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At least 1,117 records · Page 62
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Large Hyperfine Coupling Arising from Pseudo- 2 S Ground States in a Series of Lutetium(II) Metallocene Complexes

The synthesis of molecules with strong coupling between electronic and nuclear spins represents an important challenge in molecular quantum information science. Here, we report the synthesis and characterization of the divalent lutetium metallocene complexes Lu(Cp Me 5 )(Cp iPr 5 ) (Cp Me 5 = pentamethylcyclopentadienyl; Cp iPr 5 = pentaisopropylcyclopentadienyl), Lu(Cp iPr 4 Et ) 2 (Cp iPr 4 Et = ethyltetraisopropylcyclopentadienyl), and Lu(Cp iPr 4 ) 2 (Cp iPr 4 = tetraisopropylcyclopentadienyl). The molecular structures of these complexes, as determined through singlecrystal X-ray diffraction, feature a common bent sandwich geometry, with average Cp–Lu–Cp angles ranging from 159.9° to 152.6°. Analysis of continuous-wave electron paramagnetic resonance (EPR) spectra for the complexes reveals nearly isotropic g tensors with only a slight deviation from that of a free electron. Moreover, an extremely large splitting of the eight-line spectra indicates the presence of strong hyperfine coupling, and simulations provide isotropic hyperfine coupling constants of A iso = 4.38, 4.30, and 4.17 GHz across the series, where the value of A iso is found to decrease as the Cp–Lu–Cp angle becomes more acute. Notably, these values are the largest yet observed for any lanthanide complex. Moreover, EPR and computational analysis show that the large values of A iso stem from large s-orbital character up to 41.2% in the corresponding singly occupied molecular orbitals. To our knowledge, this degree of s-character in a molecular orbital is the largest yet reported for an open-shell isolable complex. These results outline a general strategy toward the isolation of paramagnetic molecules with strong hyperfine coupling and highly isotropic doublet electronic ground states.

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

Single-Electron Transfer Stabilizes Metastable Alane in a Bipyridine-Functionalized MOF Nanopore

Nanoconfinement of metastable hydrides such as alane (AlH 3 ) in functionalized porous frameworks represents a promising yet largely untapped strategy for high-capacity energy storage. Despite its potential, the underlying mechanisms responsible for the thermodynamic stabilization of metastable hydrides are poorly understood. Here, in this study, concepts from solution Lewis acid–base chemistry were applied to a crystalline metal–organic framework (MOF) to stabilize AlH 3 . The long-range order and synthetically versatile pore chemistry enabled us to reveal the intimate details of the hydride-host interactions. Powder X-ray diffraction (PXRD) of AlH 3 -infiltrated UiO-67bpy (Zr 6 O 4 (OH) 4 (bpydc) 6 ; bpydc 2– = 2,2′-bipyridine-5,5′-dicarboxylate) confirms that the framework maintains its crystallinity up to 250 °C and is stable under 70 MPa H 2 pressure. We find that thermodynamic stabilization arises from coupled single-electron and hydrogen-atom transfer from AlH 3 to bipyridine-containing linkers. Electron paramagnetic resonance detects a bipyridyl radical with an anisotropic g-tensor (g values of 2.00132, 2.00215, and 2.00275), consistent with Bader charge analysis predicting 0.82 e – transferred from the hydride to the MOF. These findings establish critical structure–property relationships underpinning AlH 3 stabilization and suggest general strategies for tuning the thermodynamics and kinetics of metastable materials.

Shivanna, Mohana [Sandia National Laboratories (SN↗
DOE OSTI2021

Unusual Seismic Signals in the Sevier Desert, Utah Possibly Related to the Black Rock Volcanic Field

Abstract On September 12, 2018 and April 14, 2019 shallow (<2.5 km from the surface, <1 km relative to sea level) earthquakes ( M w 4.0 and 4.1, respectively) struck a relatively aseismic area in south‐central Utah, within the Black Rock Desert volcanic field. Seismic waveforms are dominated by long‐period energy, no clear direct S‐wave arrivals, and signal durations of ∼100 s. Using co‐seismic interferograms, we detect clear and distinguishable surface deformation confirming the shallowness of the two mainshocks, while full moment tensor solutions rule out an isotropic source, such as an explosion or collapse. For the April 2019 sequence, we build an earthquake catalog using a dense temporary geophone array. The enhanced earthquake catalog shows a rapidly decaying aftershock sequence, with 85% of aftershocks occurring during the first three hours. Combining these observations, we argue that these earthquake sequences are related to the Black Rock Desert volcanic field.

