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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

PARTITIONING TUNGSTEN BETWEEN MATRIX PRECURSORS AND CHONDRULE PRECURSORS THROUGH RELATIVE SETTLING

Recent studies of chondrites have found a tungsten isotopic anomaly between chondrules and matrix. Given the refractory nature of tungsten, this implies that W was carried into the solar nebula by at least two distinct families of pre-solar grains. The observed chondrule/matrix split requires that the distinct families were kept separate during the dust coagulation process, and that the two families of grain interacted with the chondrule formation mechanism differently. We take the co-existence of different families of solids in the same general orbital region at the chondrule-precursor size as given, and explore the requirements for them to have interacted with the chondrule formation process at significantly different rates. We show that this sorting of families of solids into chondrule- and matrix-destined dust had to have been at least as powerful a sorting mechanism as the relative settling of aerodynamically distinct grains at least two scale heights above the midplane. The requirement that the chondrule formation mechanism was correlated in some fashion with a dust-grain sorting mechanism argues strongly for spatially localized chondrule formation mechanisms such as turbulent dissipation in non-thermally ionized disk surface layers, and argues against volume-filling mechanisms such as planetesimal bow shocks.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Cosmic Rays and Non-thermal Emission Induced by Accretion of Cool Gas onto the Galactic Disk

On both observational and theoretical grounds, the disk of our Galaxy should be accreting cool gas with temperature ≲10{sup 5} K via the halo at a rate ∼1 M{sub ⊙}yr{sup −1}. At least some of this accretion is mediated by high-velocity clouds (HVCs), observed to be traveling in the halo with velocities of a few 100 km s{sup −1} and occasionally impacting the disk at such velocities, especially in the outer regions of the Galaxy. We address the possibility of particle acceleration in shocks triggered by such HVC accretion events, and the detectability of consequent non-thermal emission in the radio to gamma-ray bands and high-energy neutrinos. For plausible shock velocities ∼300 km s{sup −1} and magnetic field strengths ∼0.3--10 μG, electrons and protons may be accelerated up to ∼1–10 TeV and ∼30--10{sup 3} TeV, respectively, in sufficiently strong adiabatic shocks during their lifetime of ∼10{sup 6} yr. The resultant pion decay and inverse Compton gamma-rays may be the origin of some unidentified Galactic GeV–TeV sources, particularly the “dark” source HESS J1503–582 that is spatially coincident with the anomalous H i structure known as “forbidden-velocity wings.” Correlation of their locations with star-forming regions may be weak, absent, or even opposite. Non-thermal radio and X-ray emission from primary and/or secondary electrons may be detectable with deeper observations. The contribution of HVC accretion to Galactic cosmic rays is subdominant, but could be non-negligible in the outer Galaxy. As the thermal emission induced by HVC accretion is likely difficult to detect, observations of such phenomena may offer a unique perspective on probing gas accretion onto the Milky Way and other galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2019

Design and analysis of machine learning exchange-correlation functionals via rotationally invariant convolutional descriptors

Here, we explore the potential of a data-driven approach to the design of exchange-correlation (xc) functionals. The approach, inspired by convolutional filters in computer vision and surrogate functions from optimization, utilizes convolutions of the electron density to form a feature space to represent local electronic environments and neural networks to map the features to the exchange-correlation energy density. These features are orbital free, and provide a systematic route to including information at various length scales. This work shows that convolutional descriptors are theoretically capable of an exact representation of the electron density, and proposes Maxwell-Cartesian spherical harmonic kernels as a class of rotationally invariant descriptors for the construction of machine learned functionals. The approach is demonstrated using data from the B3LYP functional on a number of small molecules containing C, H, O, and N along with a neural network regression model. The machine learned functionals are compared to standard physical approximations and the accuracy is assessed for the absolute energy of each molecular system as well as formation energies. The results indicate that it is possible to reproduce the exchange-correlation portion of B3LYP formation energies to within chemical accuracy using orbital-free descriptors with a spatial extent of 0.2 Å. The findings provide empirical insight into the spatial range of electron exchange, and suggest that the combination of convolutional descriptors and machine learning regression models is a promising framework for xc functional design, although challenges remain in obtaining training data and generating models consistent with pseudopotentials.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Unraveling sources of emission heterogeneity in Silicon Vacancy color centers with cryo-cathodoluminescence microscopy

