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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 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Soft and transferable pseudopotentials from multi-objective optimization

Ab initio pseudopotentials are a linchpin of modern molecular and condensed matter electronic structure calculations. In this work, we employ multi-objective optimization to maximize pseudopotential softness while maintaining high accuracy and transferability. To accomplish this, we develop a formulation in which softness and accuracy are simultaneously maximized, with accuracy determined by the ability to reproduce all-electron energy differences between Bravais lattice structures, whereupon the resulting Pareto frontier is scanned for the softest pseudopotential that provides the desired accuracy in established transferability tests. We employ an evolutionary algorithm to solve the multi-objective optimization problem and apply it to generate a comprehensive table of optimized norm-conserving Vanderbilt (ONCV) pseudopotentials (https://github.com/SPARC-X/SPMS-psps). Here, we show that the resulting table is softer than existing tables of comparable accuracy, while more accurate than tables of comparable softness. The potentials thus afford the possibility to speed up calculations in a broad range of applications areas while maintaining high accuracy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Crystallography of hyperbolic lattices

Hyperbolic lattices are a revolutionary platform for tabletop simulations of holography and quantum physics in curved space and facilitate efficient quantum error correcting codes. Their underlying geometry is non-Euclidean, and the absence of Bloch's theorem precludes the straightforward application of the often indispensable energy band theory to study model Hamiltonians on hyperbolic lattices. Motivated by recent insights into hyperbolic band theory, we initiate a crystallography of hyperbolic lattices. Here we show that many hyperbolic lattices feature a hidden crystal structure characterized by unit cells, hyperbolic Bravais lattices, and associated symmetry groups. Using the mathematical framework of higher-genus Riemann surfaces and Fuchsian groups, we derive a list of example hyperbolic {p,q} lattices and their hyperbolic Bravais lattices, including five infinite families and several graphs relevant for experiments in circuit quantum electrodynamics and topolectrical circuits. This dramatically simplifies the computation of energy spectra of tight-binding Hamiltonians on hyperbolic lattices, from exact diagonalization on the graph to solving a finite set of equations in terms of irreducible representations. The significance of this achievement needs to be compared to the all-important role played by conventional Euclidean crystallography in the study of solids. We exemplify the high potential of this approach by constructing and diagonalizing finite-dimensional Bloch wave Hamiltonians.

2-dimensional systems↗
DOE OSTI2024

Precise Fermi level engineering in a topological Weyl semimetal via fast ion implantation

The precise controllability of the Fermi level is a critical aspect of quantum materials. For topological Weyl semimetals, there is a pressing need to fine-tune the Fermi level to the Weyl nodes and unlock exotic electronic and optoelectronic effects associated with the divergent Berry curvature. However, in contrast to two-dimensional materials, where the Fermi level can be controlled through various techniques, the situation for bulk crystals beyond laborious chemical doping poses significant challenges. Here, we report the milli-electron-volt (meV) level ultra-fine-tuning of the Fermi level of bulk topological Weyl semimetal tantalum phosphide using accelerator-based high-energy hydrogen implantation and theory-driven planning. By calculating the desired carrier density and controlling the accelerator profiles, the Fermi level can be experimentally fine-tuned from 5 meV below, to 3.8 meV below, to 3.2 meV above the Weyl nodes. High-resolution transmission electron microscopy reveals the crystalline structure is largely maintained under irradiation, while electrical transport indicates that Weyl nodes are preserved and carrier mobility is also largely retained. Our work demonstrates the viability of this generic approach to tune the Fermi level in semimetal systems and could serve to achieve property fine-tuning for other bulk quantum materials with ultrahigh precision.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Negative Schottky Barriers and Spin-Polarized Fermi Crossings at WSe 2 /NbSe 2 Interfaces

Discovering and engineering spin-polarized surface states in the electronic structures of condensed matter systems is a crucial first step in the development of spintronic devices, wherein spin-polarized bands crossing the Fermi level can facilitate information transfer. Here, through nanofocused angle-resolved photoemission spectroscopy (nano-ARPES) and density functional theory-based calculations, we show that the interface between monolayer WSe 2 and metallic NbSe 2 exhibits a negative Schottky barrier height of ∼ −30 meV: the K-point valleys of the semiconducting layer are shifted by ∼800 meV to produce a surface-localized Fermi surface populated only by spin-polarized charge carriers. By increasing the WSe 2 thickness, the Fermi pockets can be moved from K to Γ, demonstrating tunability of novel semimetallic phases that exist atop a substrate additionally possessing charge density wave and superconducting phases. Together, this study provides a spectroscopic understanding into p-type, Schottky barrier-free interfaces, which are of urgent interest for bypassing the limitations of current-generation vertical field effect transistors, in addition to longer-term spintronics development.