Mesimeri, Maria↗
DOE OSTI2021

Laboratory Verification of Electron-Scale Reconnection Regions Modulated by a Three-Dimensional Instability

We report that during magnetic reconnection in collisionless space plasma, the electron fluid decouples from the magnetic field within narrow current layers, and theoretical models for this process can be distinguished in terms of their predicted current layer widths. From theory, the off-diagonal stress in the electron pressure tensor is related to the thermal noncircular orbit motion of electrons around the magnetic field lines. This stress becomes significant when the width of the reconnecting current layer approaches the small characteristic length scale of the electron motion. To aid in situ spacecraft and numerical investigations of reconnection, the structure of the electron diffusion region is here investigated using the Terrestrial Reconnection Experiment. In agreement with the closely matched kinetic simulations, laboratory observations reveal the presence of electron-scale current layer widths. Although the layers are modulated by a current-driven instability, three-dimensional simulations demonstrate that it is the off-diagonal stress that is responsible for breaking the frozen-in condition of the electron fluid.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

A Type–Curve Approach for Evaluating Aquifer Properties by Interpreting Shallow Strain Measured During Well Tests

Strains occur at shallow depths in response to pressure changes during well tests in an underlying aquifer, and recent developments in instrumentation have made it feasible to measure essentially the full strain tensor. Simulations using poroelastic analyses indicate that shallow normal strains are approximately proportional to the logarithm of time when a well is injecting into or pumping from a deep aquifer or reservoir. The drawdown is also a linear function of log time, as shown by the classic Cooper-Jacob type-curve analysis. The time when the semilog straight line intercepts the zero-strain axis is similar to the time determined from the Cooper-Jacob pressure analysis, and it can be used to estimate hydraulic diffusivity, suggesting that horizontal strain data can be used directly to estimate aquifer properties. This approach was validated using measurements from shallow (30-m deep) borehole strainmeters during an injection test at a 530-m-deep sandstone aquifer/reservoir in Oklahoma. The results show intercept times for the shallow normal strain data are essentially the same as for deep pressure data from an equivalent radial distance. The slopes of the semilog plots of the pressure and the strain increase at the same time, suggesting that they both respond to a lateral aquifer boundary. Significantly, though, strain was measured at shallow depths while the pressure data were measured at 530-m depth. This suggests that strain data from shallow depths could be an effective way to improve the characterization of an underlying aquifer.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Precursory Off-Fault Deformation in Restraining and Releasing Step Overs: Insights From Discrete Element Method Models

Accelerating geophysical activity is detected preceding some, but not all, large earthquakes. This observation may indicate that no precursors occur before some earthquakes, or that the instrumentation lacks the required sensitivity. Here, to aid crustal monitoring efforts, we use discrete element method models to identify the locations and styles of deformation that may provide useful information about approaching fault reactivation. We model the reactivation of two healed rough faults in a variety of step over configurations, embedded in a host rock with varying amounts of damage subject to shear velocity loading parallel to the faults. Both the fault geometry and ratio of fault to host rock strength control the amount of off-fault deformation. Consistent with field observations, models with larger steps and more preexisting host rock damage produce higher amounts of off-fault deformation. We assess the size of the continuous regions of high velocities and strains to compare the value of the precursory information of each velocity and strain component. Comparing the three components of the velocity vector suggests that the fault-parallel velocity produces the largest and most temporally continuous regions of elevated velocity. The size of these regions increases toward failure, indicating the usefulness of tracking this component. Comparing the volumetric and shear components of the three-dimensional strain tensor suggests that during most of the interseismic period, the shear strain provides more information about approaching fault slip than the volumetric strain. However, in the days and months preceding fault reactivation, both the shear and volumetric strains provide similarly valuable information.

