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At least 1,513 records · Page 84

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DOE OSTI2020

Giant electron–phonon coupling of the breathing plane oxygen phonons in the dynamic stripe phase of $\hbox {La}_{1.67}\hbox {Sr}_{0.33}\hbox {NiO}_4$

Doped antiferromagnets host a vast array of physical properties and learning how to control them is one of the biggest challenges of condensed matter physics. La 1.67 Sr 0.33 NiO 4 (LSNO) is a classic example of such a material. At low temperatures holes introduced via substitution of La by Sr segregate into lines to form boundaries between magnetically ordered domains in the form of stripes. The stripes become dynamic at high temperatures, but LSNO remains insulating presumably because an interplay between magnetic correlations and electron–phonon coupling localizes charge carriers. Magnetic degrees of freedom have been extensively investigated in this system, but phonons are almost completely unexplored. We searched for electron–phonon anomalies in LSNO by inelastic neutron scattering. Giant renormalization of plane Ni–O bond-stretching modes that modulate the volume around Ni appears on entering the dynamic charge stripe phase. Other phonons are a lot less sensitive to stripe melting. Dramatic overdamping of the breathing modes indicates that dynamic stripe phase may host small polarons. We argue that this feature sets electron–phonon coupling in nickelates apart from that in cuprates where breathing phonons are not overdamped and point out remarkable similarities with the colossal magnetoresistance manganites.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS2001

Carbon Dioxide Cycling And The Climate of Ancient Earth

The continental cycle of silicate weathering and metamorphism dynamically buffers atmospheric CO2 and climate. Feedback is provided by the strong temperature dependence of silicate weathering. Here we argue that hydrothermal alteration of oceanic basalts also dynamically buffers CO2. The oceanic cycle links with the mantle via subduction and the midocean ridges. Feedback is provided by the dependence of carbonatization on dissolved carbonates in seawater. Unlike the continental cycle, the oceanic cycle has no thermostat. Currently the continental cycle is more important, but earlier in Earth's history, especially if heat flow were higher than it is now, more vigorous plate tectonics would have made the oceanic cycle dominant. We find that CO2 greenhouses thick enough to defeat the faint early sun are implausible and that, if no other greenhouse gases are invoked, very cold climates are expected for much of the Proterozoic and the Archean. We echo current fashion and favor biogenic methane as the chief supplement to CO2. Fast weathering and probable subduction of abundant impact ejecta would have reduced CO2 levels still further in the Hadean. Despite its name, the Hadean would have been the coldest era in the history of the Earth.

Zahnle, Kevin↗

NASA NTRS2001

Carbon Dioxide Cycling and the Climate of Ancient Earth

The continental cycle of silicate weathering and metamorphism dynamically buffers atmospheric CO2 and climate. Feedback is provided by the strong temperature dependence of silicate weathering. Here we argue that hydrothermal alteration of oceanic basalts also dynamically buffers CO2. The oceanic cycle links with the mantle via subduction and the midocean ridges. Feedback is provided by the dependence of carbonatization on dissolved carbonates in seawater. Unlike the continental cycle, the oceanic cycle has no thermostat. Currently the continental cycle is more important, but earlier in Earth's history, especially if heat flow were higher than it is now, more vigorous plate tectonics would have made the oceanic cycle dominant. We find that CO2 greenhouses thick enough to defeat the faint early Sun are implausible and that, if no other greenhouse gases are invoked, very cold climates are expected for much of the Proterozoic and the Archean. We echo current fashion and favor biogenic methane as the chief supplement to CO2. Fast weathering and probable subduction of abundant impact ejecta would have reduced CO2 levels still further in the Hadean. Despite its name, the Hadean would have been the coldest era in the history of the Earth.

