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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 829 records · Page 46
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Electronic Structure and Phase Stability of Yb-filled CoSb 3 Skutterudite Thermoelectrics from First Principles

Filling the large voids in the crystal structure of the skutterudite CoSb$_3$ with rattler atoms $R$ provides an avenue for both increasing carrier concentration and disrupting lattice heat transport, leading to impressive thermoelectric performance. While the influence of $R$ on the lattice dynamics of skutterudite materials has been well studied, the phase stability of $R$-filled skutterudite materials and the influence of the presence and ordering of $R$ on the electronic structure remain unclear. Here, focusing on the Yb-filled skutterudite Yb$_x$Co$_4$Sb$_{12}$, we employ first-principles methods to compute the phase stability and electronic structure. Yb-filled CoSb$_3$ exhibits (1) a mild tendency for phase separation into Yb-rich and Yb-poor regions and (2) a strong tendency for chemical decomposition into Co--Sb and Yb--Sb binaries (i.e., CoSb$_3$, CoSb$_2$, and YbSb$_2$). We find that, at reasonable synthesis temperatures, configurational entropy stabilizes single-phase solid solutions with limited Yb solubility, in agreement with experiments. Filling CoSb$_3$ with Yb increases the band gap, enhances the carrier effective masses, and generates new low-energy ``emergent'' conduction band minima, which is distinct from the traditional band convergence picture of aligning the energies of existing band extrema. The explicit presence of $R$ is necessary to achieve the emergent conduction band minima, though the rattler ordering does not strongly influence the electronic structure. The emergent conduction bands are spatially localized in the Yb-rich regions, unlike the delocalized electronic states at the Brillouin zone center that form the unfilled skutterudite band edges.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Multifunctional electrochemical memory stabilized by phase coexistence

Our growing computing needs, especially in applications that heavily rely on artificial intelligence (AI), motivate a search for new components that could substantially augment the performance of general-purpose digital computers. Beyond ON/OFF switching, new components with linear multistate analog resistive tuning, nonlinear volatile switching, spiking, oscillatory, stochastic and other complex functionalities could enable highly efficient neuromorphic computing schemes for AI information processing. Compared to the extreme multifunctionality of biological neurons, realizing all the above characteristics in a single, scalable analog component remains a grand challenge. Here we investigate electrochemical gating combined with localized thermal activation to program and switch a single, vertically integrated and dimensionally scaled electrothermal chemical random access memory (ETCRAM) with a channel and reservoir composed of phase-separated vanadium oxide. Closely related to electrochemical RAM (ECRAM), ETCRAM uses an integrated gate-heater electrode to overcome kinetic barriers that help retain states at ambient temperatures. In addition to synapse-like stable and programmable analog resistance states arising from redox-tunable phase coexistence, a single component exhibits neuron-like nonlinear conductance switching with a tunable threshold and self-driven dynamics owing to the thermally driven metal-insulator phase transition in vanadium dioxide. More broadly, we demonstrate that electrochemically stabilized phase coexistence could unlock analog electronics with novel functionality, stability, reconfigurability, and scalability.

Oh, Sangheon [Sandia National Lab. (SNL-CA), Liver↗
NASA NTRS1990

The liquid/vapor boundary in a porous plug

Results are presented from measurements of pressure and temperature differences as a function of the flow rate and hydrostatic head for two types of porous plugs for phase separation of superfluid He and He vapor: (1) a plug made of sintered stainless steel, similar to that in the IRAS, IRT, and COBE dewars except for larger pores, and (2) a glass plug with pores of uniform cross section. Results show that a liquid/vapor phase boundary exists at the outer surface of the porous plug for low flows or large hydrostatic heads; as the flow increases or the hydrostatic head decreases, the boundary retreats into the plug. Some hysteresis near the phase boundary retreat was observed in the stainless steel plug.