58 GEOSCIENCES↗
DOE OSTI2022

WUS256: An Adjoint Waveform Tomography Model of the Crust and Upper Mantle of the Western United States for Improved Waveform Simulations

Abstract We report a new model (WUS256) of radially anisotropic seismic wavespeeds of the crust and upper mantle of the western United States (WUS) obtained from adjoint waveform tomography for the purpose of improving synthetic waveform fits to observed data. WUS256 is based on inversion of over 94,000 waveforms from 72 earthquakes recorded by nearly 3,400 stations. We started with the SPiRaL global model (Simmons et al., 2021, https://doi.org/10.1093/gji/ggab277 ) and waveforms in the period band of 50–120 s. We followed a conservative multiscale inversion approach with eight stages and 256 total inversion iterations which enabled monotonic misfit reduction to 20‐s minimum‐period waves. WUS256 relied on time‐frequency (TF) phase misfits and a trust region limited memory Broyden–Fletcher–Goldfarb–Shanno (L‐BFGS) optimization. Hessian‐vector products were used to qualitatively assess model resolution. Results indicate that WUS256 has good coverage of the continental regions to depths of about 150 km and is able to resolve features on lateral scales of about 200 km. We quantify waveform fits by the reduction in TF and normalized amplitude difference misfits between WUS256 and the SPiRaL starting model. WUS256 significantly improves waveform fits with misfit reduction 64% for both inversion and validation data sets compared to the SPiRaL starting model and shows even better fits compared to other models. Waveform fits illustrate that WUS256 reproduces body‐waves, fundamental mode surface waves as well as late arriving dispersed and/or scattered short period surface waves. The improvement in waveform fit indicates that WUS256 can be used to reproduce path effects on regional complete waveforms and moment tensor inversions.

58 GEOSCIENCES↗
DOE OSTI2023

Small-Magnitude Seismic Swarms in Central Utah (US): Interactions of Regional Tectonics, Local Structures and Hydrothermal Systems

Swarms in Central Utah are situated in the complex transition between the Basin and Range (BR) province and the Colorado Plateau. Transecting transverse structures, volcanic deposits, and hydrothermal systems complicate the extensional BR horst and graben structures and provide a multitude of plausible triggering mechanisms. Revisiting the catalog of the University of Utah Seismograph Stations (1981–2022), we analyze spatio-temporal patterns and characteristic features of seismic sequences. Swarms with alternating seismicity rates, bursts, and longer swarms with persistent moment release exhibit a remarkable diversity in temporal evolution. Swarm durations do not scale with cumulative seismic moment: swarms lasting less than 1 day can have similar cumulative seismic moments as month-long swarms. Here, we observe stationary swarms re-occurring for years (e.g., Mineral Mountains), as well as singular swarms in low-seismicity areas (e.g., activating a local structure). The swarms show a pronounced heterogeneity in triggering and driving mechanisms, observed in the detailed analysis of exemplary sequences (detections, relocations, moment tensors, waveform-based clustering, and repeater analysis). The 2022 Sevier Valley sequence activated a BR-related normal fault, the first resolved fault plane in the valley since 1983. The 2011 Circleville sequence is interpreted as a swarm triggered by mainshock-aftershock activity characterized by increasing magnitudes, changing rupture mechanisms, and a concentration of highly similar events in the second part of the sequence. By jointly discussing exemplary sequences and catalog statistics, we draw a comprehensive picture of swarm activity and its relation to geothermal and tectonic activity.