Zahnle, Kevin↗

DOE OSTI2024

Terahertz parametric amplification as a reporter of exciton condensate dynamics

Condensates are a hallmark of emergence in quantum materials with superconductors and charge density wave as prominent examples. An excitonic insulator (EI) is an intriguing addition to this library, exhibiting spontaneous condensation of electron-hole pairs. However, condensate observables can be obscured through parasitic coupling to the lattice. Time-resolved terahertz (THz) spectroscopy can disentangle such obscurants through measurement of the quantum dynamics. We target Ta 2 NiSe 5 , a putative room-temperature EI where electron-lattice coupling dominates the structural transition (T c = 326 K), hindering identification of excitonic correlations. A pronounced increase in the THz reflectivity manifests following photoexcitation and exhibits a BEC-like temperature dependence. This occurs well below the T c , suggesting a novel approach to monitor exciton condensate dynamics. Nonetheless, dynamic condensate-phonon coupling remains as evidenced by peaks in the enhanced reflectivity spectrum at select infrared-active phonon frequencies. This indicates that parametric reflectivity enhancement arises from phonon squeezing, validated using Fresnel-Floquet theory and density functional calculations. In conclusion, our results highlight that coherent dynamics can drive parametric stimulated emission with concomitant possibilities, including entangled THz photon generation.

36 MATERIALS SCIENCE↗

NASA NTRS1972

Temporal variations in night-time hydroxyl rotational temperature.

Airborne and groundbased OH measurements showing short-term temporal variations in OH rotational temperature are presented. These variations are interpreted in terms of a dynamic model of the OH emitting layer in which the intensity variations result from the changes in temperature the OH layer undergoes as it moves during the night.

Sivjee, G. G.↗

NASA NTRS1986

Venus mesosphere and thermosphere. I - Heat budget and thermal structure

The calculation of a reasonable global average temperature structure is the first step in the simulation of the dynamics and observed characteristics of Venus's upper mesosphere and thermosphere. Various physical processes that influence Venus temperatures are examined, using updated inputs and new parameterizations. It is demonstrated, using a one-dimensional NLTE radiative transfer code, that temperatures observed during the Pioneer Venus mission can be reproduced using an O-CO2 collisional excitation rate coefficient of 4 x 10 to the -13th cu cm/s for strong 15-micron cooling, balanced by 9.5 percent-efficient EUV heating. Cooling by eddy mixing is at best a minor contribution to the total cooling required. Exospheric temperatures are calculated to vary by 60 K or less over a solar cycle, in rough agreement with observations. It is concluded that CO2 cooling effectively buffers against such solar perturbations, due to its nonlinear temperature dependence.

Dickinson, R. E.↗

NASA NTRS1991

An equatorial temperature and wind anomaly (ETWA)

Data obtained from the WATS (Wind and Temperature Spectrometer) and LP (Langmuir Probe) experiments on board DE-2 (Dynamic Explorer) during high solar activity show evidence of anomalous latitudinal variations in the zonal winds and temperature at low latitudes. The zonal winds exhibit a broad maximum centered around the dip equator, flanked by minima on either side around 25 degrees; while the temperature exhibits a pronounced bowl-shaped minimum at the dip equator which is flanked by maxima. The two minima in the zonal winds and the corresponding maxima in the temperature are nearly collocated with the crests of the well known Equatorial Ionization Anomaly (EIA). The maximum in the zonal winds and the minimum in the gas temperature are collocated with the trough of the EIA. The differences between the maxima and minima in temperature and zonal winds, on many occasions, are observed to exceed 100 K and 100 m/s, respectively. The characteristics of this new phenomenon have eluded present day empirical models of thermospheric temperature and winds. The connection among these variables can be understood from the ion-neutral drag effect on the motions of the neutrals that in turn affect their energy balance.

Raghavarao, R.↗

NASA NTRS1998

High-Temperature, High-Flux Multifoil Shield Developed for Space Applications

Spacecraft employing solar dynamic power systems typically use parabolic, point focus concentrators to collect solar power and direct it to the aperture of a heat receiver. Solar fluxes several thousand times the intensity of one solar constant are typically produced in the focal plane of such concentrators. Under heat loading this severe, passively cooled surfaces constructed of most engineering materials would rapidly melt. Therefore, high-temperature shielding is required to protect heat receiver surfaces and other spacecraft surfaces that may be exposed to high flux. To meet this challenge for the joint U.S./Russian Solar Dynamic Flight Demonstration Program, AlliedSignal Aerospace and the NASA Lewis Research Center developed a high-temperature, high-flux multifoil shield tolerant of extreme heat loading conditions in a vacuum environment. The shield is passively cooled, obviating the need for pumped fluid loops and/or heat pipe cooling systems with their attendant cost, mass, complexity, and reliability issues.

