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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Stabilization of high-performance rock-salt LiMnSbTe3 thermoelectrics with embedded van der Waals-like gaps

Rock-salt-structured compounds like lead chalcogenides are promising thermoelectrics, as their high symmetry, strong anharmonicity, and favorable phase behavior collectively lead to high performance by enabling large power factors and ultralow thermal conductivity. Here, we report LiMnSbTe 3 , a new rock-salt semiconductor stabilized through targeted chemical design by combining hexagonal MnTe with cubic LiSbTe 2 . Embedded in the highsymmetry matrix, van der Waals-like gaps form due to Sb 2 Te 3 nanoscale segregation, which acts as effective phonon-scattering centers, leading to a low lattice thermal conductivity of 0.37Wm- 1 K -1 at 873 K with alloy scattering from disordered cations. The ordered local structure of Sb2Te 3 -type vdW-like gaps and the cross-gap interaction facilitate the carrier transport. Aided by energyconverged valence bands and a paramagnon drag effect, high Seebeck coefficients and enhanced power factor can be achieved, leading to a high ZT of 1.2 at 873 K. Furthermore, introducing Mn deficiency increases ZT to 1.5, highlighting the potential for higher performance through optimized doping or alloying. A segmented single-leg thermoelectric module achieves an output power density of 0.52 Wcm -2 and an efficiency of 8.7% under ΔT of 478 K, further demonstrating its promising thermoelectric applications.

42 ENGINEERING↗
DOE OSTI2021

Importance of charge self-consistency in first-principles description of strongly correlated systems

First-principles approaches have been successful in solving many-body Hamiltonians for real materials to an extent when correlations are weak or moderate. As the electronic correlations become stronger often embedding methods based on first-principles approaches are used to better treat the correlations by solving a suitably chosen many-body Hamiltonian with a higher level theory. The success of such embedding theories, often referred to as second-principles, is commonly measured by the quality of self-energy Σ which is either a function of energy or momentum or both. However, Σ should, in principle, also modify the electronic eigenfunctions and thus change the real space charge distribution. While such practices are not prevalent, some works that use embedding techniques do take into account these effects. In such cases, choice of partitioning, of the parameters defining the correlated Hamiltonian, of double-counting corrections, and the adequacy of low-level Hamiltonian hosting the correlated subspace hinder a systematic and unambiguous understanding of such effects. Further, for a large variety of correlated systems, strong correlations are largely confined to the charge sector. Then an adequate nonlocal low-order theory is important, and the high-order local correlations embedding contributes become redundant. Here we study the impact of charge self-consistency within two example cases, TiSe 2 and CrBr 3 , and show how real space charge re-distribution due to correlation effects taken into account within a first-principles Green’s function-based many-body perturbative approach is key in driving qualitative changes to the final electronic structure of these materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Solid-state rigid-rod polymer composite electrolytes with nanocrystalline lithium ion pathways

A critical challenge for next-generation lithium-based batteries lies in development of electrolytes that enable thermal safety along with use of high-energy-density electrodes. We describe molecular ionic composite (MIC) electrolytes based on an aligned liquid crystalline polymer combined with ionic liquids and concentrated Li salt. This high strength (200 MPa) and non-flammable solid electrolyte possesses outstanding Li + conductivity (1 mS cm -1 at 25 °C) and electrochemical stability (5.6 V vs Li|Li + ) while suppressing dendrite growth and exhibiting low interfacial resistance (32 Ω cm 2 ) and overpotentials (≤ 120 mV @ 1 mA cm -2 ) during Li symmetric cell cycling. A heterogeneous salt doping process modifies a locally ordered polymer-ion assembly to incorporate an inter-grain network filled with defective LiFSI & LiBF 4 nanocrystals, strongly enhancing Li + conduction. Furthermore, this modular material fabrication platform shows promise for safe and high-energy-density energy storage and conversion applications, incorporating the fast transport of ceramic-like conductors with the superior flexibility of polymer electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2025

Topological prethermal strong zero modes on superconducting processors

Abstract Symmetry-protected topological phases 1–4 cannot be described by any local order parameter and are beyond the conventional symmetry-breaking model 5 . They are characterized by topological boundary modes that remain stable under symmetry respecting perturbations 1–4,6–8 . In clean, gapped systems without disorder, the stability of these edge modes is restricted to the zero-temperature manifold; at finite temperatures, interactions with mobile thermal excitations lead to their decay 9–11 . Here we report the observation of a distinct type of topological edge mode 12–14 , which is protected by emergent symmetries and persists across the entire spectrum, in an array of 100 programmable superconducting qubits. Through digital quantum simulation of a one-dimensional disorder-free stabilizer Hamiltonian, we observe robust long-lived topological edge modes over up to 30 cycles for a wide range of initial states. We show that the interaction between these edge modes and bulk excitations can be suppressed by dimerizing the stabilizer strength, leading to an emergent U(1) × U(1) symmetry in the prethermal regime of the system. Furthermore, we exploit these topological edge modes as logical qubits and prepare a logical Bell state, which exhibits persistent coherence, despite the system being disorder-free and at finite temperature. Our results establish a viable digital simulation approach 15–18 to experimentally study topological matter at finite temperature and demonstrate a potential route to construct long-lived, robust boundary qubits in disorder-free systems.