Diamond color centers have proven to be versatile quantum emitters and exquisite sensors of stress, temperature, electric and magnetic fields, and biochemical processes. Among color centers, the silicon-vacancy (SiV - ) defect exhibits high brightness, minimal phonon coupling, narrow optical linewidths, and high degrees of photon indistinguishability. Yet the creation of reliable and scalable SiV - -based color centers has been hampered by heterogeneous emission, theorized to originate from surface imperfections, crystal lattice strain, defect symmetry, or other lattice impurities. Here, we advance high-resolution cryo-electron microscopy combined with cathodolumines cence spectroscopy and 4D scanning transmission electron microscopy (STEM) to elucidate the structural sources of heterogeneity in SiV - emission from nanodiamond with sub-nanometer-scale resolution. Our diamond nanoparticles are grown directly on TEM membranes from molecular-level seedings, representing the natural formation conditions of color centers in diamond. We show that individual subcrystallites within a single nanodiamond exhibit distinct zero-phonon line (ZPL) energies and differences in brightness that can vary by 0.1 meV in energy and over 70% in brightness. These changes are correlated with the atomic-scale lattice structure. We find that ZPL blue shifts result from tensile strain, while ZPL red shifts are due to compressive strain. We also find that distinct crystallites host distinct densities of SiV - emitters and that grain boundaries impact SiV - emission significantly. Finally, we interrogate nanodiamonds as small as 40 nm in diameter and show that these diamonds exhibit no spatial change to their ZPL energy. Our work provides a foundation for atomic-scale structure-emission correlation, e.g., of single atomic defects in a range of quantum and two-dimensional materials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Orbital-Selective Instabilities and Spin Fluctuations at the Verge of Superconductivity in Interlayer-Expanded Iron Selenide

Understanding electron correlation-driven instabilities and their coupling to structural phases is essential for deciphering multiorbital pairing in unconventional superconductors. We investigate Li x (C 5 H 5 N) y Fe 2 Se 2 (x ∼ 0.6; y ∼ 0.7−0.9), a tetragonal β-FeSe intercalate with a superconducting transition temperature (T c = 39 K) closely tied to an expanded Fe-layer spacing (∼11.4 Å). High-resolution synchrotron Xray diffraction and core-level absorption spectroscopy reveal subtle lattice distortions on cooling without a symmetry-breaking transition. Instead, the material exhibits negative thermal expansion (NTE) in the two-dimensional Fe network below T S ∼ 70 K, and stiffening of local Se−Fe−Se bond dynamics near T c . The spatially incoherent rearrangement of FeSe 4 tetrahedra and the site-local fluctuations, signal reduced electron correlations compared to those of parent β-FeSe (T c = 8 K). Complementary X-ray emission spectroscopy, a fast local probe of Fe 3d valence states, detects persistent local Fe spin moments below T S , unlike quenching in related systems. These findings indicate that decoupling of Fe planes leads to an electronically driven lattice instability. The latter emerges as NTE induced from weak, orbital-selective localization of in-plane Fe 3d states rather than conventional transverse vibrations. Governed by Hund’s coupling, this selectivity permits coexistence of local spin fluctuations with itinerant d-electrons critical for enhancing T c . These results suggest that intercalation-driven d-orbital differentiation moderates electron correlations, providing a pathway to optimize the superconductivity in low-dimensional quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2016

Millihertz quasi-periodic oscillations in 4U 1636-536: putting possible constraints on the neutron star size

