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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 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Chemical Long-Range Disorder in Prussian Blue Analogues for Potassium Storage

Ordered Prussian blue analogues (PBAs) are vital cathode materials for ion storage, but strong interactions between the framework and host ions, especially large ions like K + , hinder ion migration, leading to poor diffusion kinetics and reduced reaction activity. Here, in this study, we present an approach to overcome this challenge by constructing chemical long-range disorder (LRD) in PBAs, involving maintaining inherent local coordination while introducing disorder over long-range spatial dimensions. Order control is achieved by introducing a large-sized lattice to disrupt the original lattice growth during synthesis. Unlike traditional monocrystalline particles, the abundant grain boundaries in the obtained LRD structure create significant potential fluctuations, generating additional electric fields that enhance ion transport. Furthermore, the short lattice coherence length reduces interaction between the framework and K + . These factors collectively contribute to the improved electrochemical activity of LRD PBAs during K + storage. This finding opens new avenues for designing PBA structures and offers insights into their structure-electrochemical performance relationship.

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

Ammonia Electrosynthesis from Nitrate Using a Ruthenium–Copper Cocatalyst System: A Full Concentration Range Study

Electrochemical synthesis of ammonia via the nitrate reduction reaction (NO3RR) has been intensively researched as an alternative to the traditional Haber–Bosch process. Most research focuses on the low concentration range representative of the nitrate level in wastewater, leaving the high concentration range, which exists in nuclear and fertilizer wastes, unexplored. The use of a concentrated electrolyte (≥1 M) for higher rate production is hampered by poor hydrogen transfer kinetics. Herein, we demonstrate that a cocatalytic system of Ru/Cu 2 O catalyst enables NO3RR at 10.0 A in 1 M nitrate electrolyte in a 16 cm 2 flow electrolyzer, with 100% faradaic efficiency toward ammonia. Detailed mechanistic studies by deuterium labeling and operando Fourier transform infrared (FTIR) spectroscopy allow us to probe the hydrogen transfer rate and intermediate species on Ru/Cu 2 O. Ab initio molecular dynamics (AIMD) simulations reveal that adsorbed hydroxide on Ru nanoparticles increases the density of the hydrogen-bonded water network near the Cu 2 O surface, which promotes the hydrogen transfer rate. Finally, our work highlights the importance of engineering synergistic interactions in cocatalysts for addressing the kinetic bottleneck in electrosynthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Framework Short-Range Order Observed in a Spinel-Type Li Superionic Conductor

Solid-state superionic conductors are characterized by rich structural disorders. Though structural complexities are central to their functionalities, they often give rise to short-range order that eludes detection by conventional diffraction-based techniques and is thus overlooked in establishing precise structure-property relationships. In this work, we synthesized single crystals of a recently discovered lithium (Li) superionic conductor Li16.2(1)In9.00(2)Sn1.10(1)O23.8 (LISO) for in-depth characterizations of structural subtleties. LISO exhibits an unusual spinel-like phase with significant Li overstoichiometry and a face-sharing Li network. Single-crystal neutron diffraction confirms significant Li disorder, as manifested in Li site splitting and partial occupancy. More importantly, synchrotron diffuse scattering combined with 3D-ΔPDF analysis and Monte Carlo simulations reveal short-range order in the nonalkali framework that might contribute to the phase stability and ionic conductivity. This work showcases an example in which subtle local energetics can be directly visualized in structurally disordered ionic conductors.

Chen, Yu↗
DOE OSTI2020

A Model for Turbulence Spectra in the Equilibrium Range of the Stable Atmospheric Boundary Layer