Dipirro, M. J.↗
NASA NTRSDate not supplied

Lessons Learned on Mega-Constellation Deployments and Impact to Space Domain Awareness

The breakneck expansion of multi-payload launches in low Earth orbit (LEO) has seen significant escalation over the last three years in the Space Domain Awareness (SDA) enterprise. The uptick in satellite deployment frequency, gradation of Mega-constellation deployments utilizing electric propulsion, and surge in metric observation density from the Space Surveillance Network (SSN) have imposed major system enhancements to ensure spaceflight safety. Beginning with the launch phase, new tactics, software, and procedures have been developed over the last few years to optimize the tasking of the SSN and ensure custody of all recently launched satellites that are added to the space catalog. Ensuring appropriate tasking levels were pivotal during the satellite separation phase, which necessitated updates to the mission systems for improved delineation between clustered satellites in a short window of time. The improved incorporation of utilizing owner operator provided ephemeris coupled with critical code improvements have now revolutionized how we maintain custody of earth orbiting objects. The exponential population growth of low-Earth orbiting satellites have also increased the quantity of Conjunction Data Messages sent out to partners such as the Trajectory Operations Group (TOPO) in Johnson Space Center. We will discuss the need for continued collaboration between the National Aeronautics and Space Administration (NASA) and other Mega-Constellation Satellite Operators to safeguard Human Space Flight operations. Lastly, we will discuss the increase in reentry reporting for satellites falling back to Earth’s atmosphere, and the challenges associated with these events.

Christian C Ramos↗
NASA NTRSDate not supplied

Lessons Learned on Mega-Constellation Deployments and Impact to Space Domain Awareness

The breakneck expansion of multi-payload launches in low Earth orbit (LEO) has seen significant escalation over the last three years in the Space Domain Awareness (SDA) enterprise. The uptick in satellite deployment frequency, gradation of mega-constellation deployments utilizing electric propulsion, and surge in metric observation density from the Space Surveillance Network (SSN) have driven major system enhancements to ensure spaceflight safety. Beginning with the launch phase, new tactics, software, and procedures have been developed over the last few years to optimize the tasking of the SSN and ensure custody of all recently launched satellites that are added to the space catalog. Ensuring appropriate tasking levels were pivotal during the satellite separation phase, which necessitated updates to the mission systems for improved delineation between clustered satellites in a short window of time. The improved incorporation of utilizing satellite owner/operator-provided ephemeris coupled with critical code improvements have revolutionized how we maintain custody of Earth orbiting objects. The exponential population growth of Low-Earth orbiting satellites have also increased the quantity of Conjunction Data Messages sent out to partners such as the Trajectory Operations Group (TOPO) in Johnson Space Center. We will discuss the need for continued collaboration between the National Aeronautics and Space Administration (NASA) and other mega-constellation satellite operators to safeguard human spaceflight operations. Lastly, we will discuss how mega-constellations are driving best practices for safe operations across the space community.

Christian Ramos↗
DOE OSTI2023

Learning heterogeneous reaction kinetics from X-ray movies pixel-by-pixel

Reaction rates at spatially heterogeneous, unstable interfaces are notoriously difficult to quantify, yet are essential in engineering many chemical systems, such as batteries 1 and electrocatalysts 2. Experimental characterizations of such materials by operando microscopy produce rich image datasets 3–6, but data-driven methods to learn physics from these images are still lacking because of the complex coupling of reaction kinetics, surface chemistry and phase separation 7. Here we show that heterogeneous reaction kinetics can be learned from in situ scanning transmission X-ray microscopy (STXM) images of carbon-coated lithium iron phosphate (LFP) nanoparticles. Combining a large dataset of STXM images with a thermodynamically consistent electrochemical phase-field model, partial differential equation (PDE)-constrained optimization and uncertainty quantification, we extract the free-energy landscape and reaction kinetics and verify their consistency with theoretical models. We also simultaneously learn the spatial heterogeneity of the reaction rate, which closely matches the carbon-coating thickness profiles obtained through Auger electron microscopy (AEM). Across 180,000 image pixels, the mean discrepancy with the learned model is remarkably small (<7%) and comparable with experimental noise. Our results open the possibility of learning nonequilibrium material properties beyond the reach of traditional experimental methods and offer a new non-destructive technique for characterizing and optimizing heterogeneous reactive surfaces.

Chueh, William↗
DOE OSTI2019

In Situ Electron Microscopy Investigation of Sodiation of Titanium Disulfide Nanoflakes

Two-dimensional (2D) metal sulfides show great promises for their potential applications as electrode materials of sodium ion batteries because of the weak interlayer van der Waals interactions which allow the reversible accommodation and extraction of sodium ions. The sodiation of metal sulfides can undergo a distinct process compared to that of lithiation, which is determined by their metal and structural types. Yet, the structural and morphological evolution during its electrochemical sodiation is still unclear. In this report, we studied the sodiation reaction dynamics of TiS 2 by employing in situ transmission electron microscopy and first-principles calculations. During the sodium ion intercalation process, we observed multiple intermediate phases (phase II, phase Ib, and phase Ia), different from its lithiation counterpart, with varied sodium occupation sites and interlayer stacking sequences. Further insertion of Na ions prompted a multi-step extrusion reaction which led to the phase separation of Ti metal from the Na 2 S matrix, with its 2D morphology expanded to a 3D morphology. In contrast to regular conversion electrodes, TiS 2 still maintained a compacted structure after a full sodiation. Frist-principles calculations reveal that the as-identified phases are thermodynamically preferred at corresponding intercalation/extrusion stages compared to other possible phases. The current work provides the fundamental mechanistic understanding of the sodiation process of 2D transition metal sulfides.