Science & Technology - Other Topics↗
DOE OSTI2021

Shear-free mixing to achieve accurate temporospatial nanoscale kinetics through scanning-SAXS: ion-induced phase transition of dispersed cellulose nanocrystals

Time-resolved in situ characterization of well-defined mixing processes using small-angle X-ray scattering (SAXS) is usually challenging, especially if the process involves changes of material viscoelasticity. In specific, it can be difficult to create a continuous mixing experiment without shearing the material of interest; a desirable situation since shear flow both affects nanoscale structures and flow stability as well as resulting in unreliable time-resolved data. Here, we demonstrate a flow-focusing mixing device for in situ nanostructural characterization using scanning-SAXS. Given the interfacial tension and viscosity ratio between core and sheath fluids, the core material confined by sheath flows is completely detached from the walls and forms a zero-shear plug flow at the channel center, allowing for a trivial conversion of spatial coordinates to mixing times. With this technique, the time-resolved gel formation of dispersed cellulose nanocrystals (CNCs) was studied by mixing with a sodium chloride solution. It is observed how locally ordered regions, so called tactoids, are disrupted when the added monovalent ions affect the electrostatic interactions, which in turn leads to a loss of CNC alignment through enhanced rotary diffusion. The demonstrated flow-focusing scanning-SAXS technique can be used to unveil important kinetics during structural formation of nanocellulosic materials. However, the same technique is also applicable in many soft matter systems to provide new insights into the nanoscale dynamics during mixing.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Machine learning-based multidomain processing for texture-based image segmentation and analysis

Atomic and molecular resolved atomic force microscopy (AFM) images offer unique insights into materials' properties such as local ordering, molecular orientation, and topological defects, which can be used to pinpoint physical and chemical interactions occurring at the surface. Utilizing machine learning for extracting underlying physical parameters increases the throughput of AFM data processing and eliminates inconsistencies intrinsic to manual image analysis, thus enabling the creation of reliable frameworks for qualitative and quantitative evaluation of experimental data. Here, we present a robust and scalable approach to the segmentation of AFM images based on flexible pre-selected classification criteria. The usage of supervised learning and feature extraction allows us to retain the consideration of specific problem-dependent features (such as types of periodical structures observed in the images and the associated numerical parameters: spacing, orientation, etc.). We highlight the applicability of this approach for the segmentation of molecular resolved AFM images based on the crystal orientation of the observed domains, automated selection of boundaries, and collection of relevant statistics. Finally, we outline a general strategy for machine learning-enabled analysis of nanoscale systems exhibiting periodic order that could be applied to any analytical imaging technique

36 MATERIALS SCIENCE↗
DOE OSTI2021

Anomalous temperature dependence of the experimental x-ray structure factor of supercooled water

The structural changes of water upon deep supercooling were studied through wide-angle x-ray scattering at SwissFEL. The experimental setup had a momentum transfer range of 4.5 Å-1, which covered the principal doublet of the x-ray structure factor of water. The oxygen–oxygen structure factor was obtained for temperatures down to 228.5 ± 0.6 K. Similar to previous studies, the second diffraction peak increased strongly in amplitude as the structural change accelerated toward a local tetrahedral structure upon deep supercooling. We also observed an anomalous trend for the second peak position of the oxygen–oxygen structure factor (q 2 ). We found that q 2 exhibits an unprecedented positive partial derivative with respect to temperature for temperatures below 236 K. Based on Fourier inversion of our experimental data combined with reference data, we propose that the anomalous q 2 shift originates from that a repeat spacing in the tetrahedral network, associated with all peaks in the oxygen–oxygen pair-correlation function, gives rise to a less dense local ordering that resembles that of low-density amorphous ice. The findings are consistent with that liquid water consists of a pentamer-based hydrogen-bonded network with low density upon deep supercooling.

