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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Accelerating Quantum Materials Development with Advances in Transmission Electron Microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, superconductors, quantum dots, color center-hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, superconductivity, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the material’s detailed atomic-scale structure, including atomic defects, dopants, and lattice stacking. In this review, we describe how progress in the field of electron microscopy (EM), including in situ and in operando EM, can accelerate advances in quantum materials and quantum excitations. We begin by describing fundamental EM principles and operation modes. We then discuss various EM methods such as (i) EM spectroscopies, including electron energy loss spectroscopy (EELS), cathodoluminescence (CL), and electron energy gain spectroscopy (EEGS); (ii) four-dimensional scanning transmission electron microscopy (4D-STEM); (iii) dynamic and ultrafast EM (UEM); (iv) complementary ultrafast spectroscopies (UED, XFEL); and (v) atomic electron tomography (AET). We describe how these methods could inform structure–function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable precision positioning of atomic defects and high-resolution manipulation of quantum materials. For each method, we also describe existing limitations to solve open quantum mechanical questions, and how they might be addressed to accelerate progress. Among numerous notable results, our review highlights how EM is enabling identification of the 3D structure of quantum defects; measuring reversible and metastable dynamics of quantum excitations; mapping exciton states and single photon emission; measuring nanoscale thermal transport and coupled excitation dynamics; and measuring the internal electric field and charge density distribution of quantum heterointerfaces- all at the quantum materials’ intrinsic atomic and near atomic-length scale. Finally, we conclude by describing open challenges for the future, including achieving stable sample holders for ultralow temperature (below 10K) atomic-scale spatial resolution, stable spectrometers that enable meV energy resolution, and high-resolution, dynamic mapping of magnetic and spin fields. With atomic manipulation and ultrafast characterization enabled by EM, quantum materials will be poised to integrate into many of the sustainable and energy-efficient technologies needed for the 21st century.

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

Characterization of Two Positional Isomers of the Cs + Gly Complex Using Two-Color, IR–IR Photobleaching of the Cryogenically Cooled Ions

Metal ion binding to amino acid residues is an important interaction motif that controls the tertiary structures of oligopeptides. Analyses of the vibrational band patterns displayed by the amino acid scaffolds are commonly used to characterize the local docking motifs. Here we carry out two-color, IR-IR photobleaching measurements to obtain isomer-selective vibrational spectra of the Cs + Gly ion-molecule complex isolated in a cryogenically cooled, radiofrequency ion trap. The distinct band patterns of two non-interconverting isomers are observed and traced to different bidentate binding motifs between Cs + and the glycine scaffold. In one isomer, the ion attaches to the oxygen atoms of the carboxyl group whereas in the other it docks to the amino nitrogen and the carbonyl oxygen. Attachment to the acid head group yields a very diffuse absorption associated the OH group engaged in a strong intramolecular H-bond that closes a 5 membered ring. Furthermore, the band assignments, rearrangement pathways and electrostatic distortion of the electron density distributions in the glycine scaffold by the proximal ion are explored with electronic structure calculations and anharmonic theory.

Infrared spectroscopy↗
DOE OSTI2026

Surface Segregation of Liquid Metal Plasma-Facing Component Alloys: A ReaxFF Investigation

Engineering liquid metal alloys offers a transformative pathway for plasma-facing components by enabling chemically tailored surfaces that can simultaneously optimize plasma-material interactions, reduce divertor heat flux, and enhance core plasma confinement, thereby advancing the commercial viability of nuclear fusion power plants. This study, employing an atomistic simulation approach, provides direct evidence that incorporating nonmetal surface-active agents (such as O and H, or their combination) enables strong surface segregation. This capability makes tin−aluminum (Sn−Al) and tin−lithium (Sn−Li) alloys, with suitable compositions, good candidates for PFC applications. Specifically, the presence of low-Z solutes (Li, Al) leads to preferential surface enrichment, which imparts low-Z sputtering characteristics, while the Sn solvent maintains thermophysical stability. To systematically examine this behavior, we developed a ReaxFF force field spanning the full Sn/Al/Li/O/H chemistry, validated it against formation energies and elastic constants, and applied it in reactive molecular dynamics simulations at fusion-relevant temperatures. We also introduced an overlapbased segregation index that captures interfacial compositional separation directly from atomistic density distributions. Here, this metric reveals a clear hierarchy of segregation regimes and provides a unified view across all systems studied. Together, these findings establish a mechanistic link between nonmetal chemistry and interfacial structure, providing a predictive framework for designing self-adaptive, low-sputtering liquid metal alloys for fusion applications.