Based on previous studies of quasi-periodic oscillations (QPOs) in neutron star (NS) low-mass X-ray binaries, mHz QPOs are believed to be related to “marginally stable” burning on the NS surface. Our study of phase-resolved energy spectra of these oscillations in 4U 1636–53 shows that the oscillations are not caused by variations in the blackbody temperature of the NS, but reveals a correlation between the change of the count rate during the mHz QPO pulse and the spatial extent of a region emitting blackbody emission. The maximum size of the emission area, R{sub BB}{sup 2}=216.7{sub −86.4}{sup +93.2} km{sup 2}, provides direct evidence that the oscillations originate from a variable surface area constrained on the NS and are therefore not related to instabilities in the accretion disk. The obtained lower limit on the size of the NS (11.0 km) rules out equations of state that prefer small NS radii. Observations of mHz QPOs in NS LMXBs with NICER and eXTP will reduce the statistical uncertainty in the lower limit on the NS radius, which together with better estimates of the hardening factor and distance, will allow for improved discrimination between different equations of state and compact star models. Furthermore, future missions will allow us to measure the peak blackbody emission area for a single mHz QPO pulse, which will push the lower limit to larger radii.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

WE-AB-BRA-06: 4DCT-Ventilation: A Novel Imaging Modality for Thoracic Surgical Evaluation

Purpose: The current standard-of-care imaging used to evaluate lung cancer patients for surgical resection is nuclear-medicine ventilation. Surgeons use nuclear-medicine images along with pulmonary function tests (PFT) to calculate percent predicted postoperative (%PPO) PFT values by estimating the amount of functioning lung that would be lost with surgery. 4DCT-ventilation is an emerging imaging modality developed in radiation oncology that uses 4DCT data to calculate lung ventilation maps. We perform the first retrospective study to assess the use of 4DCT-ventilation for pre-operative surgical evaluation. The purpose of this work was to compare %PPO-PFT values calculated with 4DCT-ventilation and nuclear-medicine imaging. Methods: 16 lung cancer patients retrospectively reviewed had undergone 4DCTs, nuclear-medicine imaging, and had Forced Expiratory Volume in 1 second (FEV1) acquired as part of a standard PFT. For each patient, 4DCT data sets, spatial registration, and a density-change based model were used to compute 4DCT-ventilation maps. Both 4DCT and nuclear-medicine images were used to calculate %PPO-FEV1 using %PPO-FEV1=pre-operative FEV1*(1-fraction of total ventilation of resected lung). Fraction of ventilation resected was calculated assuming lobectomy and pneumonectomy. The %PPO-FEV1 values were compared between the 4DCT-ventilation-based calculations and the nuclear-medicine-based calculations using correlation coefficients and average differences. Results: The correlation between %PPO-FEV1 values calculated with 4DCT-ventilation and nuclear-medicine were 0.81 (p<0.01) and 0.99 (p<0.01) for pneumonectomy and lobectomy respectively. The average difference between the 4DCT-ventilation based and the nuclear-medicine-based %PPO-FEV1 values were small, 4.1±8.5% and 2.9±3.0% for pneumonectomy and lobectomy respectively. Conclusion: The high correlation results provide a strong rationale for a clinical trial translating 4DCT-ventilation to the surgical domain. Compared to nuclear-medicine, 4DCT-ventilation is cheaper, does not require a radioactive contrast agent, provides a faster imaging procedure, and has improved spatial resolution. 4DCT-ventilation can reduce the cost and imaging time for patients while providing improved spatial accuracy and quantitative results for surgeons. YV discloses grant from State of Colorado.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2021

Mapping Molecular Adsorption Configurations with < 5 nm Spatial Resolution through Ambient Tip-Enhanced Raman Imaging

We interrogate para-mercaptobenzoic acid (MBA) molecules chemisorbed onto plasmonic silver nanocubes through tip-enhanced Raman (TER) spectral nano-imaging. Through a detailed examination of the spectra, aided by correlation analysis and density functional theory calculations, we find that MBA chemisorbs onto the plasmonic particles with at least two distinct configurations: S- and CO2-bound. High spatial resolution TER mapping allows us to distinguish between the distinct adsorption geometries with a pixel-limited (< 5 nm) spatial resolution under ambient laboratory conditions.

