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DOE OSTI2019

In operando studies of CO oxidation on epitaxial SrCoO 2.5+δ thin films

The high abundance and fast kinetics of select transition metal oxide catalysts are attractive features for many chemical and electrochemical device applications. However, the activity of such catalysts can be accompanied by phase instabilities that prevent their widespread usage. Furthermore, complexities associated with variations in phase behavior and oxygen stoichiometry have hindered studies on the true origins of catalytic activity. Here, we explore the interactions between activity, phase stability, and microstructure using in operando synchrotron X-ray techniques and gas chromatography/mass spectroscopy (GCMS) to probe the behavior of model SrCoO 2.5+δ (SCO) catalysts. Pulsed laser deposition was used to prepare SCO thin films on (001) SrTiO 3 , (111) SrTiO 3 , and pseudocubic (001) DyScO 3 substrates. The GCMS catalytic measurements were performed with a custom-built microreactor compatible with a synchrotron X-ray diffractometer at the Advanced Photon Source. The activity for carbon monoxide oxidation was determined as a function of temperature from 500 °C to 800 °C. We show that the SrCoO 2.5+δ films are active for CO oxidation, most likely by direct reaction with lattice oxygen; consequently, the activity was observed to increase as the films become less stable, with the most active film being the one exhibiting the lowest surface and crystal quality. All films decompose at high temperatures, with in operando diffraction indicating the gradual formation of Sr-rich hexagonal and CoO phases. We find that real-time studies of model oxide systems with synchrotron X-rays is a powerful means of gaining insight into the varied processes taking place at catalytic surfaces.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Phase diagram of the TIP4P/Ice water model by enhanced sampling simulations

In this work, we studied the phase diagram for the TIP4P/Ice water model using enhanced sampling molecular dynamics simulations. Our approach is based on the calculation of ice–liquid free energy differences from biased coexistence simulations that reversibly sample the melting and growth of layers of ice. We computed a total of 19 melting points for five different ice polymorphs, which are in excellent agreement with the melting lines obtained from the integration of the Clausius–Clapeyron equation. For proton-ordered and fully proton-disordered ice phases, the results are in very good agreement with previous calculations based on thermodynamic integration. For the partially proton-disordered ice III, we find a large increase in stability that is in line with previous observations using direct coexistence simulations for the TIP4P/2005 model. This issue highlights the robustness of the approach employed here for ice polymorphs with diverse degrees of proton disorder. Our approach is general and can be applied to the calculation of other complex phase diagrams.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Laser-Induced Cooperative Transition in Molecular Electronic Crystal

The competing and non-equilibrium phase transitions, involving dynamic tunability of cooperative electronic and magnetic states in strongly correlated materials, show great promise in quantum sensing and information technology. To date, the stabilization of transient states is still in the preliminary stage, particularly with respect to molecular electronic solids. Here, a dynamic and cooperative phase in potassium-7,7,8,8-tetracyanoquinodimethane (K-TCNQ) with the control of pulsed electromagnetic excitation is demonstrated. Simultaneous dynamic and coherent lattice perturbation with 8 ns pulsed laser (532 nm, 15 MW cm -2 , 10 Hz) in such a molecular electronic crystal initiates a stable long-lived (over 400 days) conducting paramagnetic state (≈42 Ωcm), showing the charge–spin bistability over a broad temperature range from 2 to 360 K. Comprehensive noise spectroscopy, in situ high-pressure measurements, electron spin resonance (ESR), theoretical model, and scanning tunneling microscopy/spectroscopy (STM/STS) studies provide further evidence that such a transition is cooperative, requiring a dedicated charge–spin–lattice decoupling to activate and subsequently stabilize nonequilibrium phase. Finally, the cooperativity triggered by ultrahigh-strain-rate (above 10 6 s -1 ) pulsed excitation offers a collective control toward the generation and stabilization of strongly correlated electronic and magnetic orders in molecular electronic solids and offers unique electro-magnetic phases with technological promises.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Colossal Strain Tuning of Ferroelectric Transitions in KNbO 3 Thin Films