Kerslake, Thomas W.↗

DOE OSTI2023

Evolution of dislocation loops and voids in post-irradiation annealed ThO 2 : A combined in-situ TEM and cluster dynamics investigation

The effect of isochronal annealing on the evolution of dislocation loop and void population in proton irradiated ThO 2 has been investigated. Post-irradiation annealing in other actinide oxides like UO 2 shows significant loop coarsening. ThO 2 samples were irradiated with 2 MeV protons up to a dose of 0.1 dpa at 600°C. Post-irradiation isochronal annealing was performed at 600, 800, 1000 and 1100°C for 1 h at each temperature using in-situ TEM. Only faulted 1/3<111> type dislocation loops were observed, and their sizes and distribution were characterized. Further, the population of self-interstitial atom (SIA) dislocation loops did not show any significant growth and coarsening. Additionally, nanometric voids were observed at annealing temperatures of 1000 and 1100°C. Using cluster dynamics (CD), we have studied the nucleation and growth of point defects and defect clusters, i.e., SIA prismatic dislocation loops and nanometric and sub-nanometric voids in proton irradiated ThO 2 . The CD model was further utilized to predict the growth and coarsening of loops and voids during isochronal annealing at the experimental and higher temperatures. The model did not predict significant SIA loop growth which closely corresponds to the TEM observations. CD predicted SIA loop coarsening is insignificant even at high annealing temperature of 1500°C because the model only considers the growth of defect clusters by absorption of like point defects, i.e., SIA loops absorb interstitials and voids absorb vacancies, and cannot account for their migration and coalescence due to elastic interaction. The CD model also predicts the evolution of nanometric voids having mean size within the error bounds of TEM observations.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRS1986

The solar and dynamically induced oscillations in the stratosphere

The temporal and spatial features of stratospheric fluctuations are analyzed using 2.5 years of ozone and temperature data from the Nimbus 7 solar backscattered ultraviolet and the SAMS experiments. It is observed that the oscillations are dynamically induced perturbations in the winter hemisphere and the 27-day modulation of the solar UV radiation. The fluctuations in the ozone and temperature are compared with solar activity. The effects of solar and temperature perturbations on stratospheric ozone are examined; it is shown that the dynamically induced oscillations are global and independent of solar activity. The seasonal, latitudinal, and altitudinal variations of the regression factors and their influence on the ozone are studied. Multiple regression and cross-spectral analyses of ozone, temperature, and solar flux data reveal that the ozone mixing ratio is more sensitive to changes in temperature than changes in solar activity.

Chandra, S.↗

NASA NTRS1998

Final Report

This grant was made to fund two accepted proposals to observe with the ASCA satellite: (1) Debunking the myth of two-temperature coronae of active stars, and (2) Dynamic coronae of dMe stars. We obtained the requested observations and have now completed two papers that will be published in the Astrophysical Journal. The RS CVn binary star UX Ari was observed for 14 hours with all four detectors onboard the ASCA satellite. The X-ray emission was at a constant, quiescent level during the first 12 hours, after which time a powerful flare with a peak luminosity of 1.4 x 10(exp 32) ergs/s started. The flare was observed until shortly after its peak. We present a spectral and temporal analysis of the UX Ari observations and analyze the data with a two-ribbon flare model including estimates for cooling losses. A time-dependent reconstruction of the emission measure (EM) distribution shows that two separate plasma components evolve during the flare (one being identified with the quiescent EM). Most of the flare EM reaches temperatures between 50 MK and 100 MK or more. Magnetic confinement requires the loop arcade to be geometrically large, with length scales on the order of one stellar radius. The electron densities inferred from the model decrease from initial values around 10(exp 12)/cc early in the flare to about 10(exp 11)/cc at the flare peak. The best-fit models require surface magnetic field strengths of a few hundred G, compatible with the maximum photospheric fields expected from equipartition. The flare parameters imply a (conductive and radiative) cooling loss time of less than one hour at flare peak. The elemental abundances increase significantly during the flare rise, with the abundances of the low-FIP elements Fe, Mg, Si, and Ni typically increasing to higher levels than the high-FIP elements such as S or Ne. The Fe abundance increases from (17 +/- 4)% of the solar photospheric value during quiescence up to (89 +/- 18)% at flare peak. A fractionation process that occurs during the chromospheric evaporation phase may selectively enrich low-FIP elements as in the solar corona; alternatively, the chromospheric evaporation may itself bring metal-rich plasma into the metal-poor corona.

