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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
All sourcesNASA NTRSDOE OSTI
NASA NTRS1993

Thermal history effects on electrical relaxation and conductivity for potassium silicate glass with low alkali concentrations

Electrical response measurements from 10 Hz to 100 kHz between 120 and 540 C were made on potassium-silicate glasses with alkali oxide contents of 2, 3, 5 and 10 mol percent. Low alkali content glasses were chosen in order to try to reduce the Coulombic interactions between alkali ions to the point that frozen structural effects from the glass could be observed. Conductivity and electrical relaxation responses for both annealed and quenched glasses of the same composition were compared. Lower DC conductivity (sigma(sub DC)) activation energies were measured for the quenched compared to the annealed glasses. The two glasses with the lowest alkali contents exhibited a non-Arrhenius concave up curvature in the log(sigma(sub DC)) against 1/T plots, which decreased upon quenching. A sharp decrease in sigma(sub DC) was observed for glasses containing K2O concentrations of 5 mol percent or less. The log modulus loss peak (M'') maximum frequency plots against 1/T all showed Arrhenius behavior for both annealed and quenched samples. The activation energies for these plots closely agreed with the sigma(sub DC) activation energies. A sharp increase in activation energy was observed for both series as the potassium oxide concentration decreased. Changes in the electrical response are attributed to structural effects due to different alkali concentrations. Differences between the annealed and quenched response are linked to a change in the distribution of activation energies (DAE).

Angel, Paul W.↗
DOE OSTI2025

Vortex-Controlled Quasiparticle Multiplication and Self-Growth Dynamics in Superconducting Resonators

Even in the quantum limit, non-equilibrium quasiparticle (QP) populations induce QP poisoning that irreversibly relaxes the quantum state and significantly degrades the coherence of transmon qubits. A particularly detrimental yet previously unexplored mechanism arises from QP multiplication facilitated by vortex trapping in superconducting quantum circuits, where a high-energy QP relaxes by breaking additional Cooper pairs and amplifying the QP population due to the locally reduced excitation gap and enhanced quantum confinement within the vortex core. Here we directly resolve this elusive QP multiplication process by revealing vortex-controlled QP self-generation in a highly nonequilibrium regime preceding the phonon bottleneck of QP relaxation. At sufficiently low fluence, femtosecond-resolved magneto-reflection spectroscopy directly reveals a continuously increasing QP population that is strongly dependent on magnetic-field-tuned vortex density and absent at higher excitation fluences. Quantitative analysis of the emergent QP pre-bottleneck dynamics further reveals that, although the phonon population saturates within $\simeq$10~ps, both free and trapped QPs continue to grow in a self-sustained manner--hallmarks of the long-anticipated QP-vortex interactions in nonequilibrium superconductivity. We estimate a substantial increase of $\sim$34% in QP density at vortex densities of $\sim$ 100 magnetic flux quanta per $\mathrm{μm^{2}}$. Our findings establish a powerful spectroscopic tool for uncovering QP multiplication and reveal vortex-assisted QP relaxation as a critical materials bottleneck whose mitigation will be essential for resolving QP poisoning and enhancing coherence in superconducting qubits.

Park, Joong M. [Ames Lab]↗
DOE OSTI2021

Molecular-level insights into structure and dynamics in ionic liquids and polymer gel electrolytes

We report designing new electrolytes requires a better understanding of the correlation between their transport properties and their molecular structure. In this work, we present a detailed study of ionic liquids and polymer gel electrolytes probing their structure and dynamics by nuclear magnetic resonance (NMR) spectroscopy. In particular, ammonium- and phosphonium-based ionic liquids (ILs) are combined with different LiTFSI concentrations, and then with different ratios of poly(methylmethacrylate) polymer. The temperature dependence of self-diffusion coefficients of mobile species, D Li+ , D TFSI- and D P4441+ or D N4441+ , measured by pulsed field gradient (PFG) NMR spectroscopy obeys the Arrhenius equation. Diffusivity of [P4441][TFSI] ILs is found to be greater than those of the [N4441][TFSI] ILs in both liquid and gel electrolytes. Solid state NMR experiments including 13 C and 19 F MAS, 13 C{ 19 F}, 13 C{ 1 H} CPMAS probe the local structure and molecular-level interactions between ions and polymer in gel electrolytes, particularly for samples with higher PMMA content (≥25 wt%). Finally, the fast field cycling relaxometry has been used to unveil the rotational and translational dynamics of P4441 + or N4441 + and TFSI - by measuring 1 H and 19 F R 1 relaxation rate profiles at different temperatures. A comprehensive NMR analysis including relaxation studies at low magnetic field provides decisive new insights regarding the formation of ionic clusters and the interaction of ions with the polymer chain in the case of the gel electrolytes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Shape Anisotropy-Dependent Leaking in Magnetic Neurons for Bio-Mimetic Neuromorphic Computing