25 ENERGY STORAGE↗
DOE OSTI2018

Spontaneous Separation in Trapped Fermi Gas with p-Wave Interactions: Due to the Mass-Imbalance

Based on density functional theory, the spontaneous separation in the mass-imbalanced Fermi–Fermi mixture is studied. The ground-state energy density functional is constructed with the effective contact interaction, with which the ground-state density profiles of the mixture are calculated under different conditions of mass-imbalance and coupling strength. The influence of mass-imbalance on the separation and the cloud size is analyzed. In addition, the system with both mass- and population-imbalance is also calculated and studied. Despite our rough treatment in the Thomas–Fermi approximation, it is hoped that the results may provide new clues to understand the nature of phase separation of a trapped ultracold gas in both theoretical and experimental researches in the future.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

On the importance of species immiscibility in mixing-layer dynamics at supercritical pressures

The mixing dynamics of injected propellants is a key factor in determining the ignition performance and combustion-instability response of rocket engines, internal combustion engines, and gas turbines. A key source of uncertainty in the prediction of phase-exchange dynamics is the immiscibility of the injected propellants at supercritical pressure conditions, which induces liquid/vapor phase separation and surface-tension dynamics. While experimental observations indicate the presence of liquid/vapor interfacial structures, this interfacial dynamics is typically neglected in numerical analyses. To address this issue, the objective of the present study is to systematically evaluate the importance of species immiscibility on the phase-exchange dynamics of cryogenic LOX/GH2 mixing layers at typical rocket engine injection conditions. This is accomplished by comparing simulations of (i) a recently developed interface-capturing Regularized-Interface Method (RIM) formulation, and (ii) the commonly employed Diffuse-Interface Method (DIM) formulation. Analysis shows that the interfacial dynamics significantly impact the atomization and mixing of the propellants in the near-injector region, which is not captured by the DIM formulation. The findings of this study extend to other immiscible injection systems, such as LOX/kerosene and hydrocarbon-fuel/air, thereby highlighting the importance of resolving species immiscibility in simulating high-pressure combustion engines.

diffused-interface method↗
DOE OSTI2023

Impact of phase state and non-ideal mixing on equilibration timescales of secondary organic aerosol partitioning

Abstract. Evidence has accumulated that secondary organic aerosols (SOAs) exhibit complex morphologies with multiple phases that can adopt amorphous semisolid or glassy phase states. However, experimental analysis and numerical modeling on the formation and evolution of SOA still often employ equilibrium partitioning with an ideal mixing assumption in the particle phase. Here we apply the kinetic multilayer model of gas–particle partitioning (KM-GAP) to simulate condensation of semi-volatile species into a core–shell phase-separated particle to evaluate equilibration timescales of SOA partitioning. By varying bulk diffusivity and the activity coefficient of the condensing species in the shell, we probe the complex interplay of mass transfer kinetics and the thermodynamics of partitioning. We found that the interplay of non-ideality and phase state can impact SOA partitioning kinetics significantly. The effect of non-ideality on SOA partitioning is slight for liquid particles but becomes prominent in semisolid or solid particles. If the condensing species is miscible with a low activity coefficient in the viscous shell phase, the particle can reach equilibrium with the gas phase long before the dissolution of concentration gradients in the particle bulk. For the condensation of immiscible species with a high activity coefficient in the semisolid shell, the mass concentration in the shell may become higher or overshoot its equilibrium concentration due to slow bulk diffusion through the viscous shell for excess mass to be transferred to the core phase. Equilibration timescales are shorter for the condensation of lower-volatility species into semisolid shell; as the volatility increases, re-evaporation becomes significant as desorption is faster for volatile species than bulk diffusion in a semisolid matrix, leading to an increase in equilibration timescale. We also show that the equilibration timescale is longer in an open system relative to a closed system especially for partitioning of miscible species; hence, caution should be exercised when interpreting and extrapolating closed-system chamber experimental results to atmosphere conditions. Our results provide a possible explanation for discrepancies between experimental observations of fast particle–particle mixing and predictions of long mixing timescales in viscous particles and provide useful insights into description and treatment of SOA in aerosol models.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Genetic Fusion of Thermoresponsive Polypeptides with UCST‐type Behavior Mediates 1D Assembly of Coiled‐Coil Bundlemers

