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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 1,369 records · Page 76
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Ultrafast Activation and Tuning of Topological Textures in Ferroelectric Nanostructures

Polar topological textures are recently discovered in ultra–thin ferroelectrics, including stripe, labyrinth, or bubble states. Enabling to shape on–demand, these topologies herein can provide an original platform for potential applications. Here, using first–principle–based calculations, it is shown that THz electric field pulses are an efficient means for generating a plethora of topological states in ultrathin films made by a prototypical ferroelectric system, depending on the characteristics of these pulses and films. Consequently, these ultrafast electrical pulses in ultra–thin ferroelectrics offer key ingredients for mimicking neuronal and synaptic behaviors, including all–optical devices, and open a new avenue for topological objects to neuromorphic systems.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Understanding Electrochemical Reaction Mechanisms of Sulfur in All‐Solid‐State Batteries through Operando and Theoretical Studies **

Abstract Due to its outstanding safety and high energy density, all‐solid‐state lithium‐sulfur batteries (ASLSBs) are considered as a potential future energy storage technology. The electrochemical reaction pathway in ASLSBs with inorganic solid‐state electrolytes is different from Li‐S batteries with liquid electrolytes, but the mechanism remains unclear. By combining operando Raman spectroscopy and ex situ X‐ray absorption spectroscopy, we investigated the reaction mechanism of sulfur (S 8 ) in ASLSBs. Our results revealed that no Li 2 S 8, Li 2 S 6, and Li 2 S 4 were formed, yet Li 2 S 2 was detected. Furthermore, first‐principles structural calculations were employed to disclose the formation energy of solid state Li 2 S n (1≤ n ≤8), in which Li 2 S 2 was a metastable phase, consistent with experimental observations. Meanwhile, partial S 8 and Li 2 S 2 remained at the full lithiation stage, suggesting incomplete reaction due to sluggish reaction kinetics in ASLSBs.

Cao, Daxian↗
DOE OSTI2023

Understanding Electrochemical Reaction Mechanisms of Sulfur in All‐Solid‐State Batteries through Operando and Theoretical Studies **

Abstract Due to its outstanding safety and high energy density, all‐solid‐state lithium‐sulfur batteries (ASLSBs) are considered as a potential future energy storage technology. The electrochemical reaction pathway in ASLSBs with inorganic solid‐state electrolytes is different from Li‐S batteries with liquid electrolytes, but the mechanism remains unclear. By combining operando Raman spectroscopy and ex situ X‐ray absorption spectroscopy, we investigated the reaction mechanism of sulfur (S 8 ) in ASLSBs. Our results revealed that no Li 2 S 8, Li 2 S 6, and Li 2 S 4 were formed, yet Li 2 S 2 was detected. Furthermore, first‐principles structural calculations were employed to disclose the formation energy of solid state Li 2 S n (1≤ n ≤8), in which Li 2 S 2 was a metastable phase, consistent with experimental observations. Meanwhile, partial S 8 and Li 2 S 2 remained at the full lithiation stage, suggesting incomplete reaction due to sluggish reaction kinetics in ASLSBs.

25 ENERGY STORAGE↗
DOE OSTI2025

Elucidating the Role of Electric Fields in Fe Oxidation via an Environmental Atom Probe

We quantify the effects of intensely applied electric fields on the Fe oxidation mechanism. The specimen are pristine Fe single crystals exposing a variety of surface structures identified by field ion microscopy. These crystals are simultaneously exposed to low pressures of pure oxygen gas, on the order of 10 −7 mbar, while applying intense electric fields on their surface of several tens of volts per nanometer. The local composition of the different surface structures is probed directly and in real time using an Environmental Atom Probe and successfully compared with first principles-based models. We found that rough Fe{244} and Fe{112} facets are more reactive toward oxygen than compact Fe{024} and Fe{011} facets. Results demonstrate that the influence of an electric field on the oxidation kinetics depends on the timescales that are involved as the system evolves toward equilibrium. The initial oxidation kinetics show that strong increases in electric fields facilitate the formation of an oxide. However, as one approaches equilibrium, high field values mitigate this formation. Ultimately, this study elucidates how high externally applied electric fields can be used to dynamically exploit reaction dynamics at the nanoscale towards desired products in a catalytic reaction at mild reaction conditions.