Alloys↗
DOE OSTI2021

Metastable Metallic Phase of a Bilayer Blue Phosphorene Induced by Interlayer Bonding and Intralayer Charge Redistributions

We have carried out diffusion Monte Carlo calculations for an A 1 B -1 -stacked bilayer blue phosphorene to find that it undergoes a semiconductor-metal transition as the interlayer distance decreases. While the most stable bilayer structure is a semiconducting one with two monolayers coupled through weak van der Waals interaction, the metallic bilayer at a shorter interlayer distance is found to be only metastable. This is in contrast to a recent theoretical prediction based on random phase approximation that the metallic phase would be the most stable bilayer configuration of blue phosphorene. Our analysis of charge density distributions reveals that the metastable metallic phase is induced by interlayer chemical bonding and intralayer charge redistributions. This study enriches our understanding of interlayer binding of a blue phosphorene and contributes to establishment of correct energetic order between its different phases, which will be essential in devising an experimental pathway for a metallic phosphorene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Spatial Mapping of Electrostatic Fields in 2D Heterostructures

In situ electron microscopy is an effective tool for understanding the mechanisms driving novel phenomena in 2D structures. However, due to practical challenges, it is difficult to address these technologically relevant 2D heterostructures with electron microscopy. Here, we use the differential phase contrast (DPC) imaging technique to build a methodology for probing local electrostatic fields during electrical operation with nanoscale spatial resolution in such materials. We find that, by combining a traditional DPC setup with a high-pass filter, we can largely eliminate electric fluctuations emanating from short-range atomic potentials. Using a method based on this filtering algorithm, a priori electric field expectations can be directly compared with experimentally derived values to readily identify inhomogeneities and potentially problematic regions. Furthermore, we use this platform to analyze the electric field and charge density distribution across layers of hBN and MoS 2 .

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Electron–Nuclear Dynamics Accompanying Proton-Coupled Electron Transfer

Although photoinduced proton-coupled electron transfer (PCET) plays an essential role in photosynthesis, a full understanding of the mechanism is still lacking due to the complex nonequilibrium dynamics arising from the strongly coupled electronic and nuclear degrees of freedom. Here we report the photoinduced PCET dynamics of a biomimetic model system investigated by means of transient IR and two-dimensional electronic–vibrational (2DEV) spectroscopies, IR spectroelectrochemistry (IRSEC), and calculations utilizing long-range-corrected hybrid density functionals. This collective experimental and theoretical effort provides a nuanced picture of the complicated dynamics and synergistic motions involved in photoinduced PCET. In particular, the evolution of the 2DEV line shape, which is highly sensitive to the mixing of vibronic states, is interpreted by accurate computational modeling of the charge separated state and is shown to represent a gradual change in electron density distribution associated with a dihedral twist that occurs on a 120 fs time scale.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Role of Ocean and Atmosphere Variability in Scale-Dependent Thermodynamic Air-Sea Interactions

This study investigates the influence of oceanic and atmospheric processes in extratropical thermodynamic air-sea interactions resolved by satellite observations (OBS) and by two climate model simulations run with eddy-resolving high-resolution (HR) and eddy-parameterized low-resolution (LR) ocean components. Here, in this work, spectral methods are used to characterize the sea surface temperature (SST) and turbulent heat flux (THF) variability and co-variability over scales between 50 and 10,000 km and 60 days to 80 years in the Pacific Ocean. The relative roles of the ocean and atmosphere are interpreted using a stochastic upper-ocean temperature evolution model forced by noise terms representing intrinsic variability in each medium, defined using climate model data to produce realistic rather than white spectral power density distributions. The analysis of all datasets shows that the atmosphere dominates the SST and THF variability over zonal wavelengths larger than ~2,000–2,500 km. In HR and OBS, ocean processes dominate the variability of both quantities at scales smaller than the atmospheric first internal Rossby radius of deformation (R 1 , ~600–2,000 km) due to a substantial ocean forcing coinciding with a weaker atmospheric modulation of THF (and consequently of SST) than at larger scales. The ocean forcing also induces oscillations in SST and THF with periods ranging from intraseasonal to multidecadal, reflecting a red spectrum response to ocean forcing similar to that driven by atmospheric forcing. Such features are virtually absent in LR due to a weaker ocean forcing relative to HR.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Incorporating the Effect of Large‐Scale Vertical Motion on Convection Through Convective Mass Flux Adjustment in E3SMv2

