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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 379 records · Page 21
All sourcesNASA NTRSDOE OSTI
NASA NTRS1984

Space shuttle experiments on Al-In liquid phase miscibility gap (LPMG) alloys

Massive phase separation observed at low-g was studied during the phase separation process while cooling through the miscibility gap under a controlled thermal gradient was investigated. The molten drops which form during the phase separation process appear to move in a direction opposite to that predicted by the theory of thermocapillary droplet motion. A second experiment utilized a plunger arrangement designed to eliminate the surface tension driven convection currents originating at a free surface. This experiment suggests that the free surface does contribute to the coalescence process but that there are other mechanisms which are more important.

Gelles, S. H.↗
DOE OSTI2023

Magnetoresistance anomaly during the electrical triggering of a metal-insulator transition

Phase separation naturally occurs in a variety of magnetic materials and it often has a major impact on both electric and magnetotransport properties. In resistive switching systems, phase separation can be created on demand by inducing local switching, which provides an opportunity to tune the electronic and magnetic state of the device by applying voltage. Here we explore the magnetotransport properties in the ferromagnetic oxide La 0.7 ⁢Sr 0.3 ⁢MnO 3 (LSMO) during the electrical triggering of an intrinsic metal-insulator transition (MIT), which produces volatile resistive switching. This switching occurs in a characteristic spatial pattern, i.e., the formation of a high-resistance barrier perpendicular to the current flow, enabling an electrically actuated ferromagnetic-paramagnetic-ferromagnetic phase separation. At the threshold voltage of the MIT triggering, both anisotropic and colossal magnetoresistances exhibit anomalies including a large increase in magnitude and a sign flip. Computational analysis revealed that these anomalies originate from the coupling between the switching-induced phase separation state and the intrinsic magnetoresistance of LSMO. Furthermore, this work demonstrates that driving the MIT material into an out-of-equilibrium resistive switching state provides the means for electrical control of the magnetotransport phenomena.

Complex oxides↗
DOE OSTI2022

Pattern formation and flocking for particles near the jamming transition on resource gradient substrates

Here, we numerically examine a bidisperse system of active and passive particles coupled to a resource substrate. The active particles deplete the resource at a fixed rate and move toward regions with higher resources, while all of the particles interact sterically with each other. We show that at high densities, this system exhibits a rich variety of pattern-forming phases along with directed motion or flocking as a function of the relative rates of resource absorption and consumption as well as the active to passive particle ratio. These include partial phase separation into rivers of active particles flowing through passive clusters, strongly phase separated states where the active particles induce crystallization of the passive particles, mixed jammed states, and fluctuating mixed fluid phases. For higher resource recovery rates, we demonstrate that the active particles can undergo motility-induced phase separation, while at high densities, there can be a coherent flock containing only active particles or a solid mixture of active and passive particles. The directed flocking motion typically shows a transient in which the flow switches among different directions before settling into one direction, and there is a critical density below which flocking does not occur. We map out the different phases as function of system density, resource absorption and recovery rates, and the ratio of active to passive particles.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2026

ALS mutations disrupt self-association between the ubiquilin STI1 hydrophobic groove and internal placeholder sequences

Ubiquilins are molecular chaperones that play multifaceted roles in proteostasis, with point mutations in UBQLN2 leading to altered phase-separation properties and amyotrophic lateral sclerosis (ALS). Our mechanistic understanding of this essential process has been hindered by a lack of structural information on the STI1 domain, which is essential for ubiquilin chaperone activity and phase separation. Here, we present the first crystal structure of a ubiquilin-family STI1 domain bound to a transmembrane domain (TMD), and show that ALS mutations disrupt the STI1-TMD interaction. We further demonstrate that ubiquilins contain multiple conserved internal sequences that bind to the STI1 domain, including the PXX-repeat region that is a hotspot for ALS mutations. We propose that these placeholder sequences prevent solvent exposure of the STI1 hydrophobic groove and contribute to the multivalency that drives ubiquilin phase-separation. Together, this work provides a new paradigm for understanding how STI1 domains modulate ubiquilin chaperone activity and phase separation, and offers insights into the molecular basis of ALS pathogenesis.