Spiking neural networks seek to emulate biological computation through interconnected artificial neuron and synapse devices. Spintronic neurons can leverage magnetization physics to mimic biological neuron functions, such as integration tied to magnetic domain wall (DW) propagation in a patterned nanotrack and firing tied to the resistance change of a magnetic tunnel junction (MTJ), captured in the domain wall-magnetic tunnel junction (DW-MTJ) device. Leaking, relaxation of a neuron when it is not under stimulation, is also predicted to be implemented based on DW drift as a DW relaxes to a low energy position, but it has not been well explored or demonstrated in device prototypes. Here, in this work, we study DW-MTJ artificial neurons capable of leaky integrate-and-fire (LIF) behavior and demonstrate geometry-dependent leaking dynamics that results in repeatable, tunable LIF operation. Studying the behavior of five different device designs, we show tuning the geometry, stimulating fields and currents, and location of electrical contacts results in a wide range of neuron behavior. Additionally, implementation of an asymmetric notch allows for nonlinear pinning which increased expressivity without sacrificing leaking. The measured behavior is implemented in a simulated spiking neural network that outperforms a 1D model of continuous DW motion and approaches the performance of an ideal LIF activation function. The results show that the analog LIF capability of DW-MTJ neurons combines many desirable neuron functions into a single device, which can result in varied forms of multifunctional neuromorphic computing.

42 ENGINEERING↗
DOE OSTI2021

Dynamical ground state in the XY pyrochlore Yb2GaSbO7

Abstract The magnetic ground state of the pyrochlore Yb 2 GaSbO 7 has not been established. The persistent spin fluctuations observed by muon spin-relaxation measurements at low temperatures have not been adequately explained for this material using existing theories for quantum magnetism. Here we report on the synthesis and characterisation of Yb 2 GaSbO 7 to revisit the nature of the magnetic ground state. Through DC and AC magnetic susceptibility, heat capacity, and neutron scattering experiments, we observe evidence for a dynamical ground state that makes Yb 2 GaSbO 7 a promising candidate for disorder-induced spin-liquid or spin-singlet behaviour. This state is quite fragile, being tuned to a splayed ferromagnet in a modest magnetic field μ 0 H c ~ 1.5 T.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

First-principles calculations of metal surfaces. I. Slab-consistent bulk reference for convergent surface properties

The first-principles computation of the surfaces of metals is typically accomplished through slab calculations of finite thickness. The extraction of a convergent surface formation energy from slab calculations is dependent upon defining an appropriate bulk reference energy. I describe a method for an independently computed, slab-consistent bulk reference that leads to convergent surface formation energies from slab calculations that also provides realistic uncertainties for the magnitude of unavoidable nonlinear divergence in the surface formation energy with slab thickness. In conclusion, the accuracy is demonstrated on relaxed, unreconstructed low-index aluminum surfaces with slabs with up to 35 layers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Solid-state platform for cooperative quantum dynamics driven by correlated emission

While traditionally regarded as an obstacle to quantum coherence, recent breakthroughs in quantum optics have shown that the dissipative interaction of a qubit with its environment can be leveraged to protect quantum states and synthesize many-body entanglement. Inspired by this progress, here we set the stage for the—as yet uncharted—exploration of analogous cooperative phenomena in hybrid solid-state platforms. We develop a comprehensive formalism for the quantum many-body dynamics of an ensemble of solid-state spin defects interacting with the magnetic field fluctuations of a common solid-state reservoir. Our framework applies to any solid-state reservoir whose fluctuating spin, pseudospin, or charge degrees of freedom generate magnetic fields. To understand whether correlations induced by dissipative processes can play a relevant role in a realistic experimental setup, we apply our model to a qubit array interacting via the spin fluctuations of a ferromagnetic bath. Our results show that the low-temperature collective relaxation rates of the qubit ensemble can display clear signatures of super- and subradiance, i.e., forms of cooperative dynamics traditionally achieved in atomic ensembles. We find that the solid-state analog of these cooperative phenomena is robust against spatial disorder in the qubit ensemble and thermal fluctuations of the magnetic reservoir, providing a route for their feasibility in near-term experiments. Finally, our work lays the foundation for a multiqubit approach to quantum sensing of solid-state systems and the direct generation of many-body entanglement in spin-defect ensembles. Furthermore, we discuss how the tunability of solid-state reservoirs opens up novel pathways for exploring cooperative phenomena in regimes beyond the reach of conventional quantum optics setups.