Linsky, Jeffrey L.↗

DOE OSTI2020

Structural and spectral dynamics of single-crystalline Ruddlesden-Popper phase halide perovskite blue light-emitting diodes

Achieving perovskite-based high–color purity blue-emitting light-emitting diodes (LEDs) is still challenging. Here, we report successful synthesis of a series of blue-emissive two-dimensional Ruddlesden-Popper phase single crystals and their high–color purity blue-emitting LED demonstrations. Although this approach successfully achieves a series of bandgap emissions based on the different layer thicknesses, it still suffers from a conventional temperature-induced device degradation mechanism during high-voltage operations. To understand the underlying mechanism, we further elucidate temperature-induced device degradation by investigating the crystal structural and spectral evolution dynamics via in situ temperature-dependent single-crystal x-ray diffraction, photoluminescence (PL) characterization, and density functional theory calculation. The PL peak becomes asymmetrically broadened with a marked intensity decay, as temperature increases owing to [PbBr 6 ] 4- octahedra tilting and the organic chain disordering, which results in bandgap decrease. This study indicates that careful heat management under LED operation is a key factor to maintain the sharp and intense emission.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Tuning the Conformations of an M4L4 Cage and Their Impact on Catalysis

Enzymes catalyze chemical reactions with remarkable rate enhancements and selectivity. Supramolecular catalysis seeks to understand and emulate these outcomes, leveraging noncovalent interactions, electric fields, and controlled active site microenvironments to enhance catalysis in an enzyme-like fashion. The effects of conformational dynamics on supramolecular catalysts and assemblies are, however, relatively unexplored, despite their crucial role in enzyme rate enhancement. Here, we elucidate the conformational landscape of a model M4L4 supramolecular host through a rational approach: stabilizing a high-energy conformer through distal ligand modification and a transient intermediate state through symmetry-matched guest encapsulation, as well as tuning the conformer distribution through same-charge metal exchange at the host vertices. Each of these structural modifications induces a substantial shift in the host's conformational landscape, offering insights into the rational design of conformationally dynamic cages and enzymes. Although the thermodynamic properties of the dynamic Ga4L412- cage can be influenced by temperature, solvent, and guest binding, we find that conformational change occurs on a time scale that renders it rate-limiting in a model catalytic reaction, precluding rate enhancement through conformational selection. This concept is illustrated by locking the catalytically inactive conformer to a high-energy conformer that is catalytically competent. These findings demonstrate that precise modulation of the conformational landscape of supramolecular hosts provides an effective strategy for controlling their catalytic activity and binding.