Abstract Recent observational studies suggest that the large‐scale dynamical forcing (vertical motion) plays important roles in deep convection development. In this study we propose a convective mass flux adjustment (MAdj) approach to represent the dynamical effects of large‐scale vertical motion on convection in the Department of Energy's Energy Exascale Earth System Model version 2 (E3SMv2). With MAdj, convection is enhanced (suppressed) when there is large‐scale ascending (descending) motion at the planetary boundary layer top. The coupling of convection with large‐scale circulation significantly improves the simulation of climate variability in E3SMv2 across multiple scales from the diurnal cycle, convectively coupled equatorial waves, to the Madden‐Julian Oscillation (MJO). The standard E3SMv2 tends to simulate overly weak diurnal amplitude of precipitation and overly weak variance of convectively coupled equatorial Kelvin and westward inertio‐gravity (WIG) waves. It also fails to simulate the essential characteristics of the MJO: continuous eastward propagation. With MAdj, the amplitude of diurnal cycle of precipitation is systematically increased and its probability density distribution is much closer to observations. The MAdj can also simulate more realistic eastward propagation of the MJO and much stronger convectively coupled Kelvin and WIG waves. Moreover, the MAdj approach slightly improves the climatology simulations in precipitation, cloud, radiation, circulation, temperature, and moisture fields, with overall root‐mean‐square error (RMSE) of major climatological fields reduced by about 2%. The MAdj approach suppresses excessive grid‐scale precipitation, reducing precipitation wet biases over South China Sea, Philippine Sea, Himalayas, and South Pacific Convergence Zone in western Pacific in summer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Observation of the molecular response to light upon photoexcitation

Abstract When a molecule interacts with light, its electrons can absorb energy from the electromagnetic field by rapidly rearranging their positions. This constitutes the first step of photochemical and photophysical processes that include primary events in human vision and photosynthesis. Here, we report the direct measurement of the initial redistribution of electron density when the molecule 1,3-cyclohexadiene (CHD) is optically excited. Our experiments exploit the intense, ultrashort hard x-ray pulses of the Linac Coherent Light Source (LCLS) to map the change in electron density using ultrafast x-ray scattering. The nature of the excited electronic state is identified with excellent spatial resolution and in good agreement with theoretical predictions. The excited state electron density distributions are thus amenable to direct experimental observation.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

A critical look at the prediction of the temperature field around a laser-induced melt pool on metallic substrates

The study of microstructure evolution in additive manufacturing of metals would be aided by knowing the thermal history. Since temperature measurements beneath the surface are difficult, estimates are obtained from computational thermo-mechanical models calibrated against traces left in the sample revealed after etching, such as the trace of the melt pool boundary. Here we examine the question of how reliable thermal histories computed from a model that reproduces the melt pool trace are. To this end, we perform experiments in which one of two different laser beams moves with constant velocity and power over a substrate of 17-4PH SS or Ti-6Al-4V, with low enough power to avoid generating a keyhole. We find that thermal histories appear to be reliably computed provided that (a) the power density distribution of the laser beam over the substrate is well characterized, and (b) convective heat transport effects are accounted for. Poor control of the laser beam leads to potentially multiple three-dimensional melt pool shapes compatible with the melt pool trace, and therefore to multiple potential thermal histories. Ignoring convective effects leads to results that are inconsistent with experiments, even for the mild melt pools here.