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

Probing the self-ionization of liquid water with ab initio deep potential molecular dynamics

The chemical equilibrium between self-ionized and molecular water dictates the acid–base chemistry in aqueous solutions, yet understanding the microscopic mechanisms of water self-ionization remains experimentally and computationally challenging. Herein, Density Functional Theory (DFT)–based deep neural network (DNN) potentials are combined with enhanced sampling techniques and a global acid–base collective variable to perform extensive atomistic simulations of water self-ionization for model systems of increasing size. The explicit inclusion of long-range electrostatic interactions in the DNN potential is found to be crucial to accurately reproduce the DFT free energy profile of solvated water ion pairs in small (64 and 128 H 2 O) cells. The reversible work to separate the hydroxide and hydronium to a distance S is found to converge for simulation cells containing more than 500 H 2 O, and a distance of ∼ 8 Å is the threshold beyond which the work to further separate the two ions becomes approximately zero. The slow convergence of the potential of mean force with system size is related to a restructuring of water and an increase of the local order around the water ions. Calculation of the dissociation equilibrium constant illustrates the key role of long-range electrostatics and entropic effects in the water autoionization process.

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

Spontaneously Broken Noninvertible Symmetries in Transverse-Field Ising Qudit Chains

Recent developments have revealed that symmetries need not form a group, but instead can be noninvertible. Here we use analytical arguments and numerical evidence to illuminate how spontaneous symmetry breaking of a noninvertible symmetry is similar yet distinct from ordinary, invertible, symmetry breaking. We consider one-dimensional chains of group-valued qudits, whose local Hilbert space is spanned by elements of a finite group 𝐺 (reducing to ordinary qubits when 𝐺=ℤ 2 ). We construct Ising-type transverse-field Hamiltonians with Rep⁡(𝐺) symmetry whose generators multiply according to the tensor product of irreducible representations (irreps) of the group 𝐺 . For non-Abelian 𝐺 , the symmetry is noninvertible. In the symmetry broken phase there is one ground state per irrep on a closed chain. The symmetry breaking can be detected by local order parameters but, unlike the invertible case, different ground states have distinct entanglement patterns. We show that for each irrep of dimension greater than one the corresponding ground state exhibits string order, entanglement spectrum degeneracies, and has gapless edge modes on an open chain—features usually associated with symmetry-protected topological order. Consequently, domain wall excitations behave as one-dimensional non-Abelian anyons with nontrivial internal Hilbert spaces and fusion rules. Our Letter identifies properties of noninvertible symmetry breaking that existing quantum hardware can probe.

1-dimensional spin chains↗
DOE OSTI2021

Experimental evidence that zinc impurities pin pair-density-wave order in La 2-x Ba x CuO 4

Both Zn doping and c-axis magnetic fields have been observed to increase the spin stripe order in La 2-x Ba x CuO 4 with x close to 1/8. For x = 0.095, the applied magnetic field also causes superconducting layers to decouple, presumably by favoring pair-density-wave order that consequently frustrates interlayer Josephson coupling. Here we show that introducing 1% Zn also leads to an initial onset of two-dimensional (2D) superconductivity, followed by 3D superconductivity at lower temperatures, even in zero field. Overall, we infer that the Zn pins pair-density-wave order locally, establishing the generality of such behavior.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Fractionalized Excitations Revealed by Entanglement Entropy

Fractionalized excitations develop in many unusual many-body states such as quantum spin liquids, disordered phases that cannot be described using any local order parameter. Also, because these exotic excitations correspond to emergent degrees of freedom, how to probe them and establish their existence is a long-standing challenge. We present a general procedure to reveal the fractionalized excitations using real-space entanglement entropy in critical spin liquids that are particularly relevant to experiments. Furthermore, we show how to use the entanglement entropy to construct the corresponding spinon Fermi surface. Our work defines a new pathway to establish and characterize exotic excitations in novel quantum phases of matter.

2-dimensional systems↗
DOE OSTI2025

Atomic-Scale Tracking of Topological Defect Motion and Incommensurate Charge Order Melting

Charge order pervades the phase diagrams of quantum materials where it competes with superconducting and magnetic phases, hosts electronic phase transitions and topological defects, and couples to the lattice generating intricate structural distortions. Incommensurate charge order is readily stabilized in manganese oxides, where it is associated with anomalous electronic and magnetic properties, but its nanoscale structural inhomogeneity complicates precise characterization and understanding of its relationship with competing phases. Leveraging atomic-resolution variable-temperature cryogenic scanning transmission electron microscopy, we characterize the thermal evolution of charge order as it transforms from its ground state in a model manganite system. We find that mobile networks of discommensurations and dislocations generate phase inhomogeneity and induce global incommensurability in an otherwise lattice-locked modulation. Driving the order to melt at high temperatures, the discommensuration density grows, and regions of order locally decouple from the lattice periodicity. Published by the American Physical Society 2025