2D material heterostructures↗
DOE OSTI2021

Low barrier height in a ZnO nanorods/NbSe 2 heterostructure prepared by van der Waals epitaxy

Two-dimensional (2D) materials as contacts for semiconductor devices have attracted much attention due to minimizing Fermi level pinning. Schottky–Mott physics has been widely employed to design 2D material-based electrodes and to elucidate their contact behavior. In this study, we revealed that charge transfer across a 2D/semiconductor heterointerface and materials characteristics besides work function should be accounted for in fabrication of electrodes based on 2D materials. Our density functional theory (DFT) calculations predicted that charge transfer between ZnO and NbSe 2 lowers the barrier height at the heterojunction and that conductive surface states of ZnO provide an additional conduction channel in the ZnO/NbSe 2 heterostructures. Crystalline ZnO/NbSe 2 heterostructures were prepared by the hydrothermal method. Electrical characterizations of the ZnO/NbSe 2 heterostructures showed Ohmic-like behavior as predicted by the DFT calculations, opposed to the prediction based on the Schottky–Mott model.

2D materials↗
DOE OSTI2021

Poisson_CCD: A dedicated simulator for modeling CCDs

A dedicated simulator, Poisson_CCD, has been constructed which models astronomical CCDs by solving Poisson’s equation numerically and simulating charge transport within the CCD. The potentials and free carrier densities within the CCD are self-consistently solved for, giving realistic results for the charge distribution within the CCD storage wells. The simulator has been used to model the CCDs that are being used to construct the LSST digital camera. The simulator output has been validated by comparing its predictions with several different types of CCD measurements, including astrometric shifts, brighter-fatter induced pixel–pixel covariances, saturation effects, and diffusion spreading. The code is open source and freely available.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Defect levels and self-compensation in iodine-doped CdTe single crystals

This study systematically documents defect levels in n-type iodine-doped cadmium telluride (CdTe:I) crystals as measured by thermoelectric effect spectroscopy, Hall-effect measurements, and photoluminescence and calculated by density functional theory. The primary donor, I Te , was identified with an activation energy of ∼0.05 eV (measured)/∼0.13 eV (calculated). Deep acceptor states, V Cd and I Te –V Cd complex, exhibited activation energies of ∼0.1 eV (measured)/∼0.19 eV (calculated) and ∼0.12 eV (measured)/∼0.24 eV (calculated), respectively. Self-compensation and Fermi level pinning were observed at ∼0.7 eV (measured)/∼1.08 eV (calculated), contributing to high resistivity in as-grown samples. Post-growth Cd annealing effectively removes compensation centers, releases iodine donors, and significantly reduces resistivity, resulting in an ideal n-type solar cell material.

Cd annealing↗
NASA NTRS1988

Investigations on the usefulness of the Massively Parallel Processor for study of electronic properties of atomic and condensed matter systems

The usefulness of the Massively Parallel Processor (MPP) for investigation of electronic structures and hyperfine properties of atomic and condensed matter systems was explored. The major effort was directed towards the preparation of algorithms for parallelization of the computational procedure being used on serial computers for electronic structure calculations in condensed matter systems. Detailed descriptions of investigations and results are reported, including MPP adaptation of self-consistent charge extended Hueckel (SCCEH) procedure, MPP adaptation of the first-principles Hartree-Fock cluster procedure for electronic structures of large molecules and solid state systems, and MPP adaptation of the many-body procedure for atomic systems.

Das, T. P.↗
DOE OSTI2022

Stochastic Vector Techniques in Ground-State Electronic Structure

Herein we review a suite of stochastic vector computational approaches for studying the electronic structure of extended condensed matter systems. These techniques help reduce algorithmic complexity, facilitate efficient parallelization, simplify computational tasks, accelerate calculations, and diminish memory requirements. While their scope is vast, we limit our study to ground-state and finite temperature density functional theory (DFT) and second-order many-body perturbation theory. More advanced topics, such as quasiparticle (charge) and optical (neutral) excitations and higher-order processes, are covered elsewhere. We start by explaining how to use stochastic vectors in computations, characterizing the associated statistical errors. Next, we show how to estimate the electron density in DFT and discuss effective techniques to reduce statistical errors. Finally, we review the use of stochastic vectors for calculating correlation energies within the second-order Møller-Plesset perturbation theory and its finite temperature variational form. Example calculation results are presented and used to demonstrate the efficacy of the methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Advances and Challenges of SCAN and r 2 SCAN Density Functionals in Transition‐Metal Compounds

