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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Substantial oxygen loss and chemical expansion in lithium-rich layered oxides at moderate delithiation

Delithiation of layered oxide electrodes triggers irreversible oxygen loss, one of the primary degradation modes in lithium-ion batteries. However, the delithiation-dependent mechanisms of oxygen loss remain poorly understood. Here we investigate the oxygen non-stoichiometry in Li 1.18–x Ni 0.21 Mn 0.53 Co 0.08 O 2–δ electrodes as a function of Li content by using cycling protocols with long open-circuit voltage steps at varying states of charge. Surprisingly, we observe substantial oxygen loss even at moderate delithiation, corresponding to 2.5, 4.0 and 7.6 ml O 2 per gram of Li 1.18–x Ni 0.21 Mn 0.53 Co 0.08 O 2–δ after resting at upper capacity cut-offs of 135, 200 and 265 mAh g −1 for 100 h. Our observations suggest an intrinsic oxygen instability consistent with predictions of high oxygen activity at intermediate potentials versus Li/Li + . In addition, we observe a large chemical expansion coefficient with respect to oxygen non-stoichiometry, which is about three times greater than those of classical oxygen-deficient materials such as fluorite and perovskite oxides. Furthermore, our work challenges the conventional wisdom that deep delithiation is a necessary condition for oxygen loss in layered oxide electrodes and highlights the importance of calendar ageing for investigating oxygen stability.

Atomistic models↗
DOE OSTI2023

An open database of computed bulk ternary transition metal dichalcogenides

Abstract We present a dataset of structural relaxations of bulk ternary transition metal dichalcogenides (TMDs) computed via plane-wave density functional theory (DFT). We examined combinations of up to two chalcogenides with seven transition metals from groups 4–6 in octahedral (1T) or trigonal prismatic (2H) coordination. The full dataset consists of 672 unique stoichiometries, with a total of 50,337 individual configurations generated during structural relaxation. Our motivations for building this dataset are (1) to develop a training set for the generation of machine and deep learning models and (2) to obtain structural minima over a range of stoichiometries to support future electronic analyses. We provide the dataset as individual VASP xml files as well as all configurations encountered during relaxations collated into an ASE database with the corresponding total energy and atomic forces. In this report, we discuss the dataset in more detail and highlight interesting structural and electronic features of the relaxed structures.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Quantum mechanical dataset of 836k neutral closed-shell molecules with up to 5 heavy atoms from C, N, O, F, Si, P, S, Cl, Br

Abstract We introduce the Vector-QM24 (VQM24) dataset comprehensively covering all possible neutral closed-shell small organic and inorganic molecules with up to five heavy (p-block) atoms: C, N, O, F, Si, P, S, Cl, Br. All valid stoichiometries, Lewis-rule-consistent graphs, and stable conformers (identified via GFN2-xTB) were enumerated combinatorially, yielding 577k conformational isomers spanning 258k constitutional isomers and 5,599 unique stoichiometries. DFT (ωB97X-D3/cc-pVDZ) optimizations were performed for all, and diffusion quantum Monte Carlo (DMC@PBE0(ccECP/cc-pVQZ)) energies are provided for 10,793 lowest-energy conformers with up to 4 heavy atoms. VQM24 includes structures, vibrational modes, rotational constants, thermodynamic properties (Gibbs free energies, enthalpies, ZPVEs, entropies, heat capacities), and electronic properties such as atomization, electron interaction, exchange-correlation, dispersion energies, multipole moments (dipole to hexadecapole), alchemical potentials, Mulliken charges, and wavefunctions. Machine learning models of atomization energies on this dataset reveal significantly higher complexity than QM9, with none achieving chemical accuracy. VQM24 offers a rigorous, high-fidelity benchmark for evaluating quantum machine learning models.

