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At least 1,567 records · Page 87
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Hartree–Fock–Bogoliubov theory for number-parity-violating fermionic Hamiltonians

It is usually asserted that physical Hamiltonians for fermions must contain an even number of fermion operators. This is indeed true in electronic structure theory. However, when the Jordan–Wigner (JW) transformation is used to map physical spin Hamiltonians to Hamiltonians of spinless fermions, terms that contain an odd number of fermion operators may appear. The resulting fermionic Hamiltonian thus does not have number parity symmetry and requires wave functions that do not have this symmetry either. In this work, we discuss the extension of standard Hartree–Fock–Bogoliubov (HFB) theory to the number-parity-nonconserving case. These ideas had appeared in the literature before but, perhaps for lack of practical applications, had, to the best of our knowledge, never been employed. We here present a useful application for this more general HFB theory based on coherent states of the SO(2M + 1) Lie group, where M is the number of orbitals. Here, we also show how using these unusual mean-field states can provide significant improvements when studying the JW transformation of chemically relevant spin Hamiltonians.

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

Low energy electrodynamics of CrI 3 layered ferromagnet

We report on the optical properties from terahertz (THz) to Near-Infrared (NIR) of the layered magnetic compound CrI 3 at various temperatures, both in the paramagnetic and ferromagnetic phase. In the NIR spectral range, we observe an insulating electronic gap around 1.1 eV which strongly hardens with decreasing temperature. The blue shift observed represents a record in insulating materials and it is a fingerprint of a strong electron-phonon interaction. Moreover, a further gap hardening is observed below the Curie temperature, indicating the establishment of an effective interaction between electrons and magnetic degrees of freedom in the ferromagnetic phase. Similar interactions are confirmed by the disappearance of some phonon modes in the same phase, as expected from a spin-lattice interaction theory. Therefore, the optical properties of CrI 3 reveal a complex interaction among electronic, phononic and magnetic degrees of freedom, opening many possibilities for its use in 2-Dimensional heterostructures.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2019

Hyperfine Interaction and Shockley–Read–Hall Recombination in Semiconductors

Experimental and theoretical studies on optical orientation and spin-dependent recombination in a semiconductor in a magnetic field under the normal incidence of circularly polarized radiation onto the sample surface are reviewed. The experiments were carried out on GaAs{sub 1 –x}N{sub x} solid solutions, in which Ga{sup 2+} interstitial displacement defects play the role of deep paramagnetic centers responsible for spin-dependent recombination. It is established that, in the investigated materials, the hyperfine interaction of a localized electron with one nucleus of the paramagnetic center remains strong even at room temperature. The theory is compared with an experiment conducted in the steady-state excitation mode and under two-pulse pump-probe conditions. An analytical formula for spin beats in a magnetic field is derived.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

High-Temperature Thermodynamics of Uranium from Ab Initio Modeling

We present high-temperature thermodynamic properties for uranium in its γ phase (γ-U) from first-principles, relativistic, and anharmonic theory. The results are compared to CALPHAD modeling. The ab initio electronic structure is obtained from density-functional theory (DFT) that includes spin–orbit coupling and an added self-consistent orbital-polarization (OP) mechanism for more accurate treatment of magnetism. The first-principles method is coupled to a lattice dynamics scheme that is used to model anharmonic lattice vibrations, namely, Self-Consistent Ab Initio Lattice Dynamics (SCAILD). The methodology can be summarized in the acronym DFT + OP + SCAILD. Upon thermal expansion, γ-U develops non-negligible magnetic moments that are included for the first time in thermodynamic theory. The all-electron DFT approach is shown to model γ-U better than the commonly used pseudopotential method. In addition to CALPHAD, DFT + OP + SCAILD thermodynamic properties are compared with other ab initio and semiempirical modeling and experiments. Our first-principles approach produces Gibbs free energy that is essentially identical to CALPHAD. The DFT + OP + SCAILD heat capacity is close to CALPHAD and most experimental data and is predicted to have a significant thermal dependence due to the electronic contribution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Spin State Modulation via Magnetic Fields in Fe Single Atom Catalysts for High-Performance Aqueous Zinc–Sulfur Batteries