NV centers↗
NASA NTRS1983

NMR (Nuclear Magnetic Resonance) and macromolecular migration in a melt or in concentrated solutions

The purpose of this paper is to analyze the migration process of long polymer molecules in a melt or in concentrated solutions as it may be observed from the dynamics of the transverse magnetization of nuclear spins linked to these chains. The low frequency viscoelastic relaxation of polymer systems is known to be mainly controlled by the mechanism of dissociation of topological constraints excited on chains and which are called entanglements. This mechanism exhibits a strong dependence upon the chain molecular weight. These topological constraints also govern the diffusion process of polymer chains. So, the accurate description of the diffusion motion of a chain may be a convenient way to characterize disentanglement processes necessarily involved in any model proposed to explain viscoelastic effects.

Addad, J. P. C.↗
NASA NTRS1984

Toughening mechanism in elastomer-modified epoxy resins, part 2

The role of matrix ductility on the toughenability and toughening mechanism of elastomer-modified DGEBRA epoxies was investigated. Matrix ductility was varied by using epoxide resins of varying epoxide monomer molecular weights. These epoxide resins were cured using 4,4' diaminodiphenyl sulfone (DDS) and, in some cases, modified with 10% HYCAR(r)CTBN 1300X8. Fracture roughness values for the neat epoxies were found to be almost independent on the monomer molecular weight of the epoxide resin used. However, it was found that the fracture toughness of the elastomer-modified epoxies was very dependent upon the epoxide monomer molecular weight. Tensile dilatometry indicated that the toughening mechanism, when present, is similar to the mechanisms found for the piperidine cured epoxies in Part 1. SEM and OM corroborate this finding. Dynamic mechanical studies were conducted to shed light on the toughenability of the epoxies. The time-dependent small strain behavior of these epoxies were separated into their bulk and shear components. The bulk component is related to brittle fracture, whereas the shear component is related to yielding. It can be shown that the rates of shear and bulk strain energy buildup for a given stress are uniquely determined by the values of Poisson's ratio, nu. It was found that nu increases as the monomer molecular weight of the epoxide resin used increases. This increase in nu can be associated with the low temperature beta relaxation. The effect of increasing cross-link density is to shift the beta relaxation to higher temperatures and to decrease the magnitude of the beta relaxation. Thus, increasing cross-link density decreases nu and increases the tendency towards brittle fracture.

Yee, A. F.↗
NASA NTRS1984

Computer simulation of surface and film processes

All the investigations which were performed employed in one way or another a computer simulation technique based on atomistic level considerations. In general, three types of simulation methods were used for modeling systems with discrete particles that interact via well defined potential functions: molecular dynamics (a general method for solving the classical equations of motion of a model system); Monte Carlo (the use of Markov chain ensemble averaging technique to model equilibrium properties of a system); and molecular statics (provides properties of a system at T = 0 K). The effects of three-body forces on the vibrational frequencies of triatomic cluster were investigated. The multilayer relaxation phenomena for low index planes of an fcc crystal was analyzed also as a function of the three-body interactions. Various surface properties for Si and SiC system were calculated. Results obtained from static simulation calculations for slip formation were presented. The more elaborate molecular dynamics calculations on the propagation of cracks in two-dimensional systems were outlined.

Tiller, W. A.↗
NASA NTRS1985

A model of flow in a closed-loop thermosyphon including the Soret effect

This theoretical study addresses the nature of convective motions in a toroidal loop of binary fluid oriented in the vertical plane and heated from below. The boundaries of the loop are impermeable, but gradients of the solute can be set up by Soret diffusion in the direction around the loop. The existence and stability of steady solutions are discussed over the Rayleigh number-Soret coefficient parameter plane. When the Soret coefficient is negative, periodic and chaotic oscillations analogous to those of thermohaline convection are predicted. When the Soret coefficient is positive, relaxation oscillations and low Rayleigh number chaotic motions are found. Both sets of phenomena are predicted to occur for realistic thermosyphon parameters.

Hart, J. E.↗
NASA NTRS1990

Implicit methods for the Navier-Stokes equations

Numerical solutions of the Navier-Stokes equations using explicit schemes can be obtained at the expense of efficiency. Conventional implicit methods which often achieve fast convergence rates suffer high cost per iteration. A new implicit scheme based on lower-upper factorization and symmetric Gauss-Seidel relaxation offers very low cost per iteration as well as fast convergence. High efficiency is achieved by accomplishing the complete vectorizability of the algorithm on oblique planes of sweep in three dimensions.