Strong coupling between polarization ( P ) and strain (ɛ) in ferroelectric complex oxides offers unique opportunities to dramatically tune their properties. Here colossal strain tuning of ferroelectricity in epitaxial KNbO 3 thin films grown by sub‐oxide molecular beam epitaxy is demonstrated. While bulk KNbO 3 exhibits three ferroelectric transitions and a Curie temperature ( T c ) of ≈676 K, phase‐field modeling predicts that a biaxial strain of as little as −0.6% pushes its T c > 975 K, its decomposition temperature in air, and for −1.4% strain, to T c > 1325 K, its melting point. Furthermore, a strain of −1.5% can stabilize a single phase throughout the entire temperature range of its stability. A combination of temperature‐dependent second harmonic generation measurements, synchrotron‐based X‐ray reciprocal space mapping, ferroelectric measurements, and transmission electron microscopy reveal a single tetragonal phase from 10 K to 975 K, an enhancement of ≈46% in the tetragonal phase remanent polarization ( P r ), and a ≈200% enhancement in its optical second harmonic generation coefficients over bulk values. These properties in a lead‐free system, but with properties comparable or superior to lead‐based systems, make it an attractive candidate for applications ranging from high‐temperature ferroelectric memory to cryogenic temperature quantum computing.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Inverter-Based Operation of Maui: Electromagnetic Transient Simulations

As larger and larger power systems approach and reach 100% inverter-based resource (IBR) operation during some hours of the year, questions arise regarding the stability of such extremely-high IBR power systems, the potential need for grid-forming (GFM) inverter technology, and the potential need for synchronous condensers. Relatedly, questions also arise about the ability of conventional positive sequence power system modeling tools to capture high-IBR system dynamics. This presentation introduces electromagnetic transient (EMT) simulations in PSCAD of the near-future (year 2023) Maui power system at and near 100% IBR operation and compares those simulations to positive sequence (PSSE) simulations. The Maui PSCAD model is parallelized on 30 cores and includes the entire transmission system (>200 three-phase buses), >170 individual and aggregate IBR models, four wind plants, and three synchronous generators plus six synchronous condensers at two locations. We investigate system stability with varying levels of inertia using conventional grid-following IBR controls, and then we investigate the impact of GFM controls on stability. Results suggest that: 1) positive sequence simulations can miss key dynamics in extremely high IBR cases; 2) EMT simulations can also miss key dynamics if inverter inner control dynamics are not modeled; 3) synchronous condensers can stabilize a system in which 100% of the energy is supplied by IBRs, even conventional grid-following IBRs; 4) GFM controls on just some of the IBRs can stabilize a 100% IBR power system, even if that system has zero inertia (i.e. no synchronous condensers, though synchronous condensers may be needed for other purposes such as protection system operations).

41 EE - Solar Energy Technologies Office (EE-4S)↗

DOE OSTI2020

Structure and Dynamics of Domains in Ferroelectric Nanostructures – Phase-Field Modeling (Final Technical Report)