Science & Technology - Other Topics↗
DOE OSTI2020

Synthesis, transport properties and electronic structure of p-type Cu 1+x Mn 2–x InTe 4 ( x = 0, 0.2, 0.3)

The synthesis, electronic structure and temperature dependent transport properties of polycrystalline Cu 1+x Mn 2–x InTe 4 (x = 0, 0.2, 0.3) are reported for the first time. These quaternary chalcogenides were synthesized by direct reaction of the elements, followed by solid state annealing and hot press densification. The thermal conductivity is low for all specimens and intrinsic to the material system. Furthermore, the off-stoichiometry specimens illustrate the sensitivity of the transport properties to stoichiometry, with a greater than two-orders-of magnitude increase in carrier concentration with increased Cu content. First principles calculations of the electronic structure are also reported, and are in agreement with the experimental data. Here, this fundamental investigation shows the potential towards further optimization of the electrical properties that, in addition to the intrinsically low thermal conductivity, provides a basis for further research into the viability of this material system for potential energy-related applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Combinatorial investigation of structural and optical properties of cation-disordered ZnGeN 2

Cation-disordered ZnGeN 2 shows promise for application as a blue-green emitter in light-emitting devices, but more foundational work is necessary to understand structure–property relationships. In this work, we present a combinatorial exploration of the experimental phase space of wurtzite (cation-disordered) ZnGeN 2 using high-throughput co-sputtering. Structure, morphology and optical properties are explored as a function of cation composition and synthesis temperature. ZnGeN 2 is found to crystallize in the wurtzite structure ranging from Zn-rich to Ge-rich compositions. X-ray diffraction refinements reveal a continuous shift in cell volume with off-stoichiometry, indicating alloy-like structural behavior. Furthermore, the optical absorption of all films examined is lower in energy than the value predicted for cation-ordered ZnGeN 2 , suggesting that cation disorder is decreasing the bandgap. Additionally, the absorption threshold shifts continuously to higher energy for Ge-rich samples, consistent with bandgap shifts due to alloy-like structural behavior. Defect formation energy diagrams are calculated to help guide understanding of off-stoichiometry from a defect complex perspective. This work paves the way toward use of ZnGeN 2 as a bandgap-tunable optoelectronic semiconductor.

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

Mechanistic studies of NH 3 -assisted reduction of mononuclear Cu(ii) cation sites in Cu-CHA zeolites

Cu-Exchanged zeolites catalyze various redox reactions including the selective catalytic reduction (SCR) of NO x with NH 3 and the partial oxidation of hydrocarbons. The reduction of Cu(II) cations to Cu(I) by NH 3 alone has been observed experimentally, yet fundamental details regarding the Cu active site requirements, reaction stoichiometry, and reaction mechanism remain incompletely understood. Here, we synthesized model Cu-exchanged chabazite (Cu-CHA) zeolites with varying Cu ion densities and distributions of mononuclear Cu(II) ion site types (Cu 2+ , (CuOH) + ) and studied NH 3 -assisted Cu(II) reduction reactions using a combination of spectroscopic, titrimetric, and gas-phase product analysis methods. In situ UV-visible and X-ray absorption spectroscopies were used to monitor and quantify the transient reduction of Cu(II) to Cu(I) during exposure to NH 3 (473 K), in concert with titration methods that use NO and NH 3 co-reductants to fully reduce to the Cu(I) state any residual Cu(II) ions that remained after treatments in NH 3 alone for a given time period. The techniques provide quantitative evidence that both mononuclear Cu(II) site types are able to reduce in NH 3 alone, and do so to similar extents as a function of time. NH 3 temperature programmed reduction (TPR) revealed that the reaction stoichiometry of NH 3 -assisted reduction forms approximately one equivalent of N 2 per 6 Cu sites, regardless of Cu speciation or density, consistent with a six-electron reduction process whereby two NH 3 molecules react with six Cu(II) species to produce one N 2 molecule and six Cu(I) species. Furthermore, these findings provide new insights into the reaction pathways and mechanisms by which NH 3 alone reduces mononuclear Cu(II) sites in zeolites, which are undesired side-reactions that occur during steady-state NO x SCR and can unintentionally influence SCR-relevant spectroscopic or titrimetric characterization experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Application of machine learning to discover new intermetallic catalysts for the hydrogen evolution and the oxygen reduction reactions