Onwunma, Joan [Univ. of Toledo, OH (United States)↗
DOE OSTI2018

Ionic Tuning of Cobaltites at the Nanoscale

Control of materials through custom design of ionic distributions is one of the most promising approaches for developing future technologies ranging from spintronic logic and memory devices to energy storage. Perovskites have shown particular promise for ionic-devices due to their high ion mobility and sensitivity to chemical stoichiometry. In this work, we demonstrate control of ion distributions in (La,Sr)CoO3. Commensurate with control of the oxygen stoichiometry, the Co valence and saturation magnetization show a smooth continuous variation. In contrast, magnetoresistance measurements show a sharp, step-wise transition in the magnetic anisotropy and resistivity over the same range of oxygen stoichiometry. These results suggest significant phase separation, with conductive magnetic regions and oxygen-deficient, insulating, non-magnetic regions, forming percolated networks. Indeed, X-ray diffraction identifies oxygen vacancy ordering, including the emergence of Brownmillerite ordering. The unusual appearance of the Brownmillerite phase under ambient temperature is further confirmed by high resolution scanning transmission electron microscopy. This work demonstrates room-temperature ionic control of magnetism, electrical conductivity and crystalline structure, in a 40 nm film, presenting new opportunities for ionic devices that leverage multiple material properties.

thin films, magnetism, xmcd, pnr, STEM, defects↗
DOE OSTI2024

Resonant Soft X-ray Scattering Reveals Hierarchical Structure in a Multicomponent Vapor-Deposited Glass

Multiphase vapor-deposited glasses are an important class of materials for organic electronics, particularly organic photovoltaics and thermoelectrics. These blends are frequently regarded as molecular alloys and there have been few studies of their structure at nanometer scales. Here, in this work, we show that a codeposited system of TPD (N,N'-bis(3-methylphenyl)-N,N'-diphenylbenzidine) and DO37 (disperse orange 37), two small molecule glass-formers, separates into amorphous, compositionally distinct phases with a domain size and spacing ca. 10s of nanometers that depends on substrate temperature during deposition. Domains rich in one of the two components become larger and more pure at higher deposition temperatures. We use resonant soft X-ray scattering (RSoXS) complemented with atomic force microscopy (AFM) and photoinduced force microscopy to measure the phase separation, topography, and purity of the deposited films. A forward-simulation approach to RSoXS analysis, the National Institute of Standards and Technology RSoXS Simulation Suite (NIST RSoXS simulation suite), is used with models developed from AFM images to evaluate the energy dependence of scattering across multiple length scales and interpret the RSoXS with respect to structure within the films. We find that the RSoXS is sensitive to a length scale of phase separation buried within the film that is consistent with the surface composition profile, and correlates to the topography to an extent that depends on substrate temperature. We demonstrate that vacuum scattering, which is often ignored in RSoXS analysis, contributes significantly to the features and energy dependence of the RSoXS pattern, and then illustrate how to properly account for vacuum scattering to analyze films with significant roughness. We then use this analysis framework to understand structure development mechanisms that occur during vapor deposition of a TPD-DO37 codeposited glass with results that outline paths to tune morphology in multicomponent materials.

36 MATERIALS SCIENCE↗
NASA NTRS2023

Regenerable Liquid Desiccants for High Efficiency Humidity Control in Microgravity

The NASA X-Hab project aims to design, manufacture, test, and prove functionality of an air humidity control subsystem to dehumidify and re-humidify air from a space cabin. The method of regulating cabin air humidity utilizes vortex phase separation, which uses an ionic liquid (IL) desiccant for air-water phase separation. This subsystem is intended to be integrated with a CO 2 removal system requiring de-humidified air to operate efficiently. The air humidity control subsystem is composed of a cold-desiccant or cold-side Vortex Phase Separator (VPS) that dehumidifies the cabin air. The dehumidified air exits the cold-side (CS) VPS chamber to flow into the CO 2 removal module, and the cold, water-laden liquid desiccant flows to a regenerative heat exchanger. From the heat exchanger the liquid desiccant continues to the heater. After heating, the desiccant flows into a hot-desiccant or hot-side (HS) VPS as the dehumidified air from CO 2 removal module enters through the HS VPS air inlet. The rehumidified air exits the HS VPS into the space cabin. One pump installed at the liquid exit of the CS VPS and one pump installed at the liquid exit of the HS VPS transport the fluid through the system. To evaluate the system’s efficiency and effectiveness, the temperature, pressure, flow rate and relative humidity are read, recorded, and analyzed at critical points along the module.