Domain pattern formation is one of the most common phenomena in nature and is a topic of immense interest in many fields ranging from materials science and physics to chemistry and biology. This DOE sponsored research project explored the basic science concerning the thermodynamic stability of mesoscale polarization domain patterns and their temporal evolution mechanisms during formation and subsequent switching in ferroelectric nanostructures and heterostructures. The project employed the computational phase-field method in combination of microelasticity and electrostatic theories. The research was carried out in close collaboration with a number of experimental groups who used High Resolution Transmission Electron Microscopy (HRTEM), in situ TEM with Scanning Probe Microscopy (SPM), or Piezoresponse Force Microscopy (PFM) to characterize the domain structures and dynamics of ferroelectric thin films and heterostructures and who grow high-quality ferroelectric and multiferroic thin films using advanced growth techniques such as Molecular Beam Epitaxy (MBE), Pulsed Laser Deposition (PLLD), and sputtering. The research efforts of the project help establish the phase-field method as the most powerful method for understanding and predicting domain structures in ferroelectric thin films and nanostructures. The findings of the project led to the basic understanding of stability and switching mechanisms of ferroelectric domains under different mechanical boundary conditions and under either homogeneous capacitor configurations or local fields using metallic probes as electrodes and the emergence of charged domain walls during domain switching. The project predicted the spatial length scales, temperature ranges, and electromechanical conditions for different polar states in heterostructures and guided the discovery of both transient and stable novel polarization states containing vortex lattices in oxide superlattices. The project resulted in 134 journal publications and 6 PhD theses with all the PhD graduates currently working in either academia or industry within the United States. The basic understanding on the stability of mesoscale polar states and pattern evolution achieved by the project improved our ability to control and engineer properties of ferroelectric thin films and heterostructures for potential applications in nanoscale electronic devices.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Field-tailoring quantum materials via magneto-synthesis: metastable metallic and magnetically suppressed phases in a trimer iridate

We demonstrate that applying modest magnetic fields (< 0.1 T) during high-temperature crystal growth can profoundly alter the structure and ground state of a spin-orbit-coupled, antiferromagnetic trimer lattice. Using BaIrO₃ as a model system, whose ground state is intricately dictated by the trimer lattice, we show that magneto-synthesis , a field-assisted synthesis approach, stabilizes a structurally compressed, metastable metallic and magnetically suppressed phases inaccessible via conventional methods. These effects include a 0.85% reduction in unit cell, 4-order-of-magnitude decrease in resistivity, a 10-fold enhancement of the Sommerfeld coefficient, and the collapse of long-range magnetic order -- all intrinsic and bulk in origin. First-principles calculations confirm that the field-stabilized structure lies substantially above the ground state in energy, highlighting its metastable character. These large, coherent and correlated changes across multiple bulk properties, unlike those caused by dilute impurities, defects or off-stoichiometry, point to an intrinsic field-induced mechanism. The findings establish magneto-synthesis as a powerful new pathway for accessing non-equilibrium quantum phases in strongly correlated materials.

magneto-synthesis↗

DOE OSTI2025

A Panoramic View of MXenes via an Atomic Coordination‐Based Design Strategy

Two‐dimensional (2D) transition metal carbides and nitrides, known as MXenes, possess unique physical and chemical properties, enabling diverse applications in fields ranging from energy storage to communication, catalysis, sensing, healthcare, and beyond. Despite extensive research and notable advancements, a fundamental understanding of MXenes’ phase diversity and its connection to their hierarchical precursors, including the intermediate MAX phases and the ancestral bulk phases, remains limited. Here, in this study, it is hypothesized that the atomic coordination environments adopted by transition metal and nonmetallic atoms in their three‐dimensional (3D) bulk precursors may persist in 2D MXenes to govern their phase diversity. Using high‐throughput modeling based on first‐principles density functional theory, a wide range of MXene phases is unveiled and comprehensively evaluate their relative stabilities across a large chemical space. The key to the approach lies in considering various atomic coordination environments drawn from four types of ancestral bulk phases. Through this comprehensive structural library of MXenes, general guiding principles are uncovered, such as a close alignment between the phase stability of MXenes and that of their 3D precursors. These findings introduce a new design strategy in which the atomic coordination environments in bulk phases can serve as reliable predictors for accessing the diverse structural landscape of MXenes.