Gabel, Matthew L.↗
DOE OSTI2019

Theory of the spatial transfer of interface-nucleated changes of dynamical constraints and its consequences in glass-forming films

We formulate a new theory for how caging constraints in glass-forming liquids at a surface or interface are modified and then spatially transferred, in a layer-by-layer bootstrapped manner, into the film interior in the context of the dynamic free energy concept of the Nonlinear Langevin Equation (NLE) theory approach. The dynamic free energy at any mean location (cage center) involves contributions from two adjacent layers where confining forces are not the same. At the most fundamental level of the theory, the caging component of the dynamic free energy varies essentially exponentially with distance from the interface, saturating deep enough into the film with a correlation length of modest size and weak sensitivity to the thermodynamic state. This imparts a roughly exponential spatial variation of all the key features of the dynamic free energy required to compute gradients of dynamical quantities including the localization length, jump distance, cage barrier, collective elastic barrier, and alpha relaxation time. The spatial gradients are entirely of dynamical, not structural or thermodynamic, origin. The theory is implemented for the hard sphere fluid and diverse interfaces which can be a vapor, a rough pinned particle solid, a vibrating (softened) pinned particle solid, or a smooth hard wall. Their basic description at the level of the spatially heterogeneous dynamic free energy is identical, with the crucial difference arising from the first layer where dynamical constraints can be weakened, softened, or hardly changed depending on the specific interface. Numerical calculations establish the spatial dependence and fluid volume fraction sensitivity of the key dynamical property gradients for five different model interfaces. A comparison of the theoretical predictions for the dynamic localization length and glassy modulus with simulations and experiments for systems with a vapor interface reveals good agreement. Finally, the present advance sets the stage for using the Elastically Collective NLE theory to make quantitative predictions for the alpha relaxation time gradient, decoupling phenomena, T g gradient, and many film-averaged properties of both model and experimental (colloids, molecules, and polymers) systems with diverse interfaces and chemical makeup.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Experimental triplet and quadruplet fluctuation densities and spatial distribution function integrals for liquid mixtures

Kirkwood-Buff or Fluctuation Solution Theory can be used to provide experimental pair fluctuations, and/or integrals over the pair distribution functions, from experimental thermodynamic data on liquid mixtures. Here, this type of approach is used to provide triplet and quadruplet fluctuations, and the corresponding integrals over the triplet and quadruplet distribution functions, in a purely thermodynamic manner that avoids the use of structure factors. The approach is then applied to binary mixtures of water + methanol and benzene + methanol over the full composition range under ambient conditions. The observed correlations between the different species vary significantly with composition. The magnitude of the fluctuations and integrals appears to increase as the number of the most polar molecule involved in the fluctuation or integral also increases. A simple physical picture of the fluctuations is provided to help rationalize some of these variations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Exploring the Random Phase Approximation for Materials and Chemical Physics

In this work we test the performance of the fully nonlocal random phase approximation (RPA) for challenging problems in materials chemistry and physics. In this work we assessed the fully nonlocal random phase approximation (RPA) for the delicate energy differences of interest in materials chemistry and physics. The applications in this proposal are challenges for the simpler approximations of Kohn-Sham density functional theory, which are part of the current “standard model” for quantum chemistry and condensed matter physics. Direct RPA includes the full exact exchange energy and a nonlocal correlation energy from the occupied and unoccupied Kohn-Sham orbitals and orbital energies, with an approximate but universal description of long-range van der Waals attraction. RPA still cannot be a benchmark electronic structure method without a correction for its short-range correlation energy which is too deep. The short-range error of RPA can be corrected by a spatially nonlocal, exchange-only kernel. Such kernels could be a more reliable and “intrinsic” approximation to capture accurate ground-state energy differences than the expensive SOSEX and other beyond-RPA corrections. In this project we revealed the strengths and limitations of some model kernels through some materials problems focusing on structural phase transitions and transition metal chemistry. In addition we demonstrated the accuracy of the Renormalized RPA for total correlation energies of simple solids, and the pressure-induced phase transitions.