Stratification can cause turbulence spectra to deviate from Kolmogorov's isotropic -5/3 power law scaling in the universal equilibrium range at high Reynolds numbers. However, a consensus has not been reached with regard to the exact shape of the spectra. Here we propose a shape of the turbulent kinetic energy and temperature spectra in horizontal wavenumber for the equilibrium range that consists of three regimes at small Froude number: the buoyancy subrange, a transition region, and the isotropic inertial subrange through dimensional analysis and substantial revision of previous theoretical approximation. These spectral regimes are confirmed by various observations in the atmospheric boundary layer. The representation of the transition region in direct numerical simulations will require large-scale separation between the Dougherty-Ozmidov scale and the Kolmogorov scale for strongly stratified turbulence at high Reynolds numbers, which is still challenging computationally. In addition, we suggest that the failure of Monin-Obukhov similarity theory in the very stable atmospheric boundary layer is due to the fact that it does not consider the buoyancy scale that characterizes the transition region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Variations of Stress Parameters in the Southern California Plate Boundary Around the South Central Transverse Ranges

We examine the stress field in Southern California with a focus on the region near the South Central Transverse Ranges (SCTR), using a refined stress inversion methodology. We independently invert declustered and aftershocks focal mechanisms from the years 1981 to 2017. Comparisons between the stress field orientations and the stress ratios from these inversions provide information on local sources of the stress field. Regionally, the SHmax tends to be toward NNE and the stress ratios vary from transtensional stress regime near the Eastern California Shear Zone (ECSZ), to strike-slip faulting near the SCTR, and toward transpression near the Western Transverse Ranges. Detailed analysis of stress parameters near the SCTR indicates deviations from the regional strike-slip faulting including the following: (1) The San Bernardino Mountain area shows S Hmax direction toward NNW and transpressional stress components likely associated with the motions of the San Andreas Fault and ECSZ; (2) the Cajon Pass and San Gorgonio Pass show transpressional stress regime near the bottom of the seismogenic zone likely associated with the elevated topography; and (3) in Crafton Hills, rotation of the principal stress plunges and SHmax direction and transtensional stress regime below ~10 km, along with lower estimated apparent friction coefficient, suggest a weak fault possibly associated with deep creep. The performed multiscale analysis resolves effects of regional and local loadings. The average stress parameters in the analyzed 37 years do not show significant temporal variations of stress field near the SCTR region.

58 GEOSCIENCES↗
DOE OSTI2024

Assessment of Storm-Associated Precipitation and Its Extremes Using Observational Data Sets and Climate Model Short-Range Hindcasts

Heavy precipitation, often associated with weather phenomena such as tropical cyclones, extratropical cyclones (ETCs), atmospheric rivers (ARs), and mesoscale convective systems (MCSs), can cause significant socio-economic loss. Here, in this study, we apply atmospheric feature trackers to quantify the contributions of these storm types in observational data sets and climate model short-range hindcasts. We generate a global hourly storm data set at 0.25° spatial resolution covering 2006–2020, based on the tracking results from TempestExtremes and Python FLEXible object TRacKeR. Our analyses show that these four storm types account for 67% of global annual mean precipitation and 82% of top 1% precipitation extremes, with MCSs mainly over the tropics, and ARs and ETCs over the midlatitudes. The percentage of precipitation contributions from these storms also show strong seasonality over many geographical locations. We further apply the tracking results to the Energy Exascale Earth System Model (E3SM) short-range hindcasts and evaluate how well these storms are simulated. The evaluation show that E3SM, with ∼1° resolution, significantly underestimates storm-associated precipitation totals and extremes, especially for MCSs in the tropics. Our analysis also suggests that model fails to capture the correct mean diurnal phases and amplitude of MCS precipitation. This phenomenon-based approach provides a better understanding of precipitation characteristics and can lead to enhanced model evaluation by revealing underlying problems in model physics related to precipitation processes associated with the heavy-precipitating storms.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Long-range exciton diffusion in molecular non-fullerene acceptors

Abstract The short exciton diffusion length associated with most classical organic semiconductors used in organic photovoltaics (5-20 nm) imposes severe limits on the maximum size of the donor and acceptor domains within the photoactive layer of the cell. Identifying materials that are able to transport excitons over longer distances can help advancing our understanding and lead to solar cells with higher efficiency. Here, we measure the exciton diffusion length in a wide range of nonfullerene acceptor molecules using two different experimental techniques based on photocurrent and ultrafast spectroscopy measurements. The acceptors exhibit balanced ambipolar charge transport and surprisingly long exciton diffusion lengths in the range of 20 to 47 nm. With the aid of quantum-chemical calculations, we are able to rationalize the exciton dynamics and draw basic chemical design rules, particularly on the importance of the end-group substituent on the crystal packing of nonfullerene acceptors.