MXenes↗

DOE OSTI2026

CoSn-type NiIn1–xSbx (0 ≤ x ≤ 0.17): Site-Selective Substitution, Electronic Structure, Chemical Bonding, and Structural Transformation

CoSn-type intermetallic compounds have emerged as a model platform for Kagome-derived flat-band physics, where subtle chemical perturbations can strongly influence electronic structure and phase stability. Here, we present a combined experimental and theoretical study of Sb-substitution in CoSn-type NiIn1–xSbx (0 ≤ x ≤ 0.17) to elucidate the interplay between site selectivity, solubility limit, chemical bonding, and electronic structure. Rietveld refinements on Neutron powder diffraction data confirmed the selective Sb-substitution at the electron-rich In2 (2d) site forming the honeycomb substructure, while the In1 (1a) site within the Kagome layer remains exclusively occupied by In. Density functional theory (DFT) calculations revealed that pristine CoSn-type NiIn hosts Ni 3d-dominated flat bands near the Fermi level (EF), originating from the Kagome-like Ni substructure. Partial replacement of In by Sb within the honeycomb layer alters these flat-band features below EF, reducing the density of states and suppressing the flat-band topology near the Fermi level. Orbital-resolved electronic structure and chemical-bonding analyses show that Sb-substitution enhances Ni-p-block (In/Sb) covalency and optimizes charge compensation, stabilizing the CoSn-type structure up to the solubility limit x ≈ 0.17. Beyond the limit, the higher-Sb compositions show satellite reflections consistent with an incommensurately modulated phase. These results establish a link between site-selective chemical substitution, bonding optimization, and flat-band electronic structure evolution, providing fundamental insights into how chemical substitution influences the electronic properties of Kagome-based intermetallic compounds.

Roy, Nilanjan [National Institute of Technology Si↗

DOE OSTI2022

High-Accuracy Semiempirical Quantum Models Based on a Minimal Training Set

A great need exists for computationally efficient quantum simulation approaches that can achieve an accuracy similar to high-level theories at a fraction of the computational cost. In this regard, we have leveraged a machine-learned interaction potential based on Chebyshev polynomials to improve density functional tight binding (DFTB) models for organic materials. The benefit of our approach is two-fold: (1) many-body interactions can be corrected for in a systematic and rapidly tunable process, and (2) high-level quantum accuracy for a broad range of compounds can be achieved with ~0.3% of data required for one advanced deep learning potential. Our model exhibits both transferability and extensibility through comparison to quantum chemical results for organic clusters, solid carbon phases, and molecular crystal phase stability rankings. Overall, our efforts thus allow for high-throughput physical and chemical predictions with up to coupled-cluster accuracy for systems that are computationally intractable with standard approaches.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Electromagnetic signatures of a chiral quantum spin liquid

Quantum spin liquids (QSL) have emerged as a captivating subject within interacting spin systems that exhibit no magnetic ordering even at the lowest temperature accessible experimentally. However, definitive experimental evidence remains elusive. In light of the recent surge in theoretical and experimental interest in the half-filled Hubbard model on a triangular lattice, which offers the potential for stabilizing a chiral QSL, we investigate the electromagnetic signatures of this phase to facilitate experimental detection. Utilizing a combination of parton mean-field theory and unbiased density-matrix renormalization group calculations, we systematically examine the electrical charge and orbital electrical current associated with a spinon excitation in the chiral QSL. Additionally, we calculate the longitudinal and transverse optical conductivities below the Mott gap. Furthermore, employing quantum field theory analysis, we unravel the connection between spinon excitations and emergent as well as physical gauge fields. Our results demonstrate that the chiral QSL phase exhibits a distinct electromagnetic response, even within a Mott insulator regime. This finding holds great potential for enabling the experimental detection of this long-sought-after phase.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Colliding Pulse Mode Locking and Nonequilibrium Carrier Dynamics within Vertical External-Cavity Surface-Emitting Lasers