Abstract Thermoresponsive resilin‐like polypeptides (RLPs) of various lengths were genetically fused to two different computationally designed coiled coil‐forming peptides with distinct thermal stability, to develop new strategies to assemble coiled coil peptides via temperature‐triggered phase separation of the RLP units. Their successful production in bacterial expression hosts was verified via gel electrophoresis, mass spectrometry, and amino acid analysis. Circular dichroism (CD) spectroscopy, ultraviolet‐visible (UV/Vis) turbidimetry, and dynamic light scattering (DLS) measurements confirmed the stability of the coiled coils and showed that the thermosensitive phase behavior of the RLPs was preserved in the genetically fused hybrid polypeptides. Cryogenic‐transmission electron microscopy and coarse‐grained modeling revealed that functionalizing the coiled coils with thermoresponsive RLPs leads to their thermally triggered noncovalent assembly into nanofibrillar assemblies.

Patkar, Sai S.↗
DOE OSTI2017

Dewetting and spreading transitions for active matter on random pinning substrates

Here, we show that sterically interacting self-propelled disks in the presence of random pinning substrates exhibit transitions among a variety of different states. In particular, from a phase separated cluster state, the disks can spread out and homogeneously cover the substrate in what can be viewed as an example of an active matter wetting transition. We map the location of this transition as a function of activity, disk density, and substrate strength, and we also identify other phases including a cluster state, coexistence between a cluster and a labyrinth wetted phase, and a pinned liquid. Convenient measures of these phases include the cluster size, which dips at the wetting-dewetting transition, and the fraction of sixfold coordinated particles, which drops when dewetting occurs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Genetic Fusion of Thermoresponsive Polypeptides with UCST–type Behavior Mediates 1D Assembly of Coiled–Coil Bundlemers

Thermoresponsive resilin-like polypeptides (RLPs) of various lengths were genetically fused to two different computationally designed coiled coil-forming peptides with distinct thermal stability, to develop new strategies to assemble coiled coil peptides via temperature-triggered phase separation of the RLP units. Furthermore, their successful production in bacterial expression hosts was verified via gel electrophoresis, mass spectrometry, and amino acid analysis. Circular dichroism (CD) spectroscopy, ultraviolet-visible (UV/Vis) turbidimetry, and dynamic light scattering (DLS) measurements confirmed the stability of the coiled coils and showed that the thermosensitive phase behavior of the RLPs was preserved in the genetically fused hybrid polypeptides. Cryogenic-transmission electron microscopy and coarse-grained modeling revealed that functionalizing the coiled coils with thermoresponsive RLPs leads to their thermally triggered noncovalent assembly into nanofibrillar assemblies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Interfaces in coexisting metals and Mott insulators

Motivated by the direct observation of electronic phase separation in first-order Mott transitions, we model the interface between thermodynamically coexisting metals and Mott insulators. In this work, we show how to model the required slab geometry and extract the electronic spectra. We construct an effective Landau free energy and compute the variation of its parameters across the phase diagram. Finally, using a linear mixture of the density and double occupancy, we identify a natural Ising order parameter which unifies the treatment of the bandwidth and filling controlled Mott transitions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Ultrafiltration membranes from polymerization of self-assembled Pluronic block copolymer mesophases

Industrially, ultrafiltration (UF) membranes are produced through non-solvent induced phase separation (NIPS), but due to environmental hazards inherent to the NIPS process as well as the low surface porosity and fouling resistance of membranes produced via this method, an alternative route to UF membranes is desirable. Here, this work presents the self-assembly of Pluronic block copolymers in the presence of water and a monomeric phase as a new technique for the preparation of UF membranes without the need for organic solvent or post-modification. Different compositions of block copolymer, water, and monomer were polymerized to obtain both hexagonal and lamellar mesostructures, as indicated by small angle X-ray scattering (SAXS) and cross-polarized light microscopy. As-synthesized membranes were found to have pore sizes in the range of 3–4 nm with a molecular weight cutoff of 1500 g/mol and displayed both excellent fouling resistance and high permeance of water, vastly outperforming a conventional NIPS UF membrane. Additionally, in contrast to NIPS, the proposed method provides flexibility in terms of both the final membrane chemistry and pore size. As such, it is a versatile approach that can be easily tailored to produce membranes for a wide range of applications including wastewater treatment and food processing.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Imaging of Electrothermal Filament Formation in a Mott Insulator