14 SOLAR ENERGY↗
DOE OSTI2021

Atomistic simulations of dislocation mobility in refractory high-entropy alloys and the effect of chemical short-range order

Abstract Refractory high-entropy alloys (RHEAs) are designed for high elevated-temperature strength, with both edge and screw dislocations playing an important role for plastic deformation. However, they can also display a significant energetic driving force for chemical short-range ordering (SRO). Here, we investigate mechanisms underlying the mobilities of screw and edge dislocations in the body-centered cubic MoNbTaW RHEA over a wide temperature range using extensive molecular dynamics simulations based on a highly-accurate machine-learning interatomic potential. Further, we specifically evaluate how these mechanisms are affected by the presence of SRO. The mobility of edge dislocations is found to be enhanced by the presence of SRO, whereas the rate of double-kink nucleation in the motion of screw dislocations is reduced, although this influence of SRO appears to be attenuated at increasing temperature. Independent of the presence of SRO, a cross-slip locking mechanism is observed for the motion of screws, which provides for extra strengthening for refractory high-entropy alloy system.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revealing the relationship between liquid fragility and medium-range order in silicate glasses

Despite decades of studies, the nature of the glass transition remains elusive. In particular, the sharpness of the dynamical arrest of a melt at the glass transition is captured by its fragility. Here, we reveal that fragility is governed by the medium-range order structure. Based on neutron-diffraction data for a series of aluminosilicate glasses, we propose a measurable structural parameter that features a strong inverse correlation with fragility, namely, the average medium-range distance (MRD). We use in-situ high-temperature neutron-scattering data to discuss the physical origin of this correlation. We argue that glasses exhibiting low MRD values present an excess of small network rings. Such rings are unstable and deform more readily with changes in temperature, which tends to increase fragility. These results reveal that the sharpness of the dynamical arrest experienced by a silicate glass at the glass transition is surprisingly encoded into the stability of rings in its network.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Giant uniaxial negative thermal expansion in FeZr 2 alloy over a wide temperature range

Negative thermal expansion (NTE) alloys possess great practical merit as thermal offsets for positive thermal expansion due to its metallic properties. However, achieving a large NTE with a wide temperature range remains a great challenge. Herein, a metallic framework-like material FeZr 2 is found to exhibit a giant uniaxial (1D) NTE with a wide temperature range (93-1078 K, $\overline{α}_{l}$=–34.01×10 –6 K –1 ). Such uniaxial NTE is the strongest in all metal-based NTE materials. The direct experimental evidence and DFT calculations reveal that the origin of giant NTE is the couple with phonons, flexible framework-like structure, and soft bonds. Interestingly, the present metallic FeZr 2 excites giant 1D NTE mainly driven by high-frequency optical branches. It is unlike the NTE in traditional framework materials, which are generally dominated by low energy acoustic branches. In the present study, a giant uniaxial NTE alloy is reported, and the complex mechanism has been revealed. It is of great significance for understanding the nature of thermal expansion and guiding the regulation of thermal expansion.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ubiquitous short-range order in multi-principal element alloys

Recent research in multi-principal element alloys (MPEAs) has increasingly focused on the role of short-range order (SRO) on material performance. However, the mechanisms of SRO formation and its precise control remain elusive, limiting the progress of SRO engineering. Here, leveraging advanced additive manufacturing techniques that produce samples with a wide range of cooling rates (up to 10 7 K s –1 ) and an enhanced semi-quantitative electron microscopy method, we characterize SRO in three CoCrNi-based face-centered-cubic (FCC) MPEAs. Surprisingly, irrespective of the processing and thermal treatment history, all samples exhibit similar levels of SRO. Atomistic simulations reveal that during solidification, prevalent local chemical order arises in the liquid-solid interface (solidification front) even under the extreme cooling rate of 10 11 K s –1 . This phenomenon stems from the swift atomic diffusion in the supercooled liquid, which matches or even surpasses the rate of solidification. Therefore, SRO is an inherent characteristic of most FCC MPEAs, insensitive to variations in cooling rates and even annealing treatments typically available in experiments.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Collective dynamics and long-range order in thermal neuristor networks