The complex nonlinear dynamics of colliding counterpropagating ultrashort laser pulses circulating in a vertical external-cavity surface-emitting ring laser cavity are captured by a first-principles quantum-mechanical microscopic model coupled to an intracavity beam propagator. Furthermore, our numerical simulations establish that overall mode locking stability is sensitive to relative phases and delays of the pulses impinging on the semiconductor saturable absorber mirror. Delay offsets of the counterpropagating pulses lead to asymmetric carrier recovery and instability, often leading in turn to single unidirectional circulating pulses. Although computationally challenging, we also include transverse effects and show that the influence of interference patterns from spatial gratings written by the counterpropagating pulses is significant in stabilizing the modelocked pulses.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Phase and Morphology of Water-ice Grains Formed in a Cryogenic Laboratory Plasma

Abstract Grains of ice are formed spontaneously when water vapor is injected into a weakly ionized laboratory plasma in which the background gas has been cooled to cryogenic temperatures comparable to those of deep space. These ice grains are levitated indefinitely within the plasma so that their time evolution can be observed under free-floating conditions. Using microscope imaging, ice grains are shown to have a spindle-like fractal structure and grow over time. Both crystalline and amorphous phases of ice are observed using Fourier transform infrared spectroscopy. A mix of crystalline and amorphous grains coexists under certain thermal conditions, and a linear mixing model is used on the ice absorption band surrounding 3.2 μ m to examine the ice phase composition and its temporal stability. The extinction spectrum is also affected by inelastic scattering as grains grow, and characteristic grain radii are obtained from Mie scattering theory and compared to size measurements from direct imaging. Observations are used to compare possible ice nucleation mechanisms, and it is concluded that nucleation is likely catalyzed by ions, as ice does not nucleate in the absence of plasma and impurities are not detected. Ice grain properties and infrared extinction spectra show similarity to observations of some astrophysical ices observed in protoplanetary disks, implying that the fractal morphology of the ice and observed processes of homogeneous ice nucleation could occur as well in such astrophysical environments with weakly ionized conditions.

Astronomy & Astrophysics↗

DOE OSTI2021

Origin of Insulating Ferromagnetism in Iron Oxychalcogenide Ce 2 O 2 FeSe 2

An insulating ferromagnetic (FM) phase exists in the quasi-one-dimensional iron oxychalcogenide Ce 2 O 2 FeSe 2 , but its origin is unknown. To understand the FM mechanism, here a systematic investigation of this material is provided, analyzing the competition between ferromagnetic and antiferromagnetic tendencies and the interplay of hoppings, Coulomb interactions, Hund’s coupling, and crystal-field splittings. Overall, our intuitive analysis based on second-order perturbation theory shows that large entanglements between doubly occupied and half filled orbitals play a key role in stabilizing the FM order in Ce 2 O 2 FeSe 2 . In addition, via many-body computational techniques applied to a multiorbital Hubbard model, the phase diagram confirms the proposed FM mechanism.

1-dimensional spin chains↗

DOE OSTI2023

A mesoscale crystal plasticity model to predict room-temperature deformation and martensitic transformation of high-strength Quenching and Partitioning (Q&P) Steels and validation with synchrotron X-ray diffraction

Renowned for the superior mechanical properties and adeptness at cold-forming, Quenching and Partitioning (QP) steels have gained prominence as a promising candidate material in fabricating safety-critical components in various industries. The pertinent research on QP steels focus on the martensitic transformation of the Retained Austenite (RA) phase during cold-forming, a crucial mechanism that substantially influences the overall strength and ductility of QP steels. The austenite stability and transformation rate heavily rely on the local strain path and the initial microstructure, which is challenging for analytical prediction. In this paper, a mesoscale model is developed to capture the deformation and transformation kinetics of QP steels inside the microstructure. The model integrates the detailed explicit microstructure, acquired from characterization experiments, into a high-resolution finite element (FE) mesh. It distinctly model the deformation and interaction between the various phases and the effect on the transformation of RA. The model is validated with high energy X-ray diffraction (HEXRD) data, and shows excellent capability in predicting the asymmetric stress-strain behavior under uniaxial tension and compression, as well as the martensitic transformation rate. The model is used to investigate the strain and load partitioning effect of surrounding matrix to the transformation of RA, offering insights into the complex behavior of QP980 and facilitates further material development.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Chemical short-range order in derivative Cr–Ta–Ti–V–W high entropy alloys from the first-principles thermodynamic study

