model, which identifies the parameters controlling their size and formation. Colloid formation is found to be catalyzed by hydrophobic surfaces, and formation rates are modeled as an autocatalytic reaction, enabling the formation of a master curve for various surfaces that elucidates the mechanism. Surfaces differ due to differences in surface wettability, which can be correlated with Hansen solubility parameters. This work provides insights into this unusual colloidal phenomenon and guides the peptide synthesis process and drug product formulation in the pharmaceutical industry.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2026

Effect of polymer structure and material properties on mechanochemical reaction environments for polymer recycling

Plastic waste accumulation necessitates innovative recycling approaches to achieve sustainability goals. Mechanochemical depolymerization offers a solvent-free, energy-efficient route to convert polymers into valuable monomers. In addition to their chemical properties, the way that polymers absorb kinetic energy is a key parameter of any mechanochemical process. This perspective explores the principles underpinning mechanochemical recycling, emphasizing how deformation and localized transient heating mediate energy transfer between impacts and localized excitations. Key factors such as polymer crystallinity, molecular weight, viscoelasticity, and thermal effects are analyzed to elucidate their role in energy transfer mechanisms during ball milling. This work establishes a foundational framework for the design and optimization of mechanochemical recycling by connecting polymer response to mechanical energy with the intention to improve depolymerization efficiency. Future research opportunities are outlined to advance the integration of polymer science and mechanochemistry for scalable, sustainable plastic upcycling.

ball mill↗

DOE OSTI2023

Elucidating Trivalent Ion Adsorption at Floating Carboxylic Acid Monolayers: Charge Reversal or Water Reorganization?

Here we study the adsorption of trivalent neodymium on floating arachidic acid films at the air–water interface by two complementary surface specific probes, sum frequency generation spectroscopy and X-ray fluorescence near total reflection. In the absence of background ions, neodymium ions compensate for the surface charge of the arachidic acid film at a bulk concentration of 50 μM without any charge reversal. Increasing the bulk concentration to 1 mM does not change the neodymium surface coverage but affects the interfacial water structure significantly. In the presence of a high concentration of NaCl, there is overcharging at 1 mM Nd 3+ , i.e., 30% more Nd 3+ than needed to compensate for the surface charge. These results show that the total coverage of neodymium ions is not enough to describe the complete picture at the interface, and interfacial water and ion coverage needs to be considered together to understand more complex ion adsorption and transport processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Melt Pool and Heat Treatment Optimization for the Fabrication of High-Strength and High-Toughness Additively Manufactured 4340 Steel

Additively manufactured (AM) components offer superior design flexibility compared to their conventionally manufactured counterparts, and optimizing processing parameters is key to achieving high-quality depositions with desirable and predictable mechanical properties. This study was focused on 4340 steel fabricated using laser powder bed fusion (LPBF), and 42 laser power and scan speed combinations have been systematically investigated to determine an optimized melt pool geometry that would ensure fully-dense parts. The AM material was compared with a wrought 4340 equivalent and studied in two customized heat treated conditions, optimized for strength and toughness, respectively. The microstructures of the as-fabricated and heat treated AM and wrought materials were characterized to assess differences introduced by the layer-by-layer fabrication process and subsequent heat treatment. Tensile properties of both materials were also evaluated and demonstrate that the AM materials offer equal or superior properties compared to the wrought equivalents. Differences in fracture surface morphologies indicate the distinct failure mechanisms associated with the materials’ characteristic microstructures, and the role of inclusions in the failures was studied to elucidate these differences. Complementary to the experimental investigations, the dataset was leveraged to make recommendations for future design of experiments to optimize AM build parameters in other material systems. A statistical Monte Carlo analysis was used to predict the interpolation error produced using reduced datasets and to enable informed processing parameters selection. These findings are discussed to make recommendations for the use of AM materials for high-integrity structural applications.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Solid face sheets enable lattice metamaterials to withstand high-amplitude impulsive loading without yielding