09 BIOMASS FUELS↗
DOE OSTI2025

Trade‐Off Between Toxicity and Efficiency in Tin‐ versus Lead‐Based Halide Perovskites

Toxicity remains one of the major challenges that prevent Pb-based halide perovskites from widespread utilization. Ideally, non-toxic alternatives can be identified while still maintaining the superior power conversion efficiency of the Pb-based perovskite solar cells. Using the currently most promising candidate, the Sn-based halide perovskites, as an example, we show that a trade-off exists between toxicity and efficiency in the Sn- versus Pb-based halide perovskites. Indeed, the dominant nonradiative recombination center in the Sn-based halide perovskites differs from the one in its Pb-based counterparts, resulting in the nonradiative capture coefficient in CsSnI 3 being an order of magnitude higher than that in CsPbI 3 . We attribute this difference to the band alignment. Here, our results indicate that development of halide perovskites beyond the Pb and Sn bases is essential for efficient yet environmentally friendly perovskite solar cells.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Will Nontoxic High‐Performance Perovskite Photovoltaics Ever Be Possible?

Lead-based halide perovskite solar cells represent a significant advancement in photovoltaic technology, achieving certified power conversion efficiencies of over 27%. However, the toxicity of lead poses a major barrier to widespread commercialization. The demand for environmentally safe alternatives has driven extensive research into Pb-free perovskites. Current efforts include replacing Pb with Sn or Ge; forming double perovskites in which Pb is substituted by a monovalent–trivalent cation pair; and developing chalcogenide perovskites where the B site (ABX 3 ) adopts tetravalent cations (rather than Pb) to balance the charge. This concept examines the recent progress in developing Pb-free alternatives, revealing fundamental performance bottlenecks, inherent material limitations, and persistent development challenges. Through a comparative assessment of material properties and device performance limitations, this work highlights the underlying dilemma between environmental safety and efficiency in perovskite photovoltaics. The analysis identifies fundamental material constraints that create substantial barriers to simultaneously achieving both objectives.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Dynamics of heavy quarks in strongly coupled $\mathcal{N}$ = 4 SYM plasma

We calculate the probability distribution P(k) for a heavy quark with velocity v propagating through strongly coupled N = 4 SYM plasma in the ’t Hooft limit (N c → ∞, λ = g 2 N c → ∞) at a temperature T to acquire a momentum k due to interactions with the plasma. This distribution encodes the well-known drag coefficient η D and the transverse and longitudinal momentum diffusion coefficients κ T and κ L . The jet quenching parameter $\hat{q}$ can be extracted from P(k) for v = 1. Going beyond these known Gaussian characteristics of P(k), our calculation determines all of the higher order and mixed moments to leading order in 1/$\sqrt{λ}$ for the first time. These non-Gaussian features of P(k) include qualitatively novel correlations between longitudinal energy loss and transverse momentum broadening at nonzero v. We show that all higher moments scale characteristically with an effective temperature of the boosted plasma in the heavy quark rest frame, and we demonstrate that these non-Gaussian characteristics can be sizable in magnitude and even dominant in physically relevant situations. We use these results to derive a Kolmogorov equation for the evolution of the probability distribution for the total momentum of a heavy quark that propagates through strongly coupled plasma. This evolution equation accounts for all higher order correlations between transverse momentum broadening and longitudinal energy loss, which we have calculated from first principles. It reduces to a Fokker-Planck equation when truncated to only include the effects of η D , κ T and κ L . Remarkably, while heavy quarks do not reach kinetic equilibrium with the plasma if evolved with this Fokker-Planck equation, by showing that the Boltzmann distribution is a static solution of the all-order Kolmogorov equation that we have derived we demonstrate that heavy quarks do reach kinetic equilibrium if evolved with this equation. Our results thus provide a dynamically complete framework for understanding the thermalization of a heavy quark that may be initially far from equilibrium in the strongly coupled N = 4 SYM plasma — as well as new insight into heavy quark transport and equilibration in quark-gluon plasma.