The development of high-entropy alloys (HEAs) focuses on exploring compositional regions in multi-component systems with all alloy elements in equal or near-equal atomic concentrations. Initially it was based on the main idea that high mixing configurational entropy contributions to the alloy free energy could promote the formation of a single solid solution phase. By using the ab-initio based Cluster Expansion (CE) Hamiltonian model constructed for the quinary bcc Cr–Ta–Ti–V–W system in combination with Monte Carlo (MC) simulations, we show that the phase stability and chemical short-range order (SRO) of the equiatomic quinary and five sub-quaternary systems, as well as their derivative alloys, can dramatically change the order–disorder transition temperatures (ODTT) as a function of alloy compositions. In particular, it has been found, that the equiatomic quaternary Ta–Ti–V–W and Cr–Ta–Ti–W alloys had the lowest order–disorder transition temperature (500 K) among all the analysed equiatomic compositions. In all investigated alloy systems, the strongest chemical ordering has been observed between Cr and V, which led to the conclusion that decreasing the concentration of either Cr or V might be beneficial in terms of decreasing the ODTT. It also predicts that increasing concentration of Ti significantly decreases the ODTT. Our analysis of chemical SRO as a function of alloy composition allows to understand the microstructure evolution of HEAs as a function of temperature in excellent agreement with available experimental observations. Importantly, our free energy of mixing and SRO calculations predict that the origin of precipitates formed by Cr- and V-rich in the sub-quaternary Cr–Ta–V–W system is driven by the thermodynamics. The modelling results are in an excellent agreement with experimental observation of Cr and V segregation in the W 0.38 Ta 0.36 Cr 0.15 V 0.11 alloy which in turns shows an exceptional radiation resistance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Machine learned synthesizability predictions aided by density functional theory

Abstract A grand challenge of materials science is predicting synthesis pathways for novel compounds. Data-driven approaches have made significant progress in predicting a compound’s synthesizability; however, some recent attempts ignore phase stability information. Here, we combine thermodynamic stability calculated using density functional theory with composition-based features to train a machine learning model that predicts a material’s synthesizability. Our model predicts the synthesizability of ternary 1:1:1 compositions in the half-Heusler structure, achieving a cross-validated precision of 0.82 and recall of 0.82. Our model shows improvement in predicting non-half-Heuslers compared to a previous study’s model, and identifies 121 synthesizable candidates out of 4141 unreported ternary compositions. More notably, 39 stable compositions are predicted unsynthesizable while 62 unstable compositions are predicted synthesizable; these findings otherwise cannot be made using density functional theory stability alone. This study presents a new approach for accurately predicting synthesizability, and identifies new half-Heuslers for experimental synthesis.

Lee, Andrew (ORCID:0000000153014295)↗

DOE OSTI2026

T&D LIBRA: Simulation Framework for Transmission and Distribution Load and IBR Assessment

This paper introduces T&D LIBRA, a HELICS-based dynamic co-simulation framework designed for transmission and distribution (T&D) load and inverter-based resource assessment. This framework is designed to model interactions between single-phase induction motors (i.e., Motor-D), distributed energy resources (DERs) and the transmission network, emphasizing system stability during fault conditions. The primary objective of this research is to study the fault-induced delayed voltage recovery (FIDVR) behavior of the T&D networks using the co-simulation framework and to compare the results with conventional PSS/E only simulations. Simulations are validated using T&D co-simulations with a single distribution node and the IEEE 123-bus distribution test case. The co-simulation results demonstrate the value of using T&D co-simulations to capture motor stalling, DER tripping and other sources of voltage diversity on distribution networks.

24 POWER TRANSMISSION AND DISTRIBUTION↗