36 MATERIALS SCIENCE↗
DOE OSTI2014

FLUCTUATION DYNAMO AT FINITE CORRELATION TIMES AND THE KAZANTSEV SPECTRUM

Fluctuation dynamos are generic to astrophysical systems. The only analytical model of the fluctuation dynamo is the Kazantsev model which assumes a velocity field that is delta-correlated in time. We derive a generalized model of fluctuation dynamos with finite correlation time, τ, using renovating flows. For τ → 0, we recover the standard Kazantsev equation for the evolution of longitudinal magnetic correlation, M{sub L} . To the next order in τ, the generalized equation involves third and fourth spatial derivatives of M{sub L} . It can be recast to one with at most second derivatives of M{sub L} using the Landau-Lifschitz approach. Remarkably, we then find that the magnetic power spectrum remains the Kazantsev spectrum of M(k)∝k {sup 3/2}, in the large k limit, independent of τ.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2016

WE-H-207A-05: Spatial Co-Localization of F-18 NaF Vs. F-18 FDG Defined Disease Volumes

Purpose: Both [F-18]NaF and [F-18]FDG show promise for quantitative PET/CT assessment in metastatic prostate cancer to bone. Broad agreement between the tracers has been shown but voxel-wise correspondence has not been explored in depth. This study evaluates the spatial co-localization of [F-18]NaF PET and [F-18]FDG PET in bone lesions. Methods: Seventy-three lesion contours were identified in six patients receiving dynamic NaF PET/CT and FDG PET/CT scans two hours apart using identical fields-of-view. Tracer uptake (SUV) reflecting 60 minutes post-injection was modeled from kinetic parameters. Lesions were segmented by a physician separately on NaF PET and FDG PET. PET images were rigidly aligned using skeletal references on CT images. Lesion size, degree of overlap, voxel-wise tracer uptake values (SUV), and CT density distributions were compared using Dice coefficient, Positive Predictive Value (PPV), and Spearman rank correlation tests. Results: Across all patients, 42 lesions were identified on NaF PET (median 1.4 cm{sup 3}, range <1–204 cm{sup 3}) compared to 31 using FDG PET (median 1.8 cm{sup 3}, range <1–244 cm{sup 3}). Spatial cooccurrence was found in 25 lesion pairs. Lesions on NaF PET had PPV of 0.91 and on FDG a PPV of 0.65. Overall, NaF-defined lesions were 47% (±24%) larger by volume with moderate overlap to FDG, resulting in mean Dice coefficient of 34% (±22%). In areas of overlap, voxel-wise correlation of NaF and FDG SUV was moderate (ρ=0.56). Expanding to regions of non-spatial overlap, voxels contained in FDG-only contours were almost exclusively low HU (median 118), compared to dense regions of NaF-only voxels (median 250). In sclerotic sub-volumes (HU > 300) NaF-defined contours encompassed 83% of total FDG volume. Conclusion: Moderate voxel-wise correlation of FDG and NaF PET/CT uptake was observed. Spatial discrepancies in FDG and NaF PET/CT imaging of boney metastases could be influenced by poor sensitivity of FDG PET/CT in sclerotic regions. Funded by Prostate Cancer Foundation.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

Comparison of the results of refractometric measurements in the process of diffusion, obtained by means of the backgroundoriented schlieren method and the holographic interferometry method

The results of the study of interdiffusion of two liquids, obtained using the holographic recording scheme with a nonstationary reference wave with the frequency linearly varying in space and time are compared with the results of correlation processing of digital photographs, made with a random background screen. The spatio-temporal behaviour of the signal in four basic representations ('space – temporal frequency', 'space – time', 'spatial frequency – temporal frequency' and 'spatial frequency – time') is found in the holographic experiment and calculated (in the appropriate coordinates) based on the background-oriented schlieren method. Practical coincidence of the results of the correlation analysis and the holographic double-exposure interferometry is demonstrated. (interferometry)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2014