Holography and Hydrodynamics↗
DOE OSTI2023

Formation enthalpies of Al–Mn–Pd and the structure of the i-AlMnPd quasicrystal

Abstract This paper reports formation enthalpies of phases in the Al–Mn–Pd ternary alloy system as calculated from first principles using electronic density functional theory. We consider all crystal structures as reported in the assessed phase diagrams of the ternary and its binary alloy subsystems (Al–Mn, Al–Pd, and Mn–Pd), as well as additional reported or hypothetical structures. Icosahedral and decagonal quasicrystalline approximants are among the structures that we predict to be stable, or nearly so. Our results suggest the need for careful experimental reexamination of phase stability in each of the alloy systems, in tandem with further efforts to refine crystallographic and ab-initio structures.

17 WIND ENERGY↗
DOE OSTI2020

Solute-vacancy clustering in aluminum

In this study, we present an extensive first-principles database of solute-vacancy, homoatomic, heteroatomic solute-solute, and solute-solute-vacancy binding energies of relevant alloying elements in aluminum. We particularly focus on the systems with major alloying elements in aluminum, i.e., Cu, Mg, and Si. The computed binding energies of solute-vacancy, solute-solute pairs, and solute-solute-vacancy triplets agree with available experiments and theoretical results in literature. We consider physical factors such as solute size and formation energies of intermetallic compounds to correlate with binding energies. Systematic studies of the homoatomic solute-solute-vacancy and heteroatomic (Cu, Mg, or Si)-solute-vacancy complexes reveal the overarching effect of the vacancy in stabilizing solute-solute pairs. The binding energy database presented here elucidates the interaction between solute cluster and vacancy in aluminum, and it is expected to provide insight into the design of advanced Al alloys with tailored properties.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Tailoring microstructures with mild magnetic-field processing: A case study of CuNiFe alloys

Combined experimental and computational investigations of the CuNiFe spinodal system confirm that application of a mild magnetic field during thermal treatment alters elemental redistribution and the resulting microstructure, relative to that obtained from zero-field annealing. Spinodal decomposition of a Cu 40 Ni 42 Fe 18 alloy was initiated during thermal treatment at 773 K, conducted either under zero field or modest (60 mT) magnetic f ield conditions for up to 200 h. Periodic (~10 nm) chemical modulations into Cu-rich and NiFe-rich regions were observed under both conditions, with the amplitude and wavelength of the segregated regions increasing with treatment time. However, magnetic field annealing resulted in a more than twofold increase in the amplitude of elemental modulations relative to zero-field conditions – consistent with enhanced diffusional f luxes during spinodal decomposition – while the modulation wavelength remained largely unaffected. These microstructural differences are reflected in various extrinsic magnetic properties. In parallel, first-principles DFT calculations indicate that long-range ferromagnetic order, as induced by an applied magnetic field, substantially alters the strength and nature of atomic interactions, enhancing the thermodynamic instability of the CuNiFe solid solution. Collectively, these results suggest that incorporating a mild (millitesla-level) magnetic field – distinct from the strong (tesla-level) fields commonly used in prior studies – during thermal processing has the potential to deliver enhanced control of microstructures for targeted engineering outcomes.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Revisiting the SGTE lattice stability of bcc aluminum

The CALPHAD framework rests on the ability to assign well-defined free energies to all phases, including mechanically unstable ones. Given the experimental difficulties associated with the latter, researchers have turned to computational methods to obtain a theoretically justified definition of the free energy of mechanically unstable phases. Recently, a method called “inflection detection” has been shown to yield free energies that are broadly consistent with the current SGTE (Scientific Group Thermodata Europe) standard for pure elements, which were obtained through an extrapolation of stable solid solutions free energies towards unstable end members. Despite this general agreement, apparent failures for a few elements stand out, notably for the bcc–fcc enthalpy difference for the common element Al. Furthermore we revisit the definition of the bcc Al enthalpy and show that a careful CALPHAD-based analysis of enthalpy trends in five different mechanically stable binary solid solutions in fact does agree very well with the inflection-detection approach.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Resonant Raman in armchair graphene nanoribbons from first-principles