Owing to their ability to provide tunable mechanical responses, lattice materials are frequently studied to elucidate their response to static and dynamic loads. However, these roles are typically in opposition: static loads must be supported sufficiently far away from the onset of buckling or yielding, whereas dynamic loads are typically ameliorated by crushing of the lattice, which provides excellent energy-absorption due to the large plastic deformation accompanying densification. In contrast, this work considers the octet truss as an exemplar topology, in a structural role where it must simultaneously support static loads while enduring high-amplitude impulsive loads. This study focuses on the ability to withstand impulsive loads without yielding, an essential prerequisite to enduring dual loading. Computational studies using the ALE3D hydrocode were performed to examine the response of the octet truss under a short temporal width impulse shape associated with laser-driven shocks. A key finding was that covering the lattice with a solid face sheet and treating this face sheet thickness as a design variable allows the Taylor-like pulse to be attenuated prior to entering the weaker lattice, at the cost of added mass up front. Experimental validation was accomplished by laser-driven shock testing, using octet trusses printed out of Ti-5Al-5V-5Mo-3Cr. The results show that for a given quantity of mass, the attenuation is maximized when as much mass as possible is moved into the face sheet, leaving a more slender lattice structure. The effect of placing mass in the face sheet rather than lattice beams dominates the effect of relative density, to the point where a low-mass structure with most of the mass concentrated in the face sheet can outperform a high-mass structure with most of the mass in the lattice. Finally, by further understanding the propagation of short pulse width waves within under-dense structures, this study expand the domain of applicability of such structures, including lattice materials, to challenging dual-loading regimes spanning decades of strain rates.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Insights into lithium ion deposition on lithium metal surfaces

Lithium metal is among the most promising anodes for the next generation of batteries due to its high theoretical energy density and high capacity. Challenges such as extreme reactivity and lithium dendrite formation have kept lithium metal anodes away from practical applications. However, the underlying mechanisms of Li ion deposition from the electrolyte solution onto the anode surface are still poorly understood due to their inherent complexity. In this work, density functional theory calculations and thermodynamic integration via constrained molecular dynamics simulations are conducted to study the electron and ion transfer between lithium metal slab and the electrolyte in absence of an external field. Here, we explore the effect of the solvent chemistry and structure, distance of the solvated complex from the surface, anion–cation separation, and concentration of Li-salts on the deposition of lithium ions from the electrolyte phase onto the surface. Ethylene carbonate (EC), 1,2-dimethoxyethane (DME), 1,3-dioxolane (DOL), and mixtures of them are used as solvents. These species compete with the salt anion and the Li cation for electron transfer from the surface. It is found that the structure and properties of the solvation shell around the lithium cation has a great influence on the ability of the cation to diffuse as well as on its surrounding electron environment. DME molecules allow easier motion of the lithium ion compared with EC and DOL molecules. The slow growth approach allows the study of energy barriers for the ion diffusion and desolvation during the deposition pathway. This method helps elucidating the underlying mechanisms on lithium-ion deposition and provides a better understanding of the early stages of Li nucleation.

25 ENERGY STORAGE↗

DOE OSTI2022

The Presence of Virus Neutralizing Antibodies Is Highly Associated with Protection against Virulent Challenge in Domestic Pigs Immunized with ASFV live Attenuated Vaccine Candidates

African swine fever virus (ASFV) is currently producing a pandemic affecting a large area of Eurasia, and more recently, the Dominican Republic in the Western Hemisphere. ASFV is a large and structurally complex virus with a large dsDNA genome encoding for more than 150 genes. Live attenuated virus strains can induce protection in domestic swine against disease produced by homologous virulent parental viruses. The roles of the different immune mechanisms induced by the attenuated strains in protection still need to be understood. In particular, the role of ASFV neutralizing antibody in protection still is an important controversial issue to be elucidated. Here we present the development of a novel methodology to detect virus neutralizing antibodies based on the reduction of virus infectivity in a Vero cell adapted ASFV strain. The described method was used to assess levels of virus neutralizing antibodies in domestic swine inoculated with live attenuated ASFV. Results demonstrated a high association between the presence of virus neutralizing antibodies and protection in 84 animals immunized with the recombinant vaccine candidates ASFV-G-Δ9GL/ΔUK or ASFV-G-ΔI177L. To our knowledge, this is the first report demonstrating an association between virus neutralizing antibodies and protection against virulent challenge in such a large number of experimental individuals.