EXTENDED [C II] EMISSION IN LOCAL LUMINOUS INFRARED GALAXIES

We present Herschel/PACS observations of extended [C II] 157.7 μm line emission detected on ∼1-10 kpc scales in 60 local luminous infrared galaxies (LIRGs) from the Great Observatories All-sky LIRG Survey. We find that most of the extra-nuclear emission show [C II]/FIR ratios ≥4 × 10{sup –3}, larger than the mean ratio seen in the nuclei, and similar to those found in the extended disks of normal star-forming galaxies and the diffuse interstellar medium of our Galaxy. The [C II] ''deficits'' found in the most luminous local LIRGs are therefore restricted to their nuclei. There is a trend for LIRGs with warmer nuclei to show larger differences between their nuclear and extra-nuclear [C II]/FIR ratios. We find an anti-correlation between [C II]/FIR and the luminosity surface density, Σ{sub IR}, for the extended emission in the spatially resolved galaxies. However, there is an offset between this trend and that found for the LIRG nuclei. We use this offset to derive a beam filling-factor for the star-forming regions within the LIRG disks of ∼6% relative to their nuclei. We confront the observed trend to photo-dissociation region models and find that the slope of the correlation is much shallower than the model predictions. Finally, we compare the correlation found between [C II]/FIR and Σ{sub IR} with measurements of high-redshift starbursting IR-luminous galaxies.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Biotic predictors improve species distribution models for invasive plants in Western U.S. Forests at high but not low spatial resolutions

Invasions by non-native plants threaten forest health and sustainability. The ability to predict areas at greatest risk to invasion is essential for informing both monitoring and management of invasive species. Species distribution models (SDMs) are often used to identify environmental correlates of a species’ occurrence and predict geographic areas that may be suitable for its presence and are commonly constructed using solely abiotic predictors. However, mounting evidence implies that not including biotic predictors in SDMs may yield less accurate models at some resolutions typical of landscape-scale models, although this possibility has rarely been evaluated in invasive plants. In this study, we determined whether including descriptors of the biotic environment improved the accuracy of SDMs built at five decreasing spatial resolutions for infestations of five common invasive plants in forests of California, Oregon, and Washington, USA and described environmental correlates of each species’ presence. Predictors of occurrence often echoed those identified in previous studies of the focal species, indicating that our models accurately identified important environmental drivers of occurrence. Including biotic predictors in the SDMs consistently improved model accuracy only at the highest resolution we examined, which may be due to the spatial scale at which biotic interactions primarily act to constrain species’ distributions, the particular biotic predictors we used in our models, or correlations between attributes of the abiotic and biotic environment. This finding suggests that, while the practice of building SDMs using abiotic predictors alone may generally yield models whose accuracy does not differ substantially from those that also include biotic predictors, the effects of biotic interactions on the distribution of invasive plants in forests may be detectable at larger scales than previously thought.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2015

Orientation gradients in relation to grain boundaries at varying strain level and spatial resolution

The resolution dependence of orientation gradients was studied in a well-annealed 99.9995% pure polycrystalline copper pulled to failure in tension. Owing to the well developed neck, different regions in the sample correspond to different tensile strains. Post-mortem characterization was performed using EBSD on cross-sections containing the tensile axis. Kernel average misorientation (KAM) was calculated as a metric to establish correlation between defect accumulation and microstructural features, with a threshold of 5° to focus on intra-granular gradients. The region with the lowest strain (2%) showed high KAM values adjacent to grain boundaries compared to the grain interior, regardless of the point spacing, i.e. the spatial resolution. However, in the region with the highest strain (13%) a strong dependence on resolution was found. For point spacings of 0.5 μm or smaller, the same correlation of high KAM with locations near boundaries was found. At coarse spacings i.e. low spatial resolution, by contrast, the reverse was found in that the highest KAM values appear in the grain interiors, as previously observed in X-ray microscopy on the same sample which had a similar coarse resolution. An analysis of orientation gradients parallel to, and perpendicular to boundaries suggested that the latter tend to be the larger of the two. This helps to explain why boundary-adjacent points have low KAM values. The conclusion is that measurement of local orientation gradient requires a resolution that is comparable to the dislocation substructure.

36 MATERIALS SCIENCE↗