Abstract In the pursuit of scalable and energy-efficient neuromorphic devices, recent research has unveiled a novel category of spiking oscillators, termed “thermal neuristors.” These devices function via thermal interactions among neighboring vanadium dioxide resistive memories, emulating biological neuronal behavior. Here, we show that the collective dynamical behavior of networks of these neurons showcases a rich phase structure, tunable by adjusting the thermal coupling and input voltage. Notably, we identify phases exhibiting long-range order that, however, does not arise from criticality, but rather from the time non-local response of the system. In addition, we show that these thermal neuristor arrays achieve high accuracy in image recognition and time series prediction through reservoir computing, without leveraging long-range order. Our findings highlight a crucial aspect of neuromorphic computing with possible implications on the functioning of the brain: criticality may not be necessary for the efficient performance of neuromorphic systems in certain computational tasks.

Science & Technology - Other Topics↗
DOE OSTI2020

High-temperature short-range order in Mn 3 RhSi

Conventional phase transitions are well understood in terms of the order parameter, based on the Landau–Ginzburg–Wilson theory. However, unconventional magnetic orders have been observed in clean systems such as MnSi. The unconventional magnetic orders of conduction electrons in the metallic phase has been observed for high-temperature superconductors and heavy fermion compounds. However, these unconventional magnetic orders have been limited to relatively low temperatures as quantum phase transitions. Here high-temperature magnetic short-range order is observed as one of the unconventional magnetic orders at temperatures up to 720 K in a noncentrosymmetric intermetallic antiferromagnet Mn 3 RhSi with a well-ordered lattice. The magnetic Mn ions form a hyperkagome network of corner-sharing triangles, where the spins are geometrically frustrated. The spin network is equivalent to that of a spin liquid and non-Fermi-liquid material, β-Mn. Our observation indicates that a metallic phase with magnetic short-range order exists at high temperatures.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Origin of short- and medium-range order in supercooled liquid Ge 3 Sb 2 Te 6 from ab initio molecular dynamics simulations

Phase-change materials such as Ge–Sb–Te compounds have attracted much attention due to their potential value in electrical data storage. In contrast to the amorphous and crystalline phases, supercooled liquids are far from being deeply understood despite their inevitable role in both amorphization and crystallization processes. To this end, we have studied the dynamics properties and structural characteristics of liquid and supercooled liquid Ge 3 Sb 2 Te 6 during the fast cooling process. As the temperature decreases, chemical bonds become more homogeneous, but coordination numbers of Ge, Sb and Te atoms change very little. Meanwhile, the structural order of short-range configuration is obviously enhanced. Further studies suggest that Ge-centered, Sb-centered and Te-centered configurations change to the more ordered defective octahedrons mainly by adjusting the bond-angle relationship and bond length, rather than just by changing the coordination environment. It is the more ordered octahedrons that promote the formation of medium-range order. Our findings provide a deep insight into the origin of local structural order in supercooled liquid Ge 3 Sb 2 Te 6 , which is of great importance for the comprehensive understanding of amorphization and crystallization processes.

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

Simulation of the photodetachment spectra of the nitrate anion (NO 3 ₋ ) in the B ~ 2 E' energy range and non-adiabatic electronic population dynamics of NO 3

The photodetachment spectrum of the nitrate anion (NO 3 ₋ ) in the energy range of the NO 3 second excited state is simulated from first principles using quantum wave packet dynamics. The prediction at 10 K and 435 K relies on the use of an accurate full-dimensional fully coupled five state diabatic potential model utilizing an artificial neural network. The ability of this model to reproduce experimental spectra was demonstrated recently for the lower energy range. Analysis of the spectra indicates a weaker Jahn–Teller coupling compared to the first excited state. The detailed non-adiabatic dynamics is studied by computing the population dynamics. An ultra-fast non-statistical radiationless decay is found only among the Jahn–Teller components, which is followed by a slow statistical non-radiative decay among the different state manifolds. The latter is reproduced perfectly by a simple first order kinetics model. The dynamics in the second excited state is not affected by the presence of a conical intersection with the first excited state manifold.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Small angle X-ray studies of short-range order in non-stoichiometric pseudoprotic ionic liquids: the influence of chemical structure