Resonant Raman spectra of armchair graphene nanoribbons (AGNRs) are computed using Density Functional Theory (DFT) and third-order perturbation theory. Results are benchmarked against available experimental data and compared to previously used theoretical approaches based on the Placzek approximation. Comparable agreement with experiments is found for both previously and presently used methods. In addition, a numerical analysis is carried out to provide a justification for the resonant modeling method based on the use of the frequency-dependent dielectric tensor in the Placzek approximation. Finally, this work also provides additional predictions and references for wide AGNRs that might be investigated with Raman scattering experiments in the future.

42 ENGINEERING↗
DOE OSTI2022

The impacts of charge transfer, localization, and metallicity on hydrogen retention and transport capacity

Solid state hydrides such as early transition metal hydrides are of inestimable importance for the future of hydrogen energy and are actively being investigated for energy conversion and storage applications such as fuel cells, solid-state batteries and neutron moderators. The retention and transport behavior of hydrogen in these hydrides has a huge role on the extended performance of components. While early transition-metal-based compounds exhibit many peculiar properties due to their unique correlated electronic signatures arising from -orbital electrons, the fundamental chemistry and transport behavior of hydrogen in such hydrides is not well understood. In the present work, using density functional theory, a highly intricate bonding feature is revealed through the theoretical investigation of the electronic structure of early transition metal hydrides YH 2 and ZrH 2 . In particular, a pronounced charge transfer from the transition element to H, results in localized electron densities at deep energy levels. The interplay between intrinsic charge transfer, charge localization, and metallicity in YH 2 and ZrH 2 leads to strong chemical bonding between metal and hydrogen atoms and large energy barriers for the migration of hydrogen vacancies. Specifically, hydrogen vacancies are found to be stable in the neutral state due to electron screening effects, accompanied by substantially high migration barriers between 0.8–1.2 eV along different crystallographic directions. In contrast, recent literature shows the migration barrier for charged H vacancies in insulating s-block metal hydrides lie between 0.1–0.4 eV, which is suitable for fast conduction applications. This pivotal electron structure difference exploited between early transition metal hydrides and alkali/alkaline earth metal hydrides determines extended hydrogen retention in these early transition metal hydrides. Finally, this work explains fundamental differences between the electronic structure of s-block and d-block metal hydrides, and its impact on the mobility of hydrogen vacancies.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2020

Interactions and immobilization of lanthanides with dopants in uranium-based metallic fuels

In uranium-based fuels, production and migration of lanthanide fission products and subsequent chemical interactions with cladding constituents lead to fuel–cladding chemical interaction (FCCI), limiting fuel performance. In general, dopant addition to the fuel matrix to arrest lanthanides within the fuel by forming intermetallics is found to be effective in mitigating FCCI. Recently, we proposed ab-initio based alloy-design principles, which can be useful in identifying dopant(s) that can bind a lanthanide (Nd) inside the fuel matrix. Here, we demonstrate the robustness of such principles by performing a systematic study to choose dopants to form compounds with a range of experimentally-observed lanthanide fission products. Results reveal that for a given dopant, lanthanide Ce and La exhibit similar behavior in their compound-forming tendencies compared to Nd and Pr, which is linked to lanthanide intrinsic characteristics such as the electronic configurations. Our predicted lanthanide-dopant intermetallic formation is verified experimentally in selective cases. Finally, we showed alloy design principles that accurately identify previously known dopants like Pd, and also predict new dopants As and Se, that can be effective in binding all lanthanides within the uranium matrix. Altogether, this research helps to develop generic alloy-design principles for complex multi-component systems based on lanthanide and dopant intrinsic characteristics.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