Schnitzer, Noah (ORCID:0000000210421146)↗
DOE OSTI2025

Predicting interface structure using the minima hopping method

Here, we adapt the minima hopping method (MHM) to the problem of interfacial structure prediction and apply it to study a canonical problem, the tilt grain boundaries in SrTiO 3 . Our method employs a hybrid approach by first exploring the potential energy surface (PES) of different grain boundary samplings with an empirical force field, among which the fifteen candidates with lower energies are then refined using ab initio density functional theory (DFT) calculations. During the exploratory stage, we bias the search using a local order parameter to primarily sample various reconstructions in the vicinity of the interface, while preserving the crystallinity of the bulk regions. We further enhance the search by incorporating initial structures with rigid body displacements to account for translational variations between bulk phases, enabling the MHM to effectively generate both stoichiometric and nonstoichiometric SrTiO 3 Σ⁢3(111)[110] and Σ⁢3(112)[110] grain boundaries. From an algorithmic standpoint, MHM outperforms earlier studies based on genetic algorithms (GA) by identifying more stable interfacial structures of several SrTiO 3 grain boundaries. The performance of the present implementation of the MHM approach is primarily limited by exploring an approximate description of the PES with a rather simple Buckingham potential. This limitation leads to variations in performance when compared to approaches utilizing more advanced surrogate PES models, such as direct DFT-PES sampling or GA with the embedded atom method (EAM). Despite the present limitations, the MHM approach is able to yield interfacial structures with comparable or lower interfacial energies in specific cases, such as Σ⁢3(111)[110] Γ=1, ±0.5 and Σ⁢3(112)[110] Γ= ±1, −2, underscoring the robustness of the MHM approach even with a simple approximation of the DFT PES. The MHM interfacial structure prediction method thus offers an efficient approach to understanding the grain boundaries and heterointerfaces at the atomic scale, providing an important prerequisite for effective materials design.

density functional theory↗
DOE OSTI2020

Termination switching of antiferromagnetic proximity effect in topological insulator

This work reports the ferromagnetism of topological insulator, (Bi,Sb) 2 Te 3 (BST), with a Curie temperature of approximately 120 K induced by magnetic proximity effect (MPE) of an antiferromagnetic CrSe. The MPE was shown to be highly dependent on the stacking order of the heterostructure, as well as the interface symmetry: Growing CrSe on top of BST results in induced ferromagnetism, while growing BST on CrSe yielded no evidence of an MPE. Cr-termination in the former case leads to double-exchange interactions between Cr 3+ surface states and Cr 2+ bulk states. This Cr 3+ -Cr 2+ exchange stabilizes the ferromagnetic order localized at the interface and magnetically polarizes the BST Sb band. In contrast, Se-termination at the CrSe/BST interface yields no detectable MPE. These results directly confirm the MPE in BST films and provide critical insights into the sensitivity of the surface state.

42 ENGINEERING↗
DOE OSTI2025

OpenFerro v0.1.0

OpenFerro is a Python package for on-lattice atomistic dynamics simulation of ferroic materials. OpenFerro is based on JAX, a high-performance linear algebra package supporting auto-differentiation and GPU acceleration. OpenFerro is designed to minimize the effort required to build on-lattice Hamiltonian models, and to perform molecular dynamics (MD) and Landau-Lifshitz-Gilbert simulations. Unlike existing codes, OpenFerro provides a unified interface to model different types of local order parameters.

Xie, Pinchen [Lawrence Berkeley National Laborator↗
DOE OSTI2024

Modulating ion-binding at macromolecular interfaces during (bio)mineralization: A snapshot review for calcium carbonate and calcium phosphate systems

Abstract Local environments have strict influence over (bio)mineralization in calcifying systems. This snapshot review discusses recent insights into the roles of Ca 2+ -macromolecule interactions on the nucleation of calcium carbonate and calcium phosphate minerals. Experimental findings combined with simulations/modeling are providing breakthrough information and raising important questions for future studies. The emerging picture is that both nucleation and growth are driven by local ordering of ions and water about the macromolecule interface, rather than broader properties or molecular class. Tuning macromolecular properties at the atomic scale thus provides opportunities for highly specific controls on mineralization; however, many limitations and challenges remain. We highlight studies employing in-situ atomic force microscopy (AFM) and transmission electron microscopy (TEM) to observe crystallization processes on or near macromolecular substrates. As the distribution and ability of these techniques increases, fundamental studies integrating experimental and computational methods will be crucial to inform a broad range of applications. Graphical abstract

Knight, Brenna M. (ORCID:0000000244000067)↗
DOE OSTI2020

Exotic Phases of a Higgs-Yukawa Model with Reduced Staggered Fermions

We investigate the phase structure of a four dimensional SO(4) invariant lattice Higgs-Yukawa model comprising four reduced staggered fermions interacting with a real scalar field. The fermions belong to the fundamental representation of the symmetry group while the three scalar field components transform in the self-dual representation of SO(4). We explore the phase diagram and find evidence of a continuous transition between a phase where the fermions are massless to one where the fermions acquire mass. This transition is not associated with symmetry breaking and there is no obvious local order parameter.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