58 GEOSCIENCES↗
DOE OSTI2023

Enhanced Microseismicity During Production Pumping Cessation at the San Emidio Geothermal Field (Nevada, USA) in December 2016

Abstract Tectonic activity, geothermal fluids, and microseismic events (MSEs) tend to occur in similar locations as a result of spatiotemporal changes in the subsurface stress state. To quantify this association, we analyze data from a dense seismic array deployed at the San Emidio geothermal field, Nevada for 1 week in December 2016 to coincide with a 19.45‐hr shutdown of all injection and production pumping operations. 123 MSEs were detected, of which 101 occurred during the shutdown. The spatial association of the MSEs with the production wells suggests a causal relationship between the production cessation and the MSEs. Here we performed a detailed analysis to investigate reservoir material properties, distribution of seismically activated faults, and local stress state. We determined the hypocenters, magnitudes, and focal mechanisms for the MSEs, P‐wave tomographic velocity model, and local stress tensor. The results show that most MSEs occurred near the production wells. Magnitudes fall between −2.2 and 0.0 with larger events located closer to the production wells. Most MSEs occurred within a westward‐dipping normal fault zone in the reservoir associated with anomalously low P‐wave velocity values. The focal mechanism and stress inversion results show predominantly normal faulting with the maximum horizontal stress oriented north‐south. We suggest that the MSEs during shutdown were triggered on pre‐existing, small‐scale, critically stressed fault patches in the reservoir as the pore pressure increased around the production wells when the production pumping ceased. We interpret the larger MSE magnitudes closer to the production wells as a result of higher pore pressure increase.

15 GEOTHERMAL ENERGY↗
DOE OSTI2025

Crystallographic Texture, Structure, and Stress Transmission in Nugget Sandstone Examined With X‐Ray Tomography and Diffraction Microscopy

Subsurface processes in sandstones are controlled by porosity, permeability, and deformation mechanisms, all of which are controlled by a complex interplay of crystallographic rock texture, structure, and micromechanics. Texture, structure, and micromechanics have historically been studied using optical and electron microscopy of thin-sections. Here, we employed a new combination of in situ X-ray tomography and ray diffraction microscopy to study crystallographic texture, structure, and grain stresses in 3D. We examined these features in a sample of Nugget sandstone, a sandstone constituting hydrocarbon reservoirs across the American West. Our aims are threefold. First, we demonstrate the utility of X-ray diffraction microscopy probes for revealing texture, structure, and stress transmission in 3D. Second, we apply these techniques to Nugget sandstone and discuss findings in the context of prior work. Third, we study grain stress tensor evolution during mechanical compression to examine whether their heterogeneity and orientation evolution reflect that of inter-particle forces in granular materials. Our results show: (a) larger grains featured higher intra-granular misorientations, possibly from an increased prevalence of cements; (b) pores closed parallel to the loading direction and opened normal to loading; (c) grain stresses featured heterogeneity and orientations similar to inter-particle forces in non-cohesive granular materials; (d) grains featured compressive stresses in the loading direction and tensile stresses orthogonal to the loading direction, the latter resisting sample dilation and grain separation. Our work demonstrates the first known application of multi-modal X-ray tomography and diffraction microscopy to sandstone, providing new 3D insight into the nature of quartz cement and stress evolution.

high energy diffraction microscopy↗
DOE OSTI2026

Stress and Strain Heterogeneity and Persistence in Uniaxially‐ and Triaxially‐Loaded Sandstone

Two critical questions in brittle rock mechanics are how rocks developed localized strains and to what extent internal stress heterogeneity controls this localization and subsequent macroscopic failure. Definitive answers have not yet been found, but would provide insight into rock fracture mechanics as relevant to hydrocarbon extraction and sequestration. Here, we use synchrotron X‐ray tomography (XRT) and 3D X‐ray diffraction (3DXRD) during uniaxial and triaxial tests on Nugget and Bentheimer sandstones to examine strain and stress localization prior to mechanical failure. 3DXRD was used to measure intra‐granular lattice strains which were used to compute elastic stress tensors of each grain. Digital volume correlation (DVC) was applied to XRT images to determine the strain field in the sample. Both samples featured marked spatial heterogeneity, localization, and temporal persistence of elevated stresses and strains during their mechanical deformation toward failure. Both samples featured a majority of grains with at least one principal stress component that was tensile, a signature of the influence of heterogeneity on stress transmission. Measurements further revealed that compressive stress orientations and statistics evolved in a similar manner to those of inter‐particle forces in loose granular materials, with triaxially‐compressed rock exhibiting enhanced grain stress heterogeneity compared to uniaxially‐compressed rock. Our results complement recent work by others who employed XRT and scanning 3DXRD to study triaxially‐compressed sandstone, but extend those results to uniaxial compression, sandstones of varied porosity, and grain stress measurements throughout the 3D full extent of the samples rather than in a single layer examined with scanning 3DXRD.