Resistive switching—the current- and voltage-induced change of electrical resistance—is at the core of memristive devices, which play an essential role in the emerging field of neuromorphic computing. This study is about resistive switching in a Mott insulator, which undergoes a thermally driven metal-to-insulator transition. Two distinct switching mechanisms are reported for such a system: electric-field-driven resistive switching and electrothermal resistive switching. The latter results from an instability caused by Joule heating. Here, we present the visualization of the reversible resistive switching in a planar V 2 O 3 thin-film device using high-resolution wide-field microscopy in combination with electric transport measurements. We investigate the interaction of the electrothermal instability with the strain-induced spontaneous phase separation in the V 2 O 3 thin film at the Mott transition. The photomicrographs show the formation of a narrow metallic filament with a minimum width ≲500 nm. Although the filament formation and the overall shape of the current-voltage characteristics (IVCs) are typical of an electrothermal breakdown, we also observe atypical effects such as oblique filaments, filament splitting, and hysteretic IVCs with sawtoothlike jumps at high currents in the low-resistance regime. We are able to reproduce the experimental results in a numerical model based on a two-dimensional resistor network. This model demonstrates that resistive switching in this case is indeed electrothermal and that the intrinsic heterogeneity is responsible for the atypical effects. This heterogeneity is strongly influenced by strain, thereby establishing a link between switching dynamics and structural properties.

42 ENGINEERING↗
DOE OSTI2024

Ion‐Specific Interactions Engender Dynamic and Tailorable Properties in Biomimetic Cationic Polyelectrolytes

Abstract Biomaterials such as spider silk and mussel byssi are fabricated by the dynamic manipulation of intra‐ and intermolecular biopolymer interactions. Organisms modulate solution parameters, such as pH and ion co‐solute concentration, to effect these processes. These biofabrication schemes provide a conceptual framework to develop new dynamic and responsive abiotic soft material systems. Towards these ends, the chemical diversity of readily available ionic compounds offers a broad palette to manipulate the physicochemical properties of polyelectrolytes via ion‐specific interactions. In this study, we show for the first time that the ion‐specific interactions of biomimetic polyelectrolytes engenders a variety of phase separation behaviors, creating dynamic thermal‐ and ion‐responsive soft matter that exhibits a spectrum of physical properties, spanning viscous fluids to viscoelastic and viscoplastic solids. These ion‐dependent characteristics are further rendered general by the merger of lysine and phenylalanine into a single, amphiphilic vinyl monomer. The unprecedented breadth, precision, and dynamicity in the reported ion‐dependent phase behaviors thus introduce a broad array of opportunities for the future development of responsive soft matter; properties that are poised to drive developments in critical areas such as chemical sensing, soft robotics, and additive manufacturing.

Aubrecht, Filip J.↗
DOE OSTI2022

Morphology and Dynamics in Hydroxide-Conducting Polysulfones

In alkaline zinc–manganese dioxide batteries, there is a need for selective polymeric separators that have good hydroxide ion conductivity but that prevent the transport of zincate (Zn(OH) 4 ) 2- . Here we investigate the nanoscale structure and hydroxide transport in two cationic polysulfones that are promising for these separators. We present the synthesis and characterization for a tetraethylammonium-functionalized polysulfone (TEA-PSU) and compare it to our previous work on an N-butylimidazolium-functionalized polysulfone (NBI-PSU). We perform atomistic molecular dynamics (MD) simulations of both polymers at experimentally relevant water contents. The MD simulations show that both polymers develop well phase separated nanoscale water domains that percolate through the polymer. Calculation of the total scattering intensity from the MD simulations reveal weak or nonexistent ionomer peaks at low wave vectors. The lack of an ionomer peak is due to a loss of contrast in the scattering. The small water domains in both polymers, with median diameters on the order of 0.5–0.7 nm, lead to hydroxide and water diffusion constants that are 1–2 orders of magnitude smaller than their values in bulk water. This confinement lowers the conductivity but also may explain the strong exclusion of zincate from the PSU membranes seen experimentally.

25 ENERGY STORAGE↗