59 BASIC BIOLOGICAL SCIENCES↗

NASA NTRS1986

Determination of band oscillator strengths of atmospheric molecules from high resolution vacuum ultraviolet cross section measurements

An account is given of progress in work on (1) the determination of band oscillator strengths of the Schumann-Runge absorption bands of (16)O2 and (18)O2 from cross section measurements conducted at 79 K; (2) the determination of the absolute absorption cross section of the Schumann-Runge bands of (16)O(18)O from optical depth measurements performed on mixtures of (16)O2, (18)O2 and (16)O(18)O at 79K; and (3) the influence of Schumann-Runge linewing contributions on the determination of the Herzberg continuum absorption cross section of (16)O2 in the wavelength region 194 to 204 nm. The experimental investigations are effected at high resolution with a 6.65 m scanning spectrometer which is, by virtue of its small instrumental width (EWHM = 0.0013 nm), uniquely suitable for cross section measurements of molecular bands with discrete rotational structure. Absolute cross sections, which are independent of the instrumental function and from which band oscillator strengths are directly determined, are measured for the absorption bands that are most predissociated. Such measurements are needed for (1) accurate calculations of the stratospheric production of atomic oxygen and heavy ozone formed following the photopredissociation of (18)O(16)O by solar radiation penetrating between the absorption lines of (16)O2; (2) elucidation of the mechanism of predissociation of the upper state of the Schumann-Runge bands; and (3) determination of the true shape of the Herzberg continuum cross section.

Parkinson, W. H.↗

DOE OSTI2023

Field-tuned quantum renormalization of spin dynamics in the honeycomb lattice Heisenberg antiferromagnet YbCl 3

The basis for our understanding of quantum magnetism has been the study of elegantly simple model systems. However, even for the antiferromagnetic honeycomb lattice with isotropic spin interactions–one of the simplest model systems–a detailed understanding of quantum effects is still lacking. Here, using inelastic neutron scattering measurements of the honeycomb lattice material YbCl 3 , we elucidate how quantum effects renormalize the single-magnon and multimagnon excitations and how this renormalization can be tuned and ultimately driven to the classical limit by applying a magnetic field. Additionally, our work reveals that the quantum effects tuned by the magnetic field not only renormalize the magnetic excitations but also induce a distinctive sharp feature inside the multimagnon continuum. From a more general perspective, this result demonstrates that structures within magnetic continua can occur over a wide experimental parameter space and can be used as a reliable means of identifying quantum phenomena.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Elucidating the photodissociation fingerprint and quantifying the determination of organic hydroperoxides in gas-phase autoxidation

Hydroperoxides are formed in the atmospheric oxidation of volatile organic compounds, in the combustion autoxidation of fuel, in the cold environment of the interstellar medium, and also in some catalytic reactions. They play crucial roles in the formation and aging of secondary organic aerosols and in fuel autoignition. However, the concentration of organic hydroperoxides is seldom measured, and typical estimates have large uncertainties. In this work, we developed a mild and environmental-friendly method for the synthesis of alkyl hydroperoxides (ROOH) with various structures, and we systematically measured the absolute photoionization cross-sections (PICSs) of the ROOHs using synchrotron vacuum ultraviolet-photoionization mass spectrometry (SVUV-PIMS). A chemical titration method was combined with an SVUV-PIMS measurement to obtain the PICS of 4-hydroperoxy-2-pentanone, a typical molecule for combustion and atmospheric autoxidation ketohydroperoxides (KHPs). We found that organic hydroperoxide cations are largely dissociated by loss of OOH. This fingerprint was used for the identification and accurate quantification of the organic peroxides, and it can therefore be used to improve models for autoxidation chemistry. The synthesis method and photoionization dataset for organic hydroperoxides are useful for studying the chemistry of hydroperoxides and the reaction kinetics of the hydroperoxy radicals and for developing and evaluating kinetic models for the atmospheric autoxidation and combustion autoxidation of the organic compounds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Influence of liquid conductance on the temporal evolution of self-organization patterns in atmospheric pressure DC glow discharges