The adsorption energies for hydrogen, oxygen, and hydroxyl were calculated by means of density functional theory on the lowest energy surface of 24 pure metals and 332 binary intermetallic compounds with stoichiometries AB, A 2 B, and A 3 B taking into account the effect of biaxial elastic strains. This information was used to train two random forest regression models, one for the hydrogen adsorption and another for the oxygen and hydroxyl adsorption, based on 9 descriptors that characterized the geometrical and chemical features of the adsorption site as well as the applied strain. All the descriptors for each compound in the models could be obtained from physico-chemical databases. The random forest models were used to predict the adsorption energy for hydrogen, oxygen, and hydroxyl of ≈2700 binary intermetallic compounds with stoichiometries AB, A 2 B, and A 3 B made of metallic elements, excluding those that were environmentally hazardous, radioactive, or toxic. This information was used to search for potential good catalysts for the HER and ORR from the criteria that their adsorption energy for H and O/OH, respectively, should be close to that of Pt. Further, this investigation shows that the suitably trained machine learning models can predict adsorption energies with an accuracy not far away from density functional theory calculations with minimum computational cost from descriptors that are readily available in physico-chemical databases for any compound. Moreover, the strategy presented in this paper can be easily extended to other compounds and catalytic reactions, and is expected to foster the use of ML methods in catalysis.

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

Precipitation of dopants on acceptor-doped LaMnO3±δ revealed by defect chemistry from first principles

Perovskite oxides degrade at elevated temperatures while precipitating dopant-rich particles on the surface. A knowledge-based improvement of surface stability requires a fundamental and quantitative understanding of the dopant precipitation mechanism on these materials. We propose that dopant precipitation is a consequence of the variation of dopant solubility between calcination and operating conditions in solid oxide fuel cells (SOFCs) and electrolyzer cells (SOECs). To study dopant precipitation, we use 20% (D = Ca, Sr, Ba)-doped LaMnO3+δ (LDM20) as a model system. We employ a defect model taking input from density functional theory calculations. The defect model considers the equilibration of LDM20 with a reservoir consisting of dopant oxide (DO), peroxide (DO2), and O2 in the gas phase. The equilibrated non-stoichiometry of the A-site and B-site as a function of temperature, T, and oxygen partial pressure, p(O2), reveals three regimes for LDM20: A-site deficient (oxidizing conditions), A-site rich (atmospheric conditions), and near-stoichiometric (reducing conditions). Assuming an initial A/B non-stoichiometry, we compute the dopant precipitation boundaries in a p–T phase diagram. Our model predicts precipitation both under reducing (DO) and under highly oxidizing conditions (DO2). We found precipitation under anodic, SOEC conditions to be promoted by large dopant size, while under cathodic, SOFC conditions precipitation is promoted by initial A-site excess. The main driving forces for precipitation are oxygen uptake by the condensed phase under oxidizing conditions and oxygen release assisted by B-site vacancies under reducing conditions. Possible strategies for mitigating dopant precipitation under in electrolytic and fuel cell conditions are discussed.

Hess, Franziska (ORCID:000000024460643X)↗
DOE OSTI2021

Improved control of atomic layering in perovskite-related homologous series

Homologous series are layered phases that can have a range of stoichiometries depending on an index n. Examples of perovskite-related homologous series include (ABO 3 )nAO Ruddlesden–Popper phases and (Bi 2 O 2 ) (A n-1 B n O 3n+1 ) Aurivillius phases. It is challenging to precisely control n because other members of the homologous series have similar stoichiometry and a phase with the desired n is degenerate in energy with syntactic intergrowths among similar n values; this challenge is amplified as n increases. To improve the ability to synthesize a targeted phase with precise control of the atomic layering, we apply the x-ray diffraction (XRD) approach developed for superlattices of III–V semiconductors to measure minute deviations from the ideal structure so that they can be quantitatively eradicated in subsequent films. We demonstrate the precision of this approach by improving the growth of known Ruddlesden–Popper phases and ultimately, by synthesizing an unprecedented n = 20 Ruddlesden–Popper phase, (ATiO 3 ) 20 AO where the A-site occupancy is Ba 0.6 Sr 0.4 . We demonstrate the generality of this method by applying it to Aurivillius phases and the Bi 2 Sr 2 Ca n–1 Cu n O 2n+4 series of high-temperature superconducting phases.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Methods for neutron diffraction studies on hydride superconductors and other metal hydrides