42 ENGINEERING↗
DOE OSTI2021

Influence of uranyl complexation on the reaction kinetics of the dodecane radical cation with used nuclear fuel extraction ligands (TBP, DEHBA, and DEHiBA)

Specialized extractant ligands – such as tri-butyl phosphate (TBP), N,N-di-(2-ethylhexyl)butyramide (DEHBA), and N,N-di-2-ethylhexylisobutryamide (DEHiBA) – have been developed for the recovery of uranium from used nuclear fuel by reprocessing solvent extraction technologies. These ligands must function in the presence of an intense multi-component radiation field, and thus it is critical that their radiolytic behaviour be thoroughly evaluated. This is especially true for their metal complexes, where there is negligible information on the influence of complexation on radiolytic reactivity, despite the prevalence of metal complexes in used nuclear fuel reprocessing solvent systems. Here we present a kinetic investigation into the effect of uranyl (UO 2 2+ ) complexation on the reaction kinetics of the dodecane radical cation (RH˙ + ) with TBP, DEHBA, and DEHiBA. Complexation had negligible effect on the reaction of RH˙ + with TBP, for which a second-order rate coefficient (k) of (1.3 ± 0.1) × 10 10 M -1 s -1 was measured. For DEHBA and DEHiBA, UO 2 2+ complexation afforded an increase in their respective rate coefficients: k(RH˙ + + [UO 2 (NO 3 ) 2 (DEHBA) 2 ]) = (2.5 ± 0.1) × 10 10 M -1 s -1 and k(RH˙ + + [UO 2 (NO 3 ) 2 (DEHiBA) 2 ]) = (1.6 ± 0.1) × 10 10 M -1 s -1 . This enhancement with complexation is indicative of an alternative RH˙ + reaction pathway, which is more readily accessible for [UO 2 (NO 3 ) 2 (DEHBA) 2 ] as it exhibited a much larger kinetic enhancement than [UO 2 (NO 3 ) 2 (DEHiBA) 2 ], 2.6× vs. 1.4×, respectively. Complementary quantum mechanical calculations suggests that the difference in reaction kinetic enhancement between TBP and DEHBA/DEHiBA is attributed to a combination of reaction pathway (electron/hole transfer vs. proton transfer) energetics and electron density distribution, wherein attendant nitrate counter anions effectively ‘shield’ TBP from RH˙ + electron transfer processes.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2022

Experimental demonstration of necessary conditions for X-ray induced synthesis of cesium superoxide

Absorption of sufficiently energetic X-ray photons by a molecular system results in a cascade of ultrafast electronic relaxation processes which leads to a distortion and dissociation of its molecular structure. Here, in this work, we demonstrate that only decomposition of powdered cesium oxalate monohydrate induced by monochromatic X-ray irradiation under high pressure leads to the formation of cesium superoxide. Whereas, for an unhydrated form of cesium oxalate subjected to the same extreme conditions, only degradation of the electron density distribution is observed. Moreover, the corresponding model of X-ray induced electronic relaxation cascades with an emphasis on water molecules’ critical role is proposed. Our experimental results suggest that the presence of water molecules in initially solid-state systems (i.e. additional electronic relaxation channels) together with applied high pressure (reduced interatomic/intermolecular distance) could potentially be a universal criteria for chemical and structural synthesis of novel compounds via X-ray induced photochemistry.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

A novel cosmic filament catalogue from SDSS data

Here, in this work, we present a new catalogue of cosmic filaments obtained from the latest Sloan Digital Sky Survey (SDSS) public data. In order to detect filaments, we implement a version of the Subspace-Constrained Mean-Shift algorithm that is boosted by machine learning techniques. This allows us to detect cosmic filaments as one-dimensional maxima in the galaxy density distribution. Our filament catalogue uses the cosmological sample of SDSS, including Data Release 16, and therefore inherits its sky footprint (aside from small border effects) and redshift coverage. In particular, this means that, taking advantage of the quasar sample, our filament reconstruction covers redshifts up to z = 2.2, making it one of the deepest filament reconstructions to our knowledge. We follow a tomographic approach and slice the galaxy data in 269 shells at different redshift. The reconstruction algorithm is applied to 2D spherical maps. The catalogue provides the position and uncertainty of each detection for each redshift slice. The quality of our detections, which we assess with several metrics, show improvement with respect to previous public catalogues obtained with similar methods. We also detect a highly significant correlation between our filament catalogue and galaxy cluster catalogues built from microwave observations of the Planck Satellite and the Atacama Cosmology Telescope.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