58 GEOSCIENCES↗
DOE OSTI2026

Capturing Secondary Kinetic Instabilities in Three‐Dimensional Dayside Reconnection Using an Improved Gradient‐Based Closure

Magnetic reconnection is a highly dynamic process that excites a wide variety of kinetic waves and instabilities. Transverse current sheet instabilities such as the lower-hybrid drift and secondary drift-kink instabilities in particular have been shown by kinetic simulations to modify the reconnection and introduce significant turbulence and mixing to the reconnection layer. Past studies using the ten-moment fluid model to capture important kinetic physics such as the electron inertia and full representation of the pressure tensor proved advantageous to a two-fluid representation of reconnection, but the model struggled when using a local relaxation closure for the heat flux to replicate the current sheet instabilities and subsequent mixing seen in kinetic simulations. This work uses the Gkeyll software framework to perform simulations of asymmetric reconnection based on the 16 October 2015 MMS crossing of a diffusion region, the Burch event. An improved gradient-based heat flux closure is implemented, showing significant improvement in secondary kinetic instabilities that grow in the current sheet. These instabilities generate turbulence which leads to growth of secondary magnetic islands and flux ropes.

Bradshaw, K. [Princeton University, NJ (United Sta↗
DOE OSTI2021

Nanostructure-specific X-ray tomography reveals myelin levels, integrity and axon orientations in mouse and human nervous tissue

Myelin insulates neuronal axons and enables fast signal transmission, constituting a key component of brain development, aging and disease. Yet, myelin-specific imaging of macroscopic samples remains a challenge. Here, we exploit myelin’s nanostructural periodicity, and use small-angle X-ray scattering tensor tomography (SAXS-TT) to simultaneously quantify myelin levels, nanostructural integrity and axon orientations in nervous tissue. Proof-of-principle is demonstrated in whole mouse brain, mouse spinal cord and human white and gray matter samples. Outcomes are validated by 2D/3D histology and compared to MRI measurements sensitive to myelin and axon orientations. Specificity to nanostructure is exemplified by concomitantly imaging different myelin types with distinct periodicities. Finally, we illustrate the method’s sensitivity towards myelin-related diseases by quantifying myelin alterations in dysmyelinated mouse brain. This non-destructive, stain-free molecular imaging approach enables quantitative studies of myelination within and across samples during development, aging, disease and treatment, and is applicable to other ordered biomolecules or nanostructures.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Expanding the chemistry of borates with functional [BO 2 ]- anions

More than 3900 crystalline borates, including borate minerals and synthetic inorganic borates, in addition to a wealth of industrially-important boron-containing glasses, have been discovered and characterized. Of these compounds, 99.9 % contain only the traditional triangular BO 3 and tetrahedral BO 4 units, which polymerize into superstructural motifs. Herein, a mixed metal K 5 Ba 2 (B 10 O 17 ) 2 (BO 2 ) with linear BO 2 structural units was obtained, pushing the boundaries of structural diversity and providing a direct strategy toward the maximum thresholds of birefringence for optical materials design. 11 B solid-state nuclear magnetic resonance (NMR) is a ubiquitous tool in the study of glasses and optical materials; here, density functional theory-based NMR crystallography guided the direct characterization of BO 2 structural units. The full anisotropic shift and quadrupolar tensors of linear BO 2 were extracted from K 5 Ba 2 (B 10 O 17 ) 2 (BO 2 ) containing BO 2 , BO 3 , and BO 4 and serve as guides to the identification of this powerful moiety in future and, potentially, previously-characterized borate minerals, ceramics, and glasses.