Abstract Self-Organized Patterns (SOPs) at plasma-liquid interface in atmospheric pressure plasma discharges refer to the formation of intricate and puzzling structures due to the interplay of electrodynamic and hydrodynamic processes. Studies conducted to date have shown that this phenomenon results in the formation of distinctive patterns such as circular ring, star, gear, dots, spikes, etc., and primarily depends on working gas, electrolyte type, gap distance, current, conductivity, etc. However, an adequate understanding of how these patterns change from one type to another is still not available. This study aims to elucidate the influence of initial liquid conductance ( σ i ) on the temporal evolution of SOPs in liquid-anode discharges. The discharge was generated in a pin-to-liquid anode configuration at a constant helium (He) flow rate of 500 sccm and DC applied voltage of 6 kV at a gap distance of 12 mm. Through the gradual increment of σ i from 1.8 μ S to 4820 μ S, we observe that the trend in the evolution of SOPS takes place as solid discs, spikes, dots, rings, double rings, and stars. The continuous formation of reactive species onto the liquid anode in all conductive solutions results in a decrease in pH, an increase in bulk liquid temperature, and an increase in total dissolved solutes, and these have been confirmed through experimental measurements. Observations using optical emission spectroscopy show that the electrons at the plasma-liquid interface participate in the reduction of cations followed by their excitation & ionization due to which electron density as well as emissions from excited species (mainly hydroxyl radicals & excited nitrogen) decrease with time. Our investigation provides experimental evidence on the presence of cations at the plasma-liquid interface required for SOP formation.

Physics↗

DOE OSTI2025

Decoherence and Brownian motion of a polarizable particle near a medium

Optically levitated nanoparticles are ideal experimental testbeds for investigating macroscopic superpositions and microscopic thermodynamics. Integrating such levitated nanoparticles with photonic structures can enable strong coupling between their center-of-mass motion and guided photonic modes, facilitating enhanced control and probing of their motion. When coupling a particle to a photonic structure, such as a waveguide, the effects of fluctuations become prominent at nanoscales. In this work, we analyze the classical and quantized center-of-mass motion of a polarizable particle interacting with the fluctuations of the electromagnetic field in the presence of a medium. We derive a position localization master equation for the particle's quantized center of mass, and examine its classical center-of-mass momentum diffusion, elucidating correspondences between classical and quantum Brownian motion of polarizable particles near media. We study the decoherence rate of the particle in the presence of a planar surface as a function of temperature and distance from the surface, comparing it to common sources of decoherence. Our results are pertinent to experiments aimed at preparing levitated nanospheres in macroscopic quantum states and investigating their Brownian dynamics.

Brownian motion↗

DOE OSTI2023

Recursive Use of the Short-Time Fast Fourier Transform for Signature Analysis in Continuous Processes

Although a nuclear reactor is a hostile environment for sensing and electrical communications, the reactor core is amenable to acoustic communication. An acoustic measurement infrastructure (AMI) has been installed in the Advanced Test Reactor (ATR) to record acoustic signals that can capture its different operating regimes. AMI uses coolant pumps as continuous signal sources, coolant and structural components as transmission lines, and accelerometers to capture system motion. A recursive signal processing technique based on the short-time fast Fourier transform (STFFT) for continuous processes provides unique signatures for diagnostic and prognostic analyses from the system motion data. Here this article presents a recursive STFFT methodology that processes acoustic signals from continuous industrial processes. The article first discusses the initial STFFT use with simulated data to elucidate the basic principles necessary to understand and interpret the STFFT results from actual pump vibration data. Each repetitive use of the STFFT on pump vibration data using the results from the prior STFFT processing will generate additional complimentary time-frequency-based signatures. These signatures are generated by the coolant pumps operating under different process conditions. After each use of the STFFT, the resulting signatures provide exemplary examples of the diversity and intuitive nature of recursively using the STFFT. This article focuses on recursively using the STFFT to provide numerous complimentary and diverse signatures that will ultimately be inputs for machine learning algorithms that provide predictive data analytics. The intuitive nature of the information and signatures from recursive STFFT processing will also bring intuitive interpretation capabilities to machine learning and predictive data analytic techniques.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2024