Mixtures of organic acids and amines have been studied extensively owing to their unusual physicochemical properties and applications as solvents for extraction. In equimolar ratios they represent pseudoprotic ionic liquids, and in other, “nonstoichiometric” ratios they display a range of odd physicochemical behaviors. We report the results of small-angle X-ray scattering studies of a series of such systems with a range of chemical structures chosen to explore the link between molecular geometry and the character of the emergent nanoscale local liquid structure. We find that while the details vary, structure can emerge even when the hydrogen-bonding character of the components is changed significantly, and the character of their hydrocarbon substituents is altered. The consistent emergence of local order in the face of varying chemical structures indicates that the process is robust. Furthermore, this implies that the emergence of such structure may in fact be far more common in liquid mixtures than is currently recognized, and a great many structures may be suitable for the synthesis of pseudoprotic ionic liquids.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Infrared bands of neutral gas-phase carbon clusters in a broad spectral range

The identification of species in the interstellar medium requires precise and molecule-specific spectroscopic information in the laboratory framework, in broad spectral ranges and under conditions relevant to interstellar environments. In this work, we measure the gas-phase infrared spectra of neutral carbon clusters, C N (N = 6–11), in a molecular beam. The C N distribution is formed by photofragmentation of C 60 molecules, concurrently showing a top-down formation mechanism. A broad spectral range in the infrared between 500–3200 cm -1 (20–3.125 μm) is investigated. We observe strong bands between 5 and 6 μm, in conjunction with novel features in the 3 μm region. Density functional theory calculations reveal that these short wavelength modes correspond to combination bands with significant infrared intensity. Moreover, we identify the N ≤ 10 clusters as linear, while C 11 adopts a ring configuration, placing the linear-to-ring transition at N = 11 under our molecular beam conditions. The linearity of C 10 is discussed based on the formation pathway from larger clusters in energetic conditions. Given the vast and very precise infrared information already been released from the James Webb Space Telescope mission, this infrared spectroscopic data set in conjunction with information on formation mechanisms is of major relevance for identifying neutral carbon clusters in astronomical environments.

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

Range and strength of mechanical interactions of force dipoles in elastic fiber networks

Mechanical forces generated by myosin II molecular motors drive diverse cellular processes, most notably shape change, division and locomotion. These forces may be transmitted over long range through the cytoskeletal medium – a disordered, viscoelastic network of biopolymers. The resulting cell size scale force chains can in principle mediate mechanical interactions between distant actomyosin units, leading to self-organized structural order in the cell cytoskeleton. Inspired by such force transmission through elastic structures in the cytoskeleton, we consider a percolated fiber lattice network, where fibers are represented as linear elastic elements that can both bend and stretch, and the contractile activity of myosin motors is represented by force dipoles. Then, by using a variety of metrics, we show how two such contractile force dipoles interact with each other through their mutual mechanical deformations of the elastic fiber network. As a prelude to two-dipole interactions, we quantify how forces propagate through the network from a single anisotropic force dipole by analyzing clusters of nodes connected by highly strained bonds, as well as through the decay rate of strain energy with distance from a force dipole. We show that predominant fiber bending screens out force propagation, resulting in reduced and strongly network configuration-dependent dipole interactions. On the other hand, stretching-dominated networks support longer-ranged inter-dipole interactions that recapitulate the predictions of linear elasticity theory. By characterizing the differences between tensile and compressive force propagation in the fiber network, we show how inter-dipole interaction depends on the dipoles’ mutual separation and orientation. The resulting elastic interaction energy may mediate a force between multiple distant dipoles, leading to their self-organization into ordered configurations. In conclusion, this provides a potential pathway for active mechanical force-driven structural order in elastic biopolymer networks.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