Yoon, S.↗
DOE OSTI2020

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↗
DOE OSTI2021

Relaxation of a single defect spin by the low-frequency gyrotropic mode of a magnetic vortex

We excite the gyrotropic mode of a magnetic vortex and observe the resulting effect on the spin state of a nearby nitrogen-vacancy (NV) defect in diamond. Thin permalloy disks fabricated on a diamond sample are magnetized in a vortex state in which the magnetization curls around a central core. The magnetization dynamics of this configuration are described by a discrete spectrum of confined magnon modes as well as a low-frequency gyrotropic mode in which the vortex core precesses about its equilibrium position. Despite the spin transition frequencies being far-detuned from the modes of the ferromagnet, we observe enhanced relaxation of the NV spin when driving the gyrotropic mode. Moreover, we map the spatial dependence of the interaction between the vortex and the spin by translating the vortex core within the disk with an applied magnetic field, resulting in steplike motion as the vortex is pinned and de-pinned. Strong spin relaxation is observed when the vortex core is within approximately 250 nm of the NV center defect. We attribute this effect to the higher frequencies in the spectrum of the magnetic fringe field arising from the soliton-like nature of the gyrotropic mode when driven with sufficiently large amplitude.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Microscopic activated dynamics theory of the shear rheology and stress overshoot in ultradense glass-forming fluids and colloidal suspensions

We formulate a particle and force level, activated dynamics-based statistical mechanical theory for the continuous startup nonlinear shear rheology of ultradense glass-forming hard sphere fluids and colloidal suspensions in the context of the elastically collective nonlinear Langevin equation approach and a generalized Maxwell model constitutive equation. Activated structural relaxation is described as a coupled local-nonlocal event involving caging and longer range collective elasticity which controls the characteristic stress relaxation time. Theoretical predictions for the deformation-induced enhancement of mobility, the onset of relaxation acceleration at remarkably low values of stress, strain, or shear rate, apparent power law thinning of the steady-state structural relaxation time and viscosity, a nonvanishing activation barrier in the shear thinning regime, an apparent Herschel–Buckley form of the shear rate dependence of the steady-state shear stress, exponential growth of different measures of a yield or flow stress with packing fraction, and reduced fragility and dynamic heterogeneity under deformation were previously shown to be in good agreement with experiments. The central new question we address here is the defining feature of the transient response—the stress overshoot. In contrast to the steady-state flow regime, understanding the transient response requires an explicit treatment of the coupled nonequilibrium evolution of structure, elastic modulus, and stress relaxation time. We formulate a new quantitative model for this aspect in a physically motivated and computationally tractable manner. Theoretical predictions for the stress overshoot are shown to be in good agreement with experimental observations in the metastable ultradense regime of hard sphere colloidal suspensions as a function of shear rate and packing fraction, and accounting for deformation-assisted activated motion appears to be crucial for both the transient and steady-state responses.

Mechanics↗
DOE OSTI2021

Structural relaxation and crystallization in supercooled water from 170 to 260 K

The structural relaxation and crystallization of deeply supercooled water are investigated in transiently-heated nanoscale water films using infrared spectroscopy for temperatures between 170 and 260 K. For temperatures above ~230 K, the relaxation kinetics can be fit with a simple exponential decay which is characteristic of normal liquids. At lower temperatures, increasingly non-exponential decay is observed indicating the onset of heterogeneous dynamics. Water’s relaxation rate depends on its initial structure with hyper-quenched glassy water (HQW) typically relaxing more quickly than low-density amorphous solid water (LDA). At all temperatures, the relaxation time, trel is faster than the crystallization time, txtal. For HQW, the ratio, txtal/trel, goes through a minimum at ~198 K where it is about 60. The research was designed and supervised by GAK and BDK. LK and WAT conducted the experiments and analyzed the data. LK and GAK wrote the manuscript, with input from all authors.

Kringle, Loni M.↗
DOE OSTI2020

Viscoelastic Response of Dispersed Entangled Polymer Melts

Any polymer synthesis routes result in molecular weight dispersity DAI, depending on the polymerization mechanism. The lowest dispersity polymers are those made by anionic and atom-transfer radical polymerization, which exhibit relatively narrow distributions DM=g,„1A172 — 1.02-1.04. This small divergence from monodispersity results in significant number of molecules that differ in their molecular weight from the average and their impact on the viscoelastic response remains an open question. Here the effects of low dispersity on stress relaxation and shear viscosity of entangled melts are studied using a coarse-grained model for polyethylene. Polymer melts with chain length dispersity set to follow a Schulz-Zimm distribution of Dm = 1.0 — 1.16 for an entangled polyethylene melt using molecular dynamic simulations. The systems were studied to times up to 800 ,us which is beyond the terminal time. These systems are compared to those with binary and ternary distributions. The stress relaxation functions were extracted from the Green-Kubo relation and from stress-strain relaxation following a uniaxial extension. We find on the entanglement time scale, both the mean squared displacement and the stress relaxation are independent of D m . The tube diameter and the rubbery plateau for entangled dynamics do not depend on D m . At longer times, the terminal relaxation time decreases as the faster motion of the shorter chains results in constraint release for the longer chains. Probing this low dispersity regime opens the way to evaluate the degree of dispersity that affects mechanical properties.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