ABSTRACT Transition‐metal compounds (TMCs) with open‐shell d ‐electrons are characterized by a complex interplay of lattice, charge, orbital, and spin degrees of freedom, giving rise to various fascinating applications. Often exhibiting exotic properties, these compounds are commonly classified as correlated systems due to strong inter‐electronic interactions called Hubbard U . This inherent complexity presents significant challenges to Kohn‐Sham density functional theory (KS‐DFT), the most widely used electronic structure method in condensed matter physics and materials science. While KS‐DFT is, in principle, exact for the ground‐state total energy, its exchange‐correlation energy must be approximated in practice. The mean‐field nature of KS implementations, combined with the limitations of current exchange‐correlation density functional approximations, has led to the perception that DFT is inadequate for correlated systems, particularly TMCs. Consequently, a common workaround involves augmenting DFT with an on‐site Hubbard‐like U correction. In recent years, the strongly constrained and appropriately normed (SCAN) density functional, along with its refined variant r 2 SCAN, has achieved remarkable progress in accurately describing the structural, energetic, electronic, magnetic, and vibrational properties of TMCs, challenging the traditional perception of DFT's limitations. This review explores the design principles of SCAN and r 2 SCAN, highlights their key advancements in studying TMCs, explains the mechanisms driving these improvements, and addresses the remaining challenges in this evolving field.

Zhang, Yubo [Minjiang Collaborative Center for The↗
DOE OSTI2022

Relaxation time approximations in PAOFLOW 2.0

Abstract Regardless of its success, the constant relaxation time approximation has limited validity. Temperature and energy dependent effects are important to match experimental trends even in simple situations. We present the implementation of relaxation time approximation models in the calculation of Boltzmann transport in 2.0 and apply those to model band-structures. In addition, using a self-consistent fitting of the model parameters to experimental conductivity data, we provide a flexible tool to extract scattering rates with high accuracy. We illustrate the approximations using simple models and then apply the method to GaAs, Si, $$\hbox {Mg}_3\hbox {Sb}_2$$ Mg 3 Sb 2 , and $$\hbox {CoSb}_3$$ CoSb 3 .

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Crystal chemistry at high pressure

The chemistry we are taught in school, and we experience in our daily existence occurs at 1 atm. However, pressure spans an astounding 62 orders of magnitude in the Universe in going from the void of interstellar space to the crushing conditions at the center of a neutron star. The way in which pressure affects chemistry is important for Earth and planetary sciences, materials science, in understanding the extreme conditions experienced in nuclear explosions, and it may be key in addressing the future energy needs of our society. In this article we outline how the often neglected pressure variable affects chemistry, beginning from the way in which atomic energy levels are altered. This lays the foundation for understanding the unique crystal and electronic structures that emerge when matter is squeezed, as well as pressure’s effect on chemical reactivity. Finally, we give an overview of the main concepts behind conventional, or phonon-mediated, superconductivity, and describe how the pressure variable may be key in discovering and designing light-element based materials whose superconducting critical temperatures approach room temperature. Here, we discuss some of the main families of superconducting hydrides that have been predicted computationally, and the experimental successes in this exciting and rapidly developing field.

Chemical bonding↗
DOE OSTI2022

Partial densities of states from x-ray absorption and Auger electron spectroscopy: Use of core-hole memory

Ag L 3 edge x-ray absorption and L 3 −M 4,5 M 4,5 Auger electron spectra have been measured and simulated for a variety of x-ray electric-field polarization and Auger electron emission directions. The theory relies on density-functional theory, use of the Bethe–Salpeter equation, atomic multiplet theory, and a simplified model for the Auger line shape and its dependence on photon energy. We also demonstrate that partial densities of states for dT 2g , dE g , and sA g symmetry partial-wave channels at the Ag site in the solid can be deduced from the experimental measurements with only atomic theoretical input, i.e., with no solid-state theory other than assuming a Fermi edge.

36 MATERIALS SCIENCE↗
DOE OSTI2022

X-ray nanodiffraction imaging reveals distinct nanoscopic dynamics of an ultrafast phase transition

Significance Phase transitions, the changes between states of matter with distinct electronic, magnetic, or structural properties, are at the center of condensed matter physics and underlie valuable technologies. First-order phase transitions are intrinsically heterogeneous. When driven by ultrashort excitation, nanoscale phase regions evolve rapidly, which has posed a significant experimental challenge to characterize. The newly developed laser-pumped X-ray nanodiffraction imaging technique reported here has simultaneous 100-ps temporal and 25-nm spatial resolutions. This approach reveals pathways of the nanoscale structural rearrangement upon ultrafast optical excitation, different from those transitions under slowly varying parameters. The spatiotemporally resolved structural characterization provides crucial nanoscopic insights into ultrafast phase transitions and opens opportunities for controlling nanoscale phases on ultrafast time scales.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Magnetically and optically active edges in phosphorene nanoribbons

