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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 73 records · Page 4

Fragile-to-strong transition in liquid As 2 S 3 under pressure: The effect of melt metallization

The well-known classification of glass-forming melts into fragile and strong liquids has several notable exceptions, including water, silica, and certain phase-change materials (PCMs). These exceptional fluid systems exhibit a fragile-to-strong transition (FST) upon cooling: a transformation from a high-temperature liquid with fast atomic dynamics, low viscosity, and low flow activation energy, to a viscous supercooled melt with high energy barriers near the glass transition temperature T g . This behavior is critically important for non-volatile memories, photonic tensor cores, reconfigurable metamaterials, and other devices, that use PCMs, enabling nanosecond-scale crystallization in the fragile regime and long data retention in the strong regime near or below T g . A significant structural transformation is expected between these two viscosity regimes, along with a semiconductor-metal (SC-M) transition upon heating, driven by high internal pressure and associated density increase. By applying high external pressure to the canonical low-conducting chalcogenide melt As 2 S 3 , we observed both the FST and the SC-M transition, occurring simultaneously within the same domain of the P, T−phase space. These findings suggest that the FST is not limited to a few exceptional liquids but is a common phenomenon, at least in systems that exhibit melt metallization within specific regions of their P, T−phase diagrams.

first-principles molecular dynamics↗

High-speed imaging of transition from fluid breakup to phase explosion in electric explosion of tungsten wires in air

High-speed visible imaging of sub-microsecond electric explosion of wires at the low specific energy deposition threshold reveals three distinct modes of wire failure as capacitor charge voltage and energy deposition are increased. For 100 micron diameter gold-plated tungsten wires of 2 cm length, deposited energies of 1.9 eV/atom produces a liquid column that undergoes hydrodynamic breakup into droplets with radii of order of wire diameter on timescales of 200 μs. Instability growth, column breakup, and droplet coalescence follow classic Rayleigh-Plateau predictions for instability of viscous fluid column. Above 3.2 eV/atom of deposited energy, wires are seen to abruptly transition to an expanding mixture of micron scale liquid-droplets and vapor within one frame (less than 3.33 μs), which has been termed ‘phase explosion’ in literature. Between these two limits, at 2.5 eV/atom of deposited energy, wire radius is unchanged for the first 10 μs before the onset of a rapid expansion and disintegration that resembles homogenous nucleation of mechanically unstable bubbles. Here, thermodynamic calculations are presented that separate cases by temperature obtained during heating: below boiling point, near boiling point, and exceeding boiling point.

42 ENGINEERING↗

Two-dimensional hydrodynamic viscous electron flow in annular Corbino rings

The concept of fluidic viscosity is ubiquitous in condensed-matter systems hosting a continuum where macroscopic properties can emerge. While an important property of liquids and some solids, only recently was the viscosity of an electron shown to play a role in electronic transport experiments. In this Letter, we present nonlocal electronic transport measurements in concentric annular rings formed in high-mobility two-dimensional electron gases, and the resulting data show that viscous hydrodynamic flow can occur far away from the source-drain current region. Our conclusion of viscous electronic transport is further corroborated by simulations of the Navier-Stokes equations that are found to be in agreement with our measurements below T = 1 K . Finally, this work emphasizes the key role played by viscosity via electron-electron ( e − e ) interaction even when the electronic transport is restricted radially, and for which it should have played no major role. Published by the American Physical Society 2025

Vijayakrishnan, Sujatha (ORCID:0009000080933182)↗

Release of Contaminants from Burning Liquids and Solids

This report details model development, theory, and a literature review focusing on the emission of contaminants on solid substrates in fires. This is the final report from a 2-year Nuclear Safety Research and Development (NSRD) project. The work represents progress towards a goal of having modeling and simulation capabilities that are sufficiently mature and accurate that they can be utilized in place of physical tests for determining safe handling practices. At present, the guidelines for safety are largely empirically based, derived from a survey of existing datasets. This particular report details the development, verification and calibration of a number of code improvements that have been implemented in the SIERRA suite of codes, and the application of those codes to three different experimental scenarios that have been subject of prior tests. The first scenario involves a contaminated PMMA slab, which is exposed to heat. The modeling involved a novel method for simulating the viscous diffusion of the particles in the slab. The second scenario involved a small pool fire of contaminated combustible liquid mimicking historical tests and finds that the release of contaminants has a high functionality with the height of the liquid in the container. The third scenario involves the burning of a contaminated tray of shredded cellulose. A novel release mechanism was formulated based on predicted progress of the decomposition of the cellulose, and while the model was found to result in release that can be tuned to match the experiments, some modifications to the model are desirable to achieve quantitative accuracy.