Gerardo Castro↗
DOE OSTI2023

Low complexity domains of the nucleocapsid protein of SARS-CoV-2 form amyloid fibrils

The self-assembly of the Nucleocapsid protein (NCAP) of SARS-CoV-2 is crucial for its function. Computational analysis of the amino acid sequence of NCAP reveals low-complexity domains (LCDs) akin to LCDs in other proteins known to self-assemble as phase separation droplets and amyloid fibrils. Previous reports have described NCAP’s propensity to phase-separate. Here we show that the central LCD of NCAP is capable of both, phase separation and amyloid formation. Within this central LCD we identified three adhesive segments and determined the atomic structure of the fibrils formed by each. Those structures guided the design of G12, a peptide that interferes with the self-assembly of NCAP and demonstrates antiviral activity in SARS-CoV-2 infected cells. Our work, therefore, demonstrates the amyloid form of the central LCD of NCAP and suggests that amyloidogenic segments of NCAP could be targeted for drug development.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2019

Photochemical Aging Alters Secondary Organic Aerosol Partitioning Behavior

Organic aerosol is the largest fraction of the atmospheric non-refractory aerosol mass and has a significant impact on climate, visibility, and human health. A significant portion of organic aerosol is secondary organic aerosol (SOA), which forms when volatile organic compounds (VOCs) are oxidized and the reaction products partition to the particle phase. SOA formation and aging have been described using semi-volatile partitioning theory, and a typical assumption invoked is that gas-particle partitioning rapidly reaches equilibrium. However, several studies have called into question whether traditional equilibrium assumptions are valid, either due to particle-phase diffusion limitations, particle-phase reactions, or liquid/liquid phase separation and immiscibility of organic phases. Here, we investigate the ability of partitioning theory to describe laboratory SOA formation experiments using SOA mass and yield as the evaluation metric. We conduct two types of experiments; co-condensation experiments in which isoprene and a-pinene are simultaneously oxidized to form SOA, and sequential condensation experiments in which fresh isoprene SOA is exposed to aged, pre-existing isoprene- or a-pinene-derived SOA particles. In the co-condensation experiments, partitioning theory successfully predicted the time-dependent SOA concentrations without invoking diffusion limitations or organic phase separation. However, in the sequential condensation experiments, yield analysis showed that fresh isoprene SOA did not partition into either the aged a-pinene or aged isoprene SOA particles over the 4 hour experimental timescale, even at relative humidity as high as 85%. This study shows that common assumptions regarding SOA gas-particle partitioning are accurate for fresh SOA, but that these assumptions break down after SOA has been photochemically aged for modest amounts of time (~1 day). These results have important consequences for modeling SOA formation and may help to resolve some seemingly divergent conclusions regarding diffusion limitations that exist in the literature.

Secondary Organic Aerosol (SOA), gas/particle part↗
DOE OSTI2017

Velocity force curves, laning, and jamming for oppositely driven disk systems

Using simulations we examine here a two-dimensional disk system in which two disk species are driven in opposite directions. We measure the average velocity of one of the species versus the applied driving force and identify four phases as function of drive and disk density: a jammed state, a completely phase separated state, a continuously mixing phase, and a laning phase. The transitions between these phases are correlated with jumps in the velocity–force curves that are similar to the behavior observed at dynamical phase transitions in driven particle systems with quenched disorder such as vortices in type-II superconductors. In some cases the transitions between phases are associated with negative differential mobility in which the average absolute velocity of either species decreases with increasing drive. We also consider the situation where the drive is applied to only one species as well as systems in which both species are driven in the same direction with different drive amplitudes. We show that the phases are robust against the addition of thermal fluctuations. Finally, we discuss how the transitions we observe could be related to absorbing phase transitions where a system in a phase separated or laning regime organizes to a state in which contacts between the disks no longer occur and dynamical fluctuations are lost.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Thermodynamic origin of nonvolatility in resistive memory