The Milky Way’s middle-aged inner ring

Aims. We investigate the metallicity, age, and orbital anatomy of the inner Milky Way, specifically focussing on the outer bar region. Methods. We integrated a sample of APOGEE DR16 inner Galaxy stars in a state of the art bar-bulge potential with a slow pattern speed and investigated the link between the resulting orbits and their [Fe/H] and ages. By superimposing the orbits, we built density, [Fe/H], and age maps of the inner Milky Way, which we divided further using the orbital parameters eccentricity, |Xmax|, and |Zmax|. Results. We find that at low heights from the Galactic plane, the Galactic bar gradually transitions into a radially thick, vertically thin, elongated inner ring with average solar [Fe/H]. This inner ring is mainly composed of stars with AstroNN ages between 4 and 9 Gyr with a peak in age between 6 and 8 Gyr, making the average age of the ring ~6 Gyr. The vertical thickness of the ring decreases markedly towards younger ages. We also find very large L4 Lagrange orbits that have average solar to super-solar metallicities and intermediate ages. Lastly, we confirm a clear X-shape in the [Fe/H] and density distributions at large Galactic heights. Conclusions. The orbital structure obtained for the APOGEE stars reveals that the Milky Way hosts an inner ring-like structure between the planar bar and corotation. This structure is on average metal rich, intermediately aged, and enhances the horizontal metallicity gradient along the bar’s major axis.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Iodine orbital moment and chromium anisotropy contributions to CrI 3 magnetism

The recent discovery of two-dimensional (2D) magnets, with a number of interesting magnetic properties, has drawn much interest due to their potential for future 2D spintronic device applications. CrI 3 , a van der Waals magnet, exhibits two-dimensional ferromagnetism even in monolayer form, stabilized by strong magnetic anisotropy. Its interlayer magnetic ordering is coupled to structural layer stacking, implying that the charge density distribution mediating van der Waals interactions plays a key role in the magnetic interaction between the layers. Using polarization-dependent x-ray spectroscopy, we investigated the response of the electronic environment around Cr and I sites to structural changes of layer stacking order. The highly anisotropic nature of the Cr local environment is significantly enhanced and is accompanied by changes in the valence band, in the rhombohedral phase. Magnetic spectroscopy measurements reveal a sizable iodine orbital moment, indicating the iodine contribution to magnetic anisotropy. Finally, our results uncover an important role for the extended nature of anisotropic Cr orbital states in dictating interlayer magnetic interactions and the iodine contribution to magnetic anisotropy.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Quantifying leakage fields at ionic grain boundaries using off-axis electron holography

The electrical properties of interfaces in semiconductors and ionic conductors are immensely important in a wide range of applications. Electron holography is ideally suited for the direct measurement of the electrostatic potential of such interfaces. A key challenge with this approach is the contribution of the leakage field from the sample to the observed electron phase shift. This leakage field cannot be a priori independently determined and can cause an overestimation of the phase shift. In this work, we use finite element simulations to compute the three-dimensional electrostatic potential in the vicinity of an interface associated with a given interfacial charge density distribution. We then evaluate the predicted phase shift and demonstrate that the leakage field strongly affects the recovery of the projected interface potential. From the difference between the true potential and uncorrected, recovered potential, we propose a method to correct for this effect. We then demonstrate the application of this methodology to the analysis of experimental off-axis electron holography data acquired from the grain boundaries in lightly doped ceria.

36 MATERIALS SCIENCE↗
DOE OSTI2021

The effect of areal density asymmetries on scattered neutron spectra in ICF implosions

Scattered neutron spectroscopy is a diagnostic technique commonly used to measure areal density in inertial confinement fusion experiments. Deleterious areal density asymmetries modify the shape of the scattered neutron spectrum. In this work, a novel analysis is developed, which can be used to fit the shape change. This will allow experimental scattered neutron spectroscopy to directly infer the amplitude and mode of the areal density asymmetries, with little sensitivity to confounding factors that affect other diagnostics for areal density. The model is tested on spectra produced by a neutron transport calculation with both isotropic and anisotropic primary fusion neutron sources. Multiple lines of sight are required to infer the areal density distribution over the whole sphere—we investigate the error propagation and optimal detector arrangement associated with the inference of mode 1 asymmetries.

Crilly, A. J. (ORCID:0000000204299332)↗