54 ENVIRONMENTAL SCIENCES↗

Experiment and model for a Stokes layer in a strongly coupled dusty plasma

A Stokes layer, which is a flow pattern that arises in a viscous fluid adjacent to an oscillatory boundary, was observed in an experiment using a two-dimensional strongly coupled dusty plasma. Liquid conditions were maintained using laser heating, while a separate laser manipulation applied an oscillatory shear that was localized and sinusoidal. The evolution of the resulting flow was analyzed using space-time diagrams. These figures provide an intuitive visualization of a Stokes layer, including features such as the depth of penetration and wavelength. Another feature, the characteristic speed for the penetration of the oscillatory flow, also appears prominently in space-time diagrams. To model the experiment, the Maxwell-fluid model of a Stokes layer was generalized to describe a two-phase liquid. In our experiment, the phases were gas and dust, where the dust cloud was viscoelastic due to strong Coulomb coupling. Furthermore, the model is found to agree with the experiment, in the appearance of the space-time diagrams, and in the values of the characteristic speed, depth of penetration, and wavelength.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High-temperature and high-pressure NMR investigations of low viscous fluids confined in mesoporous systems

Abstract In this contribution, the relaxation and diffusional behaviors of low viscous fluids, water and methanol confined into mesoporous silica and controlled size pore glass were investigated. The engineered porous systems are relevant to geologically important subsurface energy materials. The engineered porous proxies were characterized by Brunauer–Emmett–Teller (BET) surface analyzer, nuclear magnetic resonance (NMR) spectroscopy, and electron microscopy (EM) to determine surface area, pore-wall protonation and morphology of these materials, respectively. The confined behavior of the low viscous fluids was studied by varying pore diameter, fluid-to-solid ratio, temperature, and pressure, and then compared to bulk liquid state. Both relaxation and diffusion behaviors for the confined fluids showed increasing deviation from pure bulk fluids as the fluid-to-solid ratio was decreased, and surface-to-volume ratio ( S / V ) was varied. Variable pressure deuteron NMR relaxation of confined D 2 O and confined methanol, deuterated at the hydroxyl or methyl positions, were performed to exploit the sensitivity of the deuteron quadrupole moment to molecular rotation. The methanol results demonstrated greater pressure dependence than those for water only in bulk. The deviations from bulk liquid behavior arise from different reasons such as confinement and the interactions between confined fluid and the nano-pore wall. The results of the present report give insight into the behavior of low viscosity fluid in nano-confined geometries under different state conditions.

Chemistry↗

Pushing the Boundaries of Relativistic Fluid Dynamics: From Particle Colliders to Neutron Star Mergers

This project aimed at establishing connections between fluid dynamics, kinetic theory, and string theory to develop new tools to characterize the far-from-equilibrium properties of relativistic systems, which are instrumental in understanding the emergence of liquid-like behavior of the quark-gluon plasma formed in heavy-ion collisions. This project investigated the fundamental properties of viscous fluids in the full nonlinear regime to pave the way for the systematic inclusion of viscous effects in future numerical simulations of neutron star mergers.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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↗

Elucidating the Mechanism of Helium Evaporation from Liquid Water

Here, we investigate the evaporation of trace amounts of helium solvated in liquid water using molecular dynamics simulations and theory. Consistent with experimental observations, we find a super-Maxwellian distribution of kinetic energies of evaporated helium. This excess of kinetic energy over typical thermal expectations is explained by an effective continuum theory of evaporation based on a Fokker–Planck equation, parametrized molecularly by a potential of mean force and position-dependent friction. Using this description, we find that helium evaporation is strongly influenced by the friction near the interface, which is anomalously small near the Gibbs dividing surface due to the ability of the liquid–vapor interface to deform around the gas particle. Our reduced description provides a mechanistic interpretation of trace gas evaporation as the motion of an underdamped particle in a potential subject to a viscous environment that varies rapidly across the air–water interface. From it we predict the temperature dependence of the excess kinetic energy of evaporation, which is yet to be measured.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hydrodynamic electron transport near charge neutrality