High-pressure neutron diffraction is an extremely useful technique in the quest for making and understanding novel hydride superconductors. Neutron diffraction can be used to directly determine elemental stoichiometries and atomic positions of many light elements such as hydrogen or deuterium, even in the presence of heavy elements such as rare-earth metals. In this work, we report on the current status and ongoing developments on high-pressure neutron diffraction for hydride superconductors and other metal hydrides with a special focus on current advancements at the Spallation Neutrons and Pressure (SNAP) beamline of the Spallation Neutron Source at Oak Ridge National Laboratory. For broader context, an overview of high-pressure neutron diffractometers and pressure cells is included together with insight into critical sample considerations. There, attention is given to the requirements for powdered hydride samples and the need for deuterium rather than hydrogen. Additionally, the advantages of angular access and data representation as possible at SNAP are described. We demonstrate the current capability for high-pressure neutron diffraction on two different samples created via hydrogen gas loading, specifically pure deuterium and nickel-deuteride. The deuterium example highlights the usefulness of adding sample materials that facilitate the formation of a good powder while the nickel-deuteride example demonstrates that atomic deuterium positions and stoichiometry can be directly determined. Both examples highlight the importance of large scattering apertures. These enable investigation of the data resolved by scattering angle that is needed to identify parasitic peaks and background features. Finally, future directions beyond current high-pressure neutron powder diffraction are also discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Interface atomic structures in a cadmium arsenide/III–V semiconductor heterostructure

The interface atomic structure between an epitaxial thin film of the prototype topological semimetal cadmium arsenide (Cd 3 As 2 ) and a III–V semiconductor layer is investigated using high-angle annular dark-field imaging in an aberration-corrected scanning transmission electron microscope. We find that the interface unit cell adopts a defined stoichiometry that is CdSb-like, which is achieved through the insertion of periodically arranged Cd vacancies in the terminating Cd-plane of Cd 3 As 2 . This interface stoichiometry is consistent with the Sb-termination of the III–V layer and the fact that CdSb is the thermodynamically stable phase in the Cd–Sb binary system. We find at least two distinct alignments of the film with respect to the buffer layer, which are characterized by a $\frac{1}{4}$ <100> Cd 3 As 2 shift parallel to the interface. We show that steps of half unit cell height in the III–V layer can produce these distinct interface structures.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Atomic cluster expansion potential for large scale simulations of hydrocarbons under shock compression

We present an Atomic Cluster Expansion (ACE) machine learned potential developed for high-fidelity atomistic simulations of hydrocarbons, targeting pressures and temperatures near and above supercritical fluid regimes for molecular fluids. A diverse set of stoichiometries were covered in training, including 1:0 (pure carbon), 1:4 (methane), and 1:1 (benzene), and rich bonding environments sampled at supercritical temperatures, hydrogen rich, reactive mixtures where metastable stoichiometries arise, including 1:2 (ethylene) and 1:3 (ethane). A high-fidelity training database was constructed by performing large-scale quantum molecular dynamic simulations [density functional theory (DFT) MD] of diamond, graphite, methane, and benzene. A novel approach to selecting structures from DFT MD is also presented, which allows for the rapid selection of unique DFT MD frames from complex trajectories. Comparisons to DFT and experimental data demonstrate that the presented ACE potential accurately reproduces isotherms, carbon melting curves, radial distribution functions, and shock Hugoniots for carbon and hydrocarbon systems for pressures up to 100 GPa and temperatures up to 6000 K for hydrocarbon systems and up to 9000 K for pure carbon systems. This work delivers a potential that can be used for accurate, large-scale simulations of shocked hydrocarbons and demonstrates a methodology for fitting and validating machine learning interatomic potentials to complex molecular environments, which can be applied to energetic materials in future works.

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

Electronic and structural properties of single-crystal Jahn–Teller active Co 1+x Mn 2–x O 4 thin films

Recent investigations on spinel CoMn 2 O 4 have shown its potential for applications in water splitting and fuel cell technologies as it exhibits strong catalytic behavior through oxygen reduction reactivity. To further understand this material, we report for the first time the synthesis of single-crystalline Co 1+x Mn 2-x O 4 thin films using molecular beam epitaxy. By varying sample composition, we establish links between cation stoichiometry and material properties using in-situ x-ray photoelectron spectroscopy, x-ray diffraction, scanning transmission electron microscopy, x-ray absorption spectroscopy, and spectroscopic ellipsometry. Our results indicate that excess Co ions occupy interstitial tetrahedral sites up to a certain stoichiometry, then are substitutional for octahedrally-coordinated Mn beyond this threshold. Here, we compare these results with density functional theory models of stoichiometric CoMn 2 O 4 to understand how the Jahn-Teller distortion and hybridization in Mn-O bonds impact the ability to hole dope the material with excess Co. The findings provide important insights into CoMn 2 O 4 and related spinel oxides for future application as inexpensive oxygen reduction reaction catalysts.