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

Chiral structures of electric polarization vectors quantified by X-ray resonant scattering

Resonant elastic X-ray scattering (REXS) offers a unique tool to investigate solid-state systems providing spatial knowledge from diffraction combined with electronic information through the enhanced absorption process, allowing the probing of magnetic, charge, spin, and orbital degrees of spatial order together with electronic structure. A new promising application of REXS is to elucidate the chiral structure of electrical polarization emergent in a ferroelectric oxide superlattice in which the polarization vectors in the REXS amplitude are implicitly described through an anisotropic tensor corresponding to the quadrupole moment. Here, we present a detailed theoretical framework and analysis to quantitatively analyze the experimental results of Ti L-edge REXS of a polar vortex array formed in a PbTiO 3 /SrTiO 3 superlattice. Based on this theoretical framework, REXS for polar chiral structures can become a useful tool similar to x-ray resonant magnetic scattering (XRMS), enabling a comprehensive study of both electric and magnetic REXS on the chiral structures.

36 MATERIALS SCIENCE↗
DOE OSTI2022

E(3)-equivariant graph neural networks for data-efficient and accurate interatomic potentials

Abstract This work presents Neural Equivariant Interatomic Potentials (NequIP), an E(3)-equivariant neural network approach for learning interatomic potentials from ab-initio calculations for molecular dynamics simulations. While most contemporary symmetry-aware models use invariant convolutions and only act on scalars, NequIP employs E(3)-equivariant convolutions for interactions of geometric tensors, resulting in a more information-rich and faithful representation of atomic environments. The method achieves state-of-the-art accuracy on a challenging and diverse set of molecules and materials while exhibiting remarkable data efficiency. NequIP outperforms existing models with up to three orders of magnitude fewer training data, challenging the widely held belief that deep neural networks require massive training sets. The high data efficiency of the method allows for the construction of accurate potentials using high-order quantum chemical level of theory as reference and enables high-fidelity molecular dynamics simulations over long time scales.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Atomic-scale origin of the low grain-boundary resistance in perovskite solid electrolyte Li 0.375 Sr 0.4375 Ta 0.75 Zr 0.25 O 3

Oxide solid electrolytes (OSEs) have the potential to achieve improved safety and energy density for lithium-ion batteries, but their high grain-boundary (GB) resistance generally is a bottleneck. In the well-studied perovskite oxide solid electrolyte, Li 3x La 2/3-x TiO 3 (LLTO), the ionic conductivity of grain boundaries is about three orders of magnitude lower than that of the bulk. In contrast, the related Li 0.375 Sr 0.4375 Ta 0.75 Zr 0.25 O 3 (LSTZ0.75) perovskite exhibits low grain boundary resistance for reasons yet unknown. Here, we use aberration-corrected scanning transmission electron microscopy and spectroscopy, along with an active learning moment tensor potential, to reveal the atomic scale structure and composition of LSTZ0.75 grain boundaries. Vibrational electron energy loss spectroscopy is applied for the first time to reveal atomically resolved vibrations at grain boundaries of LSTZ0.75 and to characterize the otherwise unmeasurable Li distribution therein. We find that Li depletion, which is a major reason for the low grain boundary ionic conductivity of LLTO, is absent for the grain boundaries of LSTZ0.75. Instead, the low grain boundary resistivity of LSTZ0.75 is attributed to the formation of a nanoscale defective cubic perovskite interfacial structure that contained abundant vacancies. Our study provides new insights into the atomic scale mechanisms of low grain boundary resistivity.

25 ENERGY STORAGE↗
DOE OSTI2023

Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

Abstract Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and certain topological properties, such as the Berry curvature and the quantum metric tensor, have attracted considerable interest. Here, we report giant room-temperature nonlinearities in non-centrosymmetric two-dimensional topological materials—the Janus transition metal dichalcogenides in the 1 T’ phase, synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently show orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities in 1 T’ MoSSe (e.g., > 50 times higher than 2 H MoS 2 for 18 th order harmonic generation; > 20 times higher than 2 H MoS 2 for terahertz emission). We link this giant nonlinear optical response to topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and heralds the applications of topological materials in optoelectronics down to the monolayer limit.

42 ENGINEERING↗