Catalysis↗

DOE OSTI2022

Mitigation of Molten Salt Corrosion

The desire to increase the peak operational temperature of Concentrated Solar Power (CSP) plants to lower the levelized cost of CSP-derived electricity, has led to consideration of an earth-abundant, low-cost, thermally-stable, molten MgCl 2 -KCl-NaCl (40-40-20 mole%) salt for high-temperature thermal energy storage and heat transfer. The reliable, long-term containment of such a molten salt is challenging, however, due to the corrosion of cost-effective, high-temperature structural metal alloys in this salt (particularly if this salt is contaminated with oxygen-bearing species). This project has been focused on: i) development of equipment for evaluating corrosion kinetics in molten chlorides under well-controlled thermal, fluid dynamic, and atmospheric conditions at CSP-relevant temperatures, ii) use of such equipment to evaluate the influence of forced convection on corrosion kinetics (to determine the role of liquid phase diffusion on such corrosion), and iii) identifying a corrosion-mitigation strategy that can be industrially applied to achieve a projected annual corrosion ≤30 μm at CSP-relevant temperatures. The overall goals of this project have been: i) to understand the rate-limiting step(s) and associated kinetic laws governing corrosion in molten chlorides at 750°C, ii) to determine key operational parameters affecting the corrosion kinetics in molten salts, and iii) to demonstrate the tailoring of such parameters to appreciably reduce such corrosion.

14 SOLAR ENERGY↗

NASA NTRS1985

Development of a temperature-compensated hot-film anemometer system for boundary-layer transition detection on high-performance aircraft

A hot-film constant-temperature anemometer (CTA) system was flight-tested and evaluated as a candidate sensor for determining boundary-layer transition on high-performance aircraft. The hot-film gage withstood an extreme flow environment characterized by shock waves and high dynamic pressures, although sensitivity to the local total temperature with the CTA indicated the need for some form of temperature compensation. A temperature-compensation scheme was developed and two CTAs were modified and flight-tested on the F-104/Flight Test Fixture (FTF) facility at a variety of Mach numbers and altitudes, ranging from 0.4 to 1.8 and 5,000 to 40,000 ft respectively.

Chiles, H. R.↗

NASA NTRS1985

Development of a temperature-compensated hot-film anemometer system for boundary-layer transition detection on high-performance aircraft

Chiles, H. R.↗

DOE OSTI2020

Temperature dependence of nuclear quantum effects on liquid water via artificial neural network model based on SCAN meta-GGA functional

We investigate the temperature dependence of nuclear quantum effects (NQEs) on structural and dynamic properties of liquid water by training a neural network force field using first-principles molecular dynamics (FPMD) based on the strongly constrained and appropriately normed meta-generalized gradient approximation exchange-correlation approximation. The FPMD simulation based on density functional theory has become a powerful computational approach for studying a wide range of condensed phase systems. However, its large computational cost makes it difficult to incorporate NQEs in the simulation and investigate temperature dependence of various properties. To circumvent this difficulty, we use an artificial neural network model and employ the thermostatted ring polymer MD approach for studying the temperature dependence of NQEs on various properties. The NQEs generally bring the radial distribution functions closer to the experimental measurements. Translational diffusivity and rotational dynamics of water molecules are both slowed down by the NQEs. The competing inter-molecular and intra-molecular quantum effects on hydrogen bonds, as discussed by Habershon, Markland, and Manolopoulos [J. Chem. Phys. 131(2), 024501 (2019)], can explain the observed temperature dependence of the NQEs on the dynamical properties in our simulation.

Yao, Yi (ORCID:0000000299576979)↗

DOE OSTI2023

Topology induced crossover between Langevin, subdiffusion, and Brownian diffusion regimes in supercooled water

Despite extensive studies of supercooled water, it remains challenging to understand its peculiar dynamic anomalous properties. In this work, we integrated full atomistic simulations of supercooled water over the temperature range of room temperature to 200 K using a quantum-mechanics-based polarizable force field with the dressed dynamics method that couples fast collision events and slow reorganization dynamics of hydrogen-bond networks. Our analysis unveils the salient multiscale features in the transient relaxation dynamics of supercooled water. A classical Langevin behavior dominates at fast timescales, while long-time relaxations unveil two different activation barriers in two temperature regions: below and above 230 K. The modulation of the entropy spectrum by temperature is elucidated in terms of a three-state model underlined by the complexity of the water dynamics associated with a topological transition of a strong hydrogen-bond network. This state-dependent network topology is quantitatively characterized by power-law exponents of inverse network connectivity from 200 to 298 K. Finally, this work provides valuable guidance for further studies on the transient relaxation dynamics of supercooled water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