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

Smooth, homogeneous, high-purity Nb 3 Sn superconducting RF resonant cavity by seed-free electrochemical synthesis

Abstract Workbench-size particle accelerators, enabled by Nb 3 Sn-based superconducting radio-frequency (SRF) cavities, hold the potential of driving scientific discovery by offering a widely accessible and affordable source of high-energy electrons and x-rays. Thin-film Nb 3 Sn RF superconductors with high quality factors, high operation temperatures, and high-field potentials are critical for these devices. However, surface roughness, non-stoichiometry, and impurities in Nb 3 Sn deposited by conventional Sn-vapor diffusion prevent them from reaching their theoretical capabilities. Here we demonstrate a seed-free electrochemical synthesis that pushes the limit of chemical and physical properties in Nb 3 Sn. Utilization of electrochemical Sn pre-deposits reduces the roughness of converted Nb 3 Sn by five times compared to typical vapor-diffused Nb 3 Sn. Quantitative mappings using chemical and atomic probes confirm improved stoichiometry and minimized impurity concentrations in electrochemically synthesized Nb 3 Sn. We have successfully applied this Nb 3 Sn to the large-scale 1.3 GHz SRF cavity and demonstrated ultra-low BCS surface resistances at multiple operation temperatures, notably lower than vapor-diffused cavities. Our smooth, homogeneous, high-purity Nb 3 Sn provides the route toward high efficiency and high fields for SRF applications under helium-free cryogenic operations.

Physics↗
DOE OSTI2024

Properties of Nb x Ti (1–x) N thin films deposited on 300 mm silicon wafers for upscaling superconducting digital circuits

Scaling superconducting digital circuits requires fundamental changes in the current material set and fabrication process. The transition to 300 mm wafers and the implementation of advanced lithography are instrumental in facilitating mature CMOS processes, ensuring uniformity, and optimizing the yield. Here, this study explores the properties of Nb x Ti (1–x) N films fabricated by magnetron DC sputtering on 300 mm Si wafers. As a promising alternative to traditional Nb in device manufacturing, Nb x Ti (1–x) N offers numerous advantages, including enhanced stability and scalability to smaller dimensions, in both processing and design. As a ternary material, Nb x Ti (1–x) N allows engineering material parameters by changing deposition conditions. The engineered properties can be used to modulate device parameters through the stack and mitigate failure modes. We report characterization of Nb x Ti (1–x) N films at less than 2% thickness variability, 2.4% T c variability and 3% composition variability. Film resistivity (140–375 Ωcm) shows a strong correlation with the film oxygen content, while the critical temperature T c (4.6 K–14.1 K) is strongly affected by film stoichiometry and its microstructure has only a moderate effect on modifying T c . Our results offer insights about the interplay between film stoichiometry, film microstructure and critical temperature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Kinetic and substrate complex characterization of RamA, a corrinoid protein reductive activase from Methanosarcina barkeri

ABSTRACT In microbial corrinoid-dependent methyltransferase systems, adventitious Co(I)-corrinoid oxidation halts catalysis and necessitates repair by ATP-dependent reductive activases. RamA, an activase with a C-terminal ferredoxin domain with two [4Fe-4S] clusters from methanogenic archaea, has been far less studied than the bacterial activases bearing an N-terminal ferredoxin domain with one [2Fe-2S] cluster. These differences suggest RamA might prove to have other distinctive characteristics. Here, we examine RamA kinetics and the stoichiometry of the corrinoid protein:RamA complex. Like bacterial activases, K+ stimulates RamA. Potassium stimulation had been questioned due to differences in the primary structure of bacterial and methanogen activases. Unlike one bacterial activase, ATP is not inhibitory allowing the first determination of apparent kinetic parameters for any corrinoid activase. Unlike bacterial activases, a single RamA monomer complexes a single corrinoid protein monomer. Alanine replacement of a RamA serine residue corresponding to the serine of one bacterial activase which ligates the corrinoid cobalt during complex formation led to only moderate changes in the kinetics of RamA. These results reveal new differences in the two types of corrinoid activases, and provide direct evidence for the proposal that corrinoid activases act as catalytic monomers, unlike other enzymes that couple ATP hydrolysis to difficult reductions.