We develop the theory of hydrodynamic electron transport in a long-range disorder potential for conductors in which the underlying electron liquid lacks Galilean invariance. For weak disorder, we express the transport coefficients of the system in terms of the intrinsic kinetic coefficients of the electron liquid and the correlation function of the disorder potential. We apply these results to analyze the doping and temperature dependence of transport coefficients of graphene devices. In this work, we show that at charge neutrality, long-range disorder increases the conductivity of the system above the intrinsic value. The enhancement arises from the predominantly vortical hydrodynamic flow caused by local deviations from charge neutrality. Its magnitude is inversely proportional to the shear viscosity of the electron liquid and scales as the square of the disorder correlation radius. This is qualitatively different from the situation away from charge neutrality. In that case, the flow is predominantly potential and produces negative viscous contributions to the conductivity, which are proportional to the sum of shear and bulk viscosities and inversely proportional to the square of disorder correlation radius.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Heterogeneous oxidation of amorphous organic aerosol surrogates by O 3 , NO 3 , and OH at typical tropospheric temperatures

Typical tropospheric temperatures render possible phase states of amorphous organic aerosol (OA) particles of solid, semisolid, and liquid. This will affect the multiphase oxidation kinetics involving the organic condensed-phase and gaseous oxidants and radicals. To quantify this effect, we determined the reactive uptake coefficients (γ) of O 3 , NO 3 , and OH by substrate films composed of single and binary OA surrogate species under dry conditions for temperatures from 213 to 313 K. A temperature-controlled coated-wall flow reactor coupled to a chemical ionization mass spectrometer was applied to determine γ with consideration of gas diffusion transport limitation and gas flow entrance effects, which can impact heterogeneous reaction kinetics. The phase state of the organic substrates was probed via the poke-flow technique, allowing the estimation of the substrates' glass transition temperatures. γ values for O 3 and OH uptake to a canola oil substrate, NO 3 uptake to a levoglucosan and a levoglucosan / xylitol substrate, and OH uptake to a glucose and glucose / 1,2,6-hexanetriol substrate have been determined as a function of temperature. We observed the greatest changes in γ with temperature for substrates that experienced the largest changes in viscosity as a result of a solid-to-liquid phase transition. Organic substrates that maintain a semisolid or solid phase state and as such a relatively higher viscosity do not display large variations in heterogeneous reactivity. From 213 to 293 K, γ values of O 3 with canola oil, of NO 3 with a levoglucosan / xylitol mixture, and of OH with a glucose / 1,2,6-hexanetriol mixture and canola oil, increase by about a factor of 34, 3, 2, and 5, respectively, due to a solid-to-liquid phase transition of the substrate. These results demonstrate that the surface and bulk lifetime of the OA surrogate species can significantly increase due to the slowed heterogeneous kinetics when OA species are solid or highly viscous in the middle and upper troposphere. This experimental study will further our understanding of the chemical evolution of OA particles with subsequent important consequences for source apportionment, air quality, and climate.

54 ENVIRONMENTAL SCIENCES↗

Directional self-locomotion of active droplets enabled by nematic environment

Active matter comprised of self-propelled interacting units holds a major promise for the extraction of useful work from its seemingly chaotic dynamics. Streamlining active matter is especially important at microscale, where the viscous forces prevail over inertia and transport requires a non-reciprocal motion. Here we report that microscopic active droplets representing aqueous dispersions of swimming bacteria Bacillus subtilis become unidirectionally motile when placed in an inactive nematic liquid crystal medium. Random motion of bacteria inside the droplet is rectified into a directional self-locomotion of the droplet by the polar director structure that the droplet creates in the surrounding nematic through anisotropic molecular interactions at its surface. Droplets without active swimmers show no net displacement. The trajectory of the active droplet can be predesigned by patterning the molecular orientation of the nematic. As a result, the effect demonstrates that broken spatial symmetry of the medium can be the reason for and the means to control directional microscale transport.