Data-Efficient Dimensionality Reduction and Surrogate Modeling of High-Dimensional Stress Fields

Tensor datatypes representing field variables like stress, displacement, velocity, etc., have increasingly become a common occurrence in data-driven modeling and analysis of simulations. Numerous methods [such as convolutional neural networks (CNNs)] exist to address the meta-modeling of field data from simulations. As the complexity of the simulation increases, so does the cost of acquisition, leading to limited data scenarios. Modeling of tensor datatypes under limited data scenarios remains a hindrance for engineering applications. Here, in this article, we introduce a direct image-to-image modeling framework of convolutional autoencoders enhanced by information bottleneck loss function to tackle the tensor data types with limited data. The information bottleneck method penalizes the nuisance information in the latent space while maximizing relevant information making it robust for limited data scenarios. The entire neural network framework is further combined with robust hyperparameter optimization. We perform numerical studies to compare the predictive performance of the proposed method with a dimensionality reduction-based surrogate modeling framework on a representative linear elastic ellipsoidal void problem with uniaxial loading. The data structure focuses on the low-data regime (fewer than 100 data points) and includes the parameterized geometry of the ellipsoidal void as the input and the predicted stress field as the output. The results of the numerical studies show that the information bottleneck approach yields improved overall accuracy and more precise prediction of the extremes of the stress field. Additionally, an in-depth analysis is carried out to elucidate the information compression behavior of the proposed framework.

artificial intelligence↗

DOE OSTI2026

Juvenile Salmon and Their Habitats in the Columbia River Estuary: A Review and Synthesis of Knowledge Development 2000–2025

[This is a 90% discussion draft.] This is the third Synthesis Memorandum funded by the U.S. Army Corps of Engineers and developed for the Columbia Estuary Ecosystem Restoration Program (CEERP) on the topic of habitat restoration in the Columbia River Estuary (CRE) from Bonneville Dam to the river mouth. While the first two were developed by PNNL and NOAA without the benefit of stakeholder participation, for the current memo, two key activities were initiated: (1) review, by the Expert Regional Technical Group (ERTG), of status and trends monitoring and action effectiveness monitoring funded by CEERP, and (2) a workshop including representatives of the Bonneville Power Administration and the U.S. Army Corps of Engineers (the action agencies [AAs]), the National Oceanic and Atmospheric Administration (NOAA), major research agencies contributing to CEERP, and sponsors who implement CEERP restoration actions. A systematic literature review was conducted using ClarivateTM Web of ScienceTM database. The topics of interest for CRE relevant research included salmon ecology, physical processes, and wetland habitats, and therefore required the use of broad search terms. Our final search criteria included a combination of Boolean operators and an approach to combine different sets of search terms. The final search result yielded 669 records. The records were classified by groups and assigned to the relevant disciplinary expert for review. The review identified substantive advances in understanding the provision of salmon habitat functions through spatiotemporally dynamic physical and ecological processes, and the use of CRE habitats by numerous stocks of juvenile salmon. It also uncovered heretofore unincorporated historical documentation of riparian habitats across the CRE. The characterization of the structural components of floodplain habitat including plant associations and channel networks has advanced considerably, together with the understanding of seasonal changes and long-term trends. The relative influence of salmon-habitat location in the CRE as compared with temporal factors, mainly season, has been well described, which affects the prioritization of restoration. Stressors on the ecosystem and fish, and the drivers of these stressors, have been more carefully elucidated and predictive models are in various stages of development. The vision, aims, and design of restoration projects have advanced together with methods of data collection, analysis, and modeling that have seen substantial improvements. Experiments intended to inform the design of restoration projects are underway or have been completed. An important outstanding area of research that has lagged behind the advances in fundamental understanding of the ecosystem and salmon habitat functions remains the peer-reviewed documentation of the outcomes of restoration for both habitats and fish functions.