Microbiology↗
DOE OSTI2021

A defined medium based on R2A for cultivation and exometabolite profiling of soil bacteria

SummaryExometabolomics is an approach to assess how microorganisms alter their environments through the depletion and secretion of chemical compounds. Comparisons of inoculated with uninoculated media can be used to provide direct biochemical observations on depleted and secreted metabolites which can be used to predict resource competition, cross-feeding and secondary metabolite production in microbial isolates and communities. This approach is most powerful when used with defined media that enable tracking of all depleted metabolites. However, microbial growth media have traditionally been developed for the isolation and growth of microorganisms but not metabolite utilization profiling through LC-MS/MS. Here, we describe the construction of a defined medium, the Northen Lab Defined Medium (NLDM), that not only supports the growth of diverse bacteria but is defined and therefore suited for exometabolomic experiments. Metabolites included in NLDM were selected based on their presence in R2A medium and soil, elemental stoichiometry requirements, as well as knowledge of metabolite usage by different bacteria. We found that NLDM supported the growth of 53 phylogenetically diverse soil bacterial isolates and all of its metabolites were trackable through LC–MS/MS analysis. These results demonstrate the viability and utility of the constructed NLDM medium for cultivating and characterizing diverse microbial isolates and communities.Originality-Significance StatementWe build a defined medium based on the metabolite composition of R2A medium and soil, elemental stoichiometry requirements, and knowledge of metabolite usage by different bacteria. The newly formulated defined medium was evaluated on its ability to support the growth of soil isolates and its application for metabolite utilization profiling. We found that of 53 phylogenetically diverse soil bacterial isolates grew on the defined medium and all of its metabolites were trackable through LC–MS/MS analysis. This demonstrates the viability and utility of the constructed defined medium for cultivating and characterizing diverse microbial isolates and communities.

de Raad, Markus↗
DOE OSTI2025

Structural stability, elemental ordering, and transport properties of layered ScTaN 2

Ternary transition metal (TM) nitrides have gained significant attention in thin film research due to their promising properties for a broad range of applications. Particularly, some of the ternary TM nitrides have been predicted to adopt layered structures that make them interesting for thermoelectric conversion and quantum materials applications. Unfortunately, synthesis of TM ternary nitride films by physical vapor deposition often favors disordered 3D structures rather than the predicted 2D-like layered structure. In this study, we investigate the structural interplay in the Sc-Ta-N ternary system using a combinatorial approach. Combinatorial libraries S⁢c 𝑥 ⁢T⁢a 1−𝑥 ⁢N are synthesized following a two-step method: First, deposit film precursors by cosputtering and then process the resulting 3D-structured samples with rapid thermal annealing. Synchrotron grazing-incidence wide-angle x-ray scattering on films annealed at 1200 ⁢°⁢C for 20 min leads to the nucleation of ScTaN 2 layered structure (𝑃⁢6 3 /𝑚⁢𝑚⁢𝑐) near stoichiometry. We find that the layered structure can accommodate large off-stoichiometry in the Ta-rich region (𝑥 < 0.5), facilitated by the alloying with quasi-isostructural Ta 5 ⁢N 6 compound that exists on a composition tie line at 𝑥 = 0. While focusing on ScTaN 2 , we estimate the long-range order parameter in near-stoichiometric films to be 0.86, corresponding to a fraction of Sc/Ta antisites of 7%. Transport measurements on ScTaN 2 reveal a nearly temperature-independent high carrier density (10 21 c⁢m −3 ), suggesting a heavily doped semiconductor or semimetallic character, consistent with a small positive Seebeck coefficient of +19 µV/K. The carrier mobility at 2 K is relatively small (9.5c⁢m 2 V −1 s −1 ) and the residual-resistivity ratio is minor, suggesting that electrical conduction is dominated by defects or disorder. Measured magnetoresistance suggests possible weak antilocalization at 2 K. This paper highlights the interplay between ScTaN 2 and Ta 5 ⁢N 6 crystal structures in stabilizing layered materials, emphasizes the importance of cation order/disorder for potential tunable alloys, and suggests that ScTaN 2 is a promising platform for exploring electronic properties.

36 MATERIALS SCIENCE↗