59 BASIC BIOLOGICAL SCIENCES↗

Crystalline Organic Compounds as Effective Nuclei in Contact Efflorescence of Ammonium Sulfate

Contact nucleation is believed to play a role in liquid-to-solid phase transitions in the atmosphere including ice nucleation and salt efflorescence. Here, for this work, contact efflorescence of optically levitated ammonium sulfate droplets by collisions with organic particles is probed using a long working-distance optical trap. Two highly viscous water-soluble organic compounds (d-(+)-raffinose and citric acid), and two insoluble highly surface-active organic compounds (stearic acid and cis-pinonic acid) were probed for their ability to induce efflorescence upon contact. While three of the organics showed minimal effectiveness as contact nuclei, cis-pinonic acid showed a remarkable ability to initiate contact efflorescence of ammonium sulfate, occurring near ammonium sulfate’s deliquescence relative humidity. Further analysis of cis-pinonic acid using bright-field microscopy in an electrodynamic balance provided evidence that the cis-pinonic acid particles are crystalline under the laboratory conditions. We suggest that the close lattice match between crystalline ammonium sulfate and crystalline cis-pinonic acid may account for the observed effectiveness in initiating contact efflorescence of ammonium sulfate. In contrast, tests of contact nucleation between cis-pinonic acid and sodium chloride, a pair with a poor lattice match, did not result in efflorescence. These findings suggest that crystalline organic compounds in the atmosphere could act as effective nuclei for contact efflorescence of atmospherically relevant salts, provided they share a compatible lattice structure.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Pressure drop in a prototypical 3D magnetohydrodynamic flow across contraction of a fusion blanket manifold

Predicting 3D magnetohydrodynamic (MHD) pressure losses associated with liquid metal flows in complex geometry ducts is required to design breeding blankets for fusion reactors. Of such components, manifolds exhibit major pressure losses. Recent correlations [T. Rhodeset al. Magnetohydrodynamic pressure drop and flow balancing of liquid metal flow in a prototypic fusion blanket manifold. Phys. Fluids. 2018; 30: 057101.] demonstrate promise for predicting pressure drops in electrically insulated inlet manifolds. In the present work, the extend to which these correlations can be applied to outlet manifolds, which feature sudden contractions, is investigated in both viscous-electromagnetic (VE) and inertial-electromagnetic (IE) regimes for Reynolds numbers 50 < Re < 1500, Hartmann numbers 2500 < Ha < 5475, and expansion/contraction ratio 10. Numerical computations have shown that the MHD pressure drops in the eutectic lead-lithium (PbLi) flows in contractions are almost identical to those in the flows featuring expansion with slightly higher magnitudes in the contraction cases. The small discripancy in the MHD pressure drop between contractions and expansions (<8%) suggests that the earlier obtained correlations for the 3D MHD pressure drop in a duct flow with a sudden expansion can also be applied to flows with a sudden contraction.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Molecular Modes Elucidate the Nuclear Magnetic Resonance Relaxation of Viscous Fluids

The Bloembergen, Purcell, and Pound (BPP) theory of nuclear magnetic resonance (NMR) relaxation in fluids dating back to 1948 continues to be the linchpin in interpreting NMR relaxation data in applications ranging from characterizing fluids in porous media to medical imaging (MRI). The BPP theory is founded on assuming molecules are hard spheres with 1 H– 1 H dipole pairs reorienting randomly; assumptions that are severe in light of modern understanding of liquids. Nevertheless, it is intriguing to this day that the BPP theory was consistent with the original experimental data for glycerol, a hydrogen-bonding molecular fluid for which the hard-sphere-rigid-dipole assumption is inapplicable. To better understand this incongruity, atomistic molecular simulations are used to compute 1 H NMR T 1 relaxation dispersion (i.e., frequency dependence) in two contrasting cases: glycerol, and a (non hydrogen-bonding) viscosity standard. At high viscosities, simulations predict distinct functional forms of T 1 for glycerol compared to the viscosity standard, in agreement with modern measurements, yet both in contrast to BPP theory. The cause of these departures from BPP theory is elucidated, without assuming any relaxation models and without any free parameters, by decomposing the simulated T 1 response into dynamic molecular modes for both intramolecular and intermolecular interactions. The decomposition into dynamic molecular modes provides an alternative framework to understand the physics of NMR relaxation for viscous fluids.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Particle-Phase Diffusion Modulates Partitioning of Semivolatile Organic Compounds to Aged Secondary Organic Aerosol