Electronic switches based on the migration of high-density point defects, or memristors, are poised to revolutionize post-digital electronics. Despite significant research, key mechanisms for filament formation and oxygen transport remain unresolved, hindering our ability to predict and design device properties. For example, experiments have achieved 10 orders of magnitude longer retention times than predicted by current models. Here, using electrical measurements, scanning probe microscopy, and first-principles calculations on tantalum oxide memristors, we reveal that the formation and stability of conductive filaments crucially depend on the thermodynamic stability of the amorphous oxygen-rich and oxygen-poor compounds, which undergo composition phase separation. Including the previously neglected effects of this amorphous phase separation reconciles unexplained discrepancies in retention and enables predictive design of key performance indicators such as retention stability. Furthermore, this result emphasizes non-ideal thermodynamic interactions as key design criteria in post-digital devices with defect densities substantially exceeding those of today’s covalent semiconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2026

A structural and electrochemical study of perfluoropolyether-poly(ethylene oxide) solid polymer electrolytes

Solid polymer electrolytes offer attractive safety, processability, and interfacial adhesion for enabling high–energy solid-state lithium batteries, but they are often limited by narrow oxidative stability windows and low lithium-ion transference numbers. In an attempt to broaden the electrochemical stability window and increase lithium-ion transference number of poly(ethylene oxide) (PEO)-based solid polymer electrolytes, we produce an optically clear, crosslinked membrane of PEO and perfluoropolyether (PFPE) using a mixed solvent method and subsequently infuse the membrane with a lithium salt. Structural and thermal analyses reveal nanoscale phase separation between fluorocarbon and hydrocarbon domains with characteristic spacings of 7–8 nm and an elevated glass transition for the hydrocarbon phase. Consistent with this, PFPE-containing membranes exhibit substantially lower ionic conductivity than PEO analogs (dry and plasticized). The transference number and electrochemical stability are similar to pure PEO. These results demonstrate that fluorination implemented as segregated nanoscale domains does not deliver the anticipated transport or stability benefits; instead, phase separation increases tortuosity and suppresses hydrocarbon-phase dynamics. The work underscores the importance of fluorine placement and morphology control, guiding the design of partially fluorinated solid polymer electrolytes toward architectures that avoid detrimental nanoscale phase separation.

Carden, Peyton [ORNL] (ORCID:0000000162296538)↗
DOE OSTI2024

Effect of Molecular Conformation on Intermolecular Interactions and Photovoltaic Performances of Giant Molecule Acceptors

The molecular conformation of giant molecule acceptors (GMAs) plays a significant role in regulating the intermolecular interactions and their photovoltaic performances in organic solar cells (OSCs). For the linear GMA GT‐l, the stronger homo‐molecular interaction causes its aggregation being weakly affected by the donor, thus forming an ordered molecular stacking and proper phase separation in its blend film. The star‐shaped GMA GT‐s‐based blend film shows a dominant hetero‐molecular interaction that suppresses the aggregation of the donor and acceptor, resulting in smaller phase separation and more uniform vertical phase distribution. While for another star‐shaped GMA GTs, the weakest hetero‐molecular interaction causes its blend film to form larger phase separation. Therefore, the GT‐l based OSC with PM6 as donor shows the highest charge mobilities, the fastest charge transfer (CT) process, reduced energy loss and less charge recombination, contributing to a higher power conversion efficiency (PCE) of 19.03%. Comparatively, the PCEs of the OSCs based on GTs and GT‐s are 18.05% and 17.58% respectively. Notably, all the three GMAs based OSCs show excellent thermal stability and long‐term storage stability. This study provides a facile strategy by tuning the linking unit and its connecting mode for designing highly efficient and stable organic photovoltaic materials.