estuary↗

DOE OSTI2024

Comparative study of machine learning techniques for post-combustion carbon capture systems

Computational analysis of countercurrent flows in packed absorption columns, often used in solvent-based post-combustion carbon capture systems (CCSs), is challenging. Typically, computational fluid dynamics (CFD) approaches are used to simulate the interactions between a solvent, gas, and column's packing geometry while accounting for the thermodynamics, kinetics, heat, and mass transfer effects of the absorption process. These simulations can then be used explain a column's hydrodynamic characteristics and evaluate its CO 2 -capture efficiency. However, these approaches are computationally expensive, making it difficult to evaluate numerous designs and operating conditions to improve efficiency at industrial scales. In this work, we comprehensively explore the application of statistical ML methods, convolutional neural networks (CNNs), and graph neural networks (GNNs) to aid and accelerate the scale-up and design optimization of solvent-based post-combustion CCSs. We apply these methods to CFD datasets of countercurrent flows in absorption columns with structured packings characterized by several geometric parameters. We train models to use these parameters, inlet velocity conditions, and other model-specific representations of the column to estimate key determinants of CO 2 -capture efficiency without having to simulate additional CFD datasets. We also evaluate the impact of different input types on the accuracy and generalizability of each model. We discuss the strengths and limitations of each approach to further elucidate the role of CNNs, GNNs, and other machine learning approaches for CO 2 -capture property prediction and design optimization.

97 MATHEMATICS AND COMPUTING↗

NASA NTRS1993

A coupled subsurface-boundary layer model of water on Mars

A 1D numerical model of the exchange of H2O between the atmosphere and subsurface of Mars through the PBL is employed to explore the mechanisms of H2O exchange and to elucidate the role played by the regolith in the local H2O budget. The atmospheric model includes effects of Coriolis, pressure gradient, and frictional forces for momentum: radiation, sensible heat flux, and advection for heat. It is suggested that in most cases, the flux through the Martian surface reverses twice in the course of each sol. The effects of surface albedo, thermal inertia, solar declination, atmospheric optical depth, and regolith pore structure are explored. It is proposed that higher thermal inertia forces more H2O into the atmosphere because the regolith is warmer at depth.

Zent, Aaron P.↗

NASA NTRS1999

Buffer Effects in the Solubility, Nucleation and Growth of Chicken Egg White Lysozyme

The growth of protein crystals is important for determination of their three-dimensional structure, which relates to their biochemical functions and to the practical goal of designing pharmaceuticals to modify that function. While many proteins have been successfully crystallized by a variety of methods, there is still limited understanding of the process of nucleation and growth of even the simplest proteins. Chicken egg-white lysozyme (CEWL) is readily crystallized under a variety of conditions, and studies underway at MSFC are designed to elucidate the mechanisms by which the crystals nucleate and grow. We have investigated the effect of buffer choice on the solubility, nucleation and growth of CEWL. CEWL was purified by dialysis against a .05M phosphate buffer and chromatographic separation from contaminants in a sepharose column. Solubility studies were made as a function of buffer concentration for phosphate and formate buffers, and the nucleation and growth of crystals at 10 C was studied as a function of pH for oxalate, succinate, formate, butyrate, carbonate, phosphate and acetate buffer solutions. The solubility data support the conclusion that there is a solubility minimum as a function of buffer concentration for amphiphilic molecules, while no minimum is observed for a phosphate buffer. Nucleation is suppressed at pH greater than pKa for all buffers except phosphate. The aspect ratio of the (110) faces is shown to be a function of crystal size, rather than pH.

Gibson, Ursula J.↗