The diffusivity of semivolatile organic compounds (SVOCs) in the bulk particle phase of a viscous atmospheric secondary organic aerosol (SOA) can have a profound impact on aerosol growth and size distribution dynamics. Here, we investigate the bulk diffusivity of SVOCs formed from photo-oxidation of isoprene as they partition to a bimodal aerosol consisting of an Aitken (potassium sulfate) and accumulation mode (aged α-pinene SOA) particles as a function of relative humidity (RH). The model analysis of the observed size distribution evolution shows that liquid-like diffusion coefficient values of D b > 10 –10 cm 2 s –1 fail to explain the growth of the Aitken mode. Instead, much lower values of Db between 2.5 × 10 –15 cm 2 s –1 at 32% RH and 8 × 10 –15 cm 2 s –1 at 82% RH were needed to successfully reproduce the growth of both modes. The diffusivity within the aged α-pinene SOA remains appreciably slow even at 80% RH, resulting in hindered partitioning of SVOCs to large viscous particles and allowing smaller and relatively less viscous particles to effectively absorb the available SVOCs and grow much faster than would be possible otherwise. Our results have important implications for modeling SOA formation and growth in the ambient atmosphere.

54 ENVIRONMENTAL SCIENCES↗

The relaxation behavior of supercooled and glassy imidacloprid

Employing dielectric spectroscopy, oscillatory shear rheology, and calorimetry, the present work explores the molecular dynamics of the widely used insecticide imidacloprid above and below its glass transition temperature. In its supercooled liquid regime, the applied techniques yield good agreement regarding the characteristic structural (alpha) relaxation times of this material. In addition, the generalized Gemant–DiMarzio–Bishop model provides a good conversion between the frequency-dependent dielectric and shear mechanical responses in its viscous state, allowing for an assessment of imidacloprid’s molecular hydrodynamic radius. In order to characterize the molecular dynamics in its glassy regime, we employ several approaches. These include the application of frequency–temperature superposition (FTS) to its isostructural dielectric and rheological responses as well as use of dielectric and calorimetric physical aging and the Adam–Gibbs–Vogel model. While the latter approach and dielectric FTS provide relaxation times that are close to each other, the other methods predict notably longer times that are closer to those reflecting a complete recovery of ergodicity. In conclusion, this seemingly conflicting dissimilarity demonstrates that the molecular dynamics of glassy imidacloprid strongly depends on its thermal history, with high relevance for the use of this insecticide as an active ingredient in technological applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Closed-form theoretical model of the secondary drop size in partial coalescence—Capturing pertinent timescales and viscous forces

One of the most important outcomes of partial drop coalescence is the ratio of the secondary drop radius to the primary drop radius, known as the drop ratio, ri. This ratio is thought to be approximately constant and independent of physical parameters of the fluids involved. However, here we reveal that ambient fluid viscosity can alter the size of the secondary drop and the drop ratio consequently. Using scaling analysis, we derive a model that predicts the behavior of the drop ratio as a function of the Ohnesorge number, a dimensionless ratio of viscous to inertial forces. In addition, we present our experimental results of coalescing drops on a planar interface under the influence of surface tension gradients. A high-speed digital camera is used to observe the evolution of drops as they coalesce with a bulk liquid. We show that this process is influenced by the surface tension gradient between the drop and the bulk liquid. The ratio of the secondary drop to the primary drop in partial coalescence is smaller than the reported values for coalescence without a surface tension gradient. The analytical model derived through this study is based on a new modified Ohnesorge number that includes surface tension gradients. Our analytical model is compared against other models and the results illustrate good agreement with our experimental findings and experimental data in the literature.

42 ENGINEERING↗