Abstract Nanoribbons, nanometre-wide strips of a two-dimensional material, are a unique system in condensed matter. They combine the exotic electronic structures of low-dimensional materials with an enhanced number of exposed edges, where phenomena including ultralong spin coherence times 1,2 , quantum confinement 3 and topologically protected states 4,5 can emerge. An exciting prospect for this material concept is the potential for both a tunable semiconducting electronic structure and magnetism along the nanoribbon edge, a key property for spin-based electronics such as (low-energy) non-volatile transistors 6 . Here we report the magnetic and semiconducting properties of phosphorene nanoribbons (PNRs). We demonstrate that at room temperature, films of PNRs show macroscopic magnetic properties arising from their edge, with internal fields of roughly 240 to 850 mT. In solution, a giant magnetic anisotropy enables the alignment of PNRs at sub-1-T fields. By leveraging this alignment effect, we discover that on photoexcitation, energy is rapidly funnelled to a state that is localized to the magnetic edge and coupled to a symmetry-forbidden edge phonon mode. Our results establish PNRs as a fascinating system for studying the interplay between magnetism and semiconducting ground states at room temperature and provide a stepping-stone towards using low-dimensional nanomaterials in quantum electronics.

Science & Technology - Other Topics↗
DOE OSTI2025

Unification of finite symmetries in the simulation of many-body systems on quantum computers

Symmetry is fundamental in the description and simulation of quantum systems. Leveraging symmetries in classical simulations of many-body quantum systems can result in significant overhead due to the exponentially growing size of some symmetry groups as the number of particles increases. Quantum computers hold the promise of achieving exponential speedup in simulating quantum many-body systems; however, a general method for utilizing symmetries in quantum simulations has not yet been established. In this work, we present a unified framework for incorporating symmetry group transforms on quantum computers to simulate many-body systems. The core of our approach lies in the development of efficient quantum circuits for symmetry-adapted projection onto irreducible representations of a group or pairs of commuting groups. We provide resource estimations for common groups, including the cyclic and permutation groups. Our algorithms demonstrate the capability to prepare coherent superpositions of symmetry-adapted states and to perform quantum evolution across a wide range of models in condensed-matter physics and ab initio electronic structure in quantum chemistry. Specifically, we execute a symmetry-adapted quantum subroutine for small molecules in first-quantization on noisy hardware and demonstrate the emulation of symmetry-adapted quantum phase estimation for preparing coherent superpositions of quantum states in various irreducible representations of a symmetry group. In addition, we present a discussion of open problems regarding treating symmetries in digital quantum simulations of many-body systems, paving the way for future systematic investigations into leveraging symmetries quantumly for practical quantum advantage. The broad applicability and rigorous resource estimation for symmetry transformations make our framework appealing for achieving provable quantum advantage on fault-tolerant quantum computers, especially for symmetry-related properties.

quantum algorithms↗
DOE OSTI2021

Sparse expansions of multicomponent oxide configuration energy using coherency and redundancy

We report that compressed sensing has become a widely accepted paradigm to construct high dimensional cluster expansion models used for statistical mechanical studies of atomic configuration in complex multicomponent crystalline materials. However, strict sampling requirements necessary to obtain minimal coherence measurements for compressed sensing to guarantee accurate estimation of model parameters are difficult and in some cases impossible to satisfy due to the inability of physical systems to access certain configurations. Nevertheless, the dependence of energy on atomic configuration can still be adequately learned without these strict requirements by using compressed sensing by way of coherent measurements using redundant function sets known as frames. We develop a particular frame constructed from the union of all occupancy-based cluster expansion basis sets. We illustrate how using this highly redundant frame yields sparse expansions of the configuration energy of complex oxide materials that are competitive and often surpass the prediction accuracy and sparsity of models obtained from standard cluster expansions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Observation of Coulomb blockade and Coulomb staircases in superconducting Pr 0.8 Sr 0.2 NiO 2 films

Motivated by the discovery of superconductivity in the infinite-layer nickelate family, we report an experimental endeavor to clean the surface of nickelate superconductor Pr 0.8 Sr 0.2 NiO 2 films by Ar + ion sputtering and subsequent annealing, and we study their electronic structures by cryogenic scanning tunneling microscopy and spectroscopy. The annealed surfaces are characterized by nano-sized clusters and Coulomb staircases with periodicity inversely proportional to the projected area of the nanoclusters, consistent with a double-barrier tunneling junction model. Moreover, the dynamical Coulomb blockade effects are observed and result in well-defined energy gaps around the Fermi level, which correlate closely with the specific configuration of the junctions. These Coulomb blockade-related phenomena provide an alternative plausible cause of the observed gap structure that should be considered in the spectroscopic understanding of nickelate superconductors with the nano-clustered surface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