Chemistry↗
DOE OSTI2019

Reversibility, pattern formation, and edge transport in active chiral and passive disk mixtures

In this study, we numerically examine mixtures of circularly moving and passive disks as a function of density and active orbit radius. For low or intermediate densities and/or small orbit radii, the system can organize into a reversible partially phase separated labyrinth state in which there are no collisions between disks, with the degree of phase separation increasing as the orbit radius increases. As a function of orbit radius, we find a divergence in the number of cycles required to reach a collision-free steady state at a critical radius, while above this radius, the system remains in a fluctuating liquid state. For high densities, the system can organize into a fully phase separated state that is mostly reversible, but collisions at the boundaries between the phases lead to a net transport of disks along the boundary edges in a direction determined by the chirality of the active disk orbits. We map the dynamic phases as a function of density and orbit radii and discuss the results in terms of the reversible-irreversible transition found in other periodically driven non-thermal systems. Finally, we also consider mixtures of circularly driven disks and ac driven disks where the ac drive is either in or out of phase with the circular motion and find a rich variety of pattern forming and reentrant disordered phases.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

A review of recent research on nonequilibrium solid solution behavior in Li X FePO 4 [A review of nonequilibrium solid solution in Li X FePO 4 ]

Li X FePO 4 (0 < X < 1) is one of the most well-studied cathode battery materials and is notable for its large miscibility gap. Although its phase-separating behaviors under equilibrium conditions have been well documented, recent research has shown that phase separation is suppressed at elevated rates of lithium insertion and removal. Specifically, Li X FePO 4 exhibits a nonequilibrium solid solution behavior at elevated cycling rates. This article reviews recent research on nonequilibrium solid solution in Li X FePO 4 ; these insights have been largely enabled by operando characterization techniques. As a result, such studies have not only unambiguously confirmed the existence of this solid solution, but also show how surface reaction and diffusion kinetics ultimately affect phase separation and other spatially nonuniform lithiation and delithiation behavior.

36 MATERIALS SCIENCE↗
NASA NTRS1999

Identification of Gravity-Related Effects on Crystal Growth From Melts With an Immiscibility Gap

This work involves an experimental-numerical approach to study the effects of natural and Marangoni convections on solidification of single crystals from a silicate melt with a liquid-liquid immiscibility gap. Industrial use of crystals grown from silicate melts is becoming increasingly important in electronic, optical, and high temperature structural applications. Even the simplest silicate systems like Al203-SiO2 have had, and will continue to have, a significant role in the development of traditional and advanced ceramics. A unique feature of crystals grown from the silicate systems is their outstanding linear electro-optic properties. They also exhibit exceptionally high optical rotativity. As a result, these crystals are attractive materials for dielectric, optical, and microwave applications. Experimental work in our laboratory has indicated that directional solidification of a single crystal mullite appears to be preceded by liquid-liquid phase separation in the melt. Disruption of the immiscible state results in crystallization of a two phase structure. There is also evidence that mixing in the melt caused by density-driven convection can significantly affect the stability of the immiscible liquid layers and result in poly-crystalline growth. On earth, the immiscible state has only been observed for small diameter crystals grown in float zone systems where natural convection is almost negligible. Therefore, it is anticipated that growth of large single crystals from silicate melts would benefit from microgravity conditions because of the reduction of the natural convective mixing. The main objective of this research is to determine the effects of transport processes on the phase separation in the melt during growth of a single crystal while addressing the following issues: (1) When do the immiscible layers form and are they real?; (2) What are the main physical characteristics of the immiscible liquids?; and (3) How mixing by natural or Marangoni convection affects the stability of the phase separated melt.

Kassemi, M.↗
DOE OSTI2025

Correction to “COCOMO2: A Coarse-Grained Model for Interacting Folded and Disordered Proteins”

Biomolecular interactions are essential in many biological processes, including complex formation and phase separation processes. Coarse-grained computational models are especially valuable for studying such processes via simulation. Here, we present COCOMO2, an updated residue-based coarse-grained model that extends its applicability from intrinsically disordered peptides to folded proteins. This is accomplished with the introduction of a surface exposure scaling factor, which adjusts interaction strengths based on solvent accessibility, to enable the more realistic modeling of interactions involving folded domains without additional computational costs. COCOMO2 was parametrized directly with solubility and phase separation data to improve its performance on predicting concentration-dependent phase separation for a broader range of biomolecular systems compared to the original version. COCOMO2 enables new applications including the study of condensates that involve IDPs together with folded domains and the study of complex assembly processes. COCOMO2 also provides an expanded foundation for the development of multiscale approaches for modeling biomolecular interactions that span from residue-level to atomistic resolution.

Molecular interactions↗