Aqueous zinc–sulfur battery has garnered significant attention as a high-energy, low-cost, and safe energy storage system. However, the multielectron transfer kinetics of sulfur cathodes are relatively slow, presenting challenges such as limited sulfur utilization and lower discharge voltage, which significantly hinder their practical applications. Here, in this study, we explored a comprehensive design approach for high-performance, long-cycle aqueous zinc–sulfur batteries. The simultaneous introduction of ZnI 2 and Fe single atoms (Fe-SAs) as catalytically active agents decouples the redox reactions, effectively facilitating ZnS oxidation and S reduction separately. The application of an external magnetic field regulates the spin state of Fe-SAs, further enhancing their catalytic activity and electron transfer capability. Electrochemical tests demonstrate that the S@Fe-NC HS/ZnI 2 cathode assembled under a magnetic field exhibits excellent rate performance, achieving an impressive specific capacity of 1399 mAh g –1 at a high current density of 5 A g –1 and good cycling stability over 300 cycles, representing the highest reported high-current discharge capacity to date. This study provides a comprehensive design framework for optimizing zinc–sulfur (Zn–S) battery performance and elucidates the influence of magnetic field-induced spin state modulation on catalytic behavior.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Anyon superconductivity from topological criticality in a Hofstadter–Hubbard model

We argue that the combination of strong repulsive interactions and high magnetic fields can generate electron pairing and superconductivity. Inspired by the large lattice constants of moiré materials, which make large flux per unit cell accessible at laboratory fields, we study the triangular lattice Hofstadter-Hubbard model at one-quarter flux quantum per plaquette, where previous literature has argued that a chiral spin liquid separates a weak-coupling integer quantum Hall phase and a strong-coupling topologically trivial antiferromagnetic insulator at a density of one electron per site. We argue that topological superconductivity emerges upon doping in the vicinity of the integer quantum Hall to chiral spin liquid transition. We employ exact diagonalization and density matrix renormalization group methods to examine this theoretical scenario and find that electronic pairing indeed occurs on both sides of criticality over a remarkably broad range of interaction strengths. On the chiral spin liquid side, our results provide a concrete model realization of the long-hypothesized mechanism of anyon superconductivity. Our study thus establishes a beyond-Bardeen-Cooper-Schrieffer route to electron pairing in a well-controlled limit, relying crucially on the interplay between electron correlations and band topology.

Hubbard model↗
DOE OSTI2023

Electronic noise of a single skyrmion

To enable the practical use of skyrmion-based devices, it is essential to achieve a balance between energy efficiency and thermal stability while also ensuring reliable electrical detection against noise. Understanding how a skyrmion interacts with material disorder and external perturbations is thus essential. Here, we investigate the electronic noise of a single skyrmion under the influence of thermal fluctuations and spin currents in a magnetic thin film. We detect the thermally induced noise with a 1/ƒ $\gamma$ signature in the strong pinning regime but a random telegraph noise in the intermediate pinning regime. Both the thermally dominated and current-induced telegraphlike signals are detected in the weak pinning regime. Our results provide a comprehensive electronic noise picture of a single skyrmion, demonstrating the potential of noise fluctuation as a valuable tool for characterizing the pinning condition of a skyrmion. In conclusion, these insights could also aid in the development of low-noise and reliable skyrmion-based devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Exploring the Light-induced Dynamics in Solvated Metallogrid Complexes with Femtosecond Pulses Across the Electromagnetic Spectrum

Oligonuclear complexes of d 4 -d 7 transition metal ion centers that undergo spin-switching have long been developed for their practical role in molecular electronics. Recently, they also have appeared as promising photochemical reactants demonstrating improved stability. However, the lack of knowledge about their photophysical properties in the solution phase compared to their mononuclear congeners is currently hampering their inclusion into advanced light-driven reactions. In the present study, the ultrafast photoinduced dynamics in a solvated [2x2] iron(II) metallogrid complex are characterized by combining transient optical, infrared absorption and X-ray emission spectroscopic measurements on the femtosecond timescale. The analysis is supported by DFT calculations. The photocycle can be described in terms of intra-site transitions, where the Fe II in the low-spin (LS) state are independently photoexcited. The Franck-Condon state decays via the formation of a vibrationally-hot high-spin (HS) state that displays coherent behavior within a few picoseconds and thermalizes within tens of picosecond to yield a metastable HS state living for several hundreds of nanoseconds. Additionally, systematic comparison with the closely related mononuclear complex [Fe(terpy) 2 ] 2+ reveals that nuclearity has a profound impact on the photoinduced dynamics. Finally, this work provides guidelines for expanding the integration of oligonuclear complexes into new photoconversion schemes that may be triggered by ultrafast spin-switching.

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

Ab initio description of bcc iron with correlation matrix renormalization theory

We applied the ab initio spin-polarized correlation matrix renormalization theory to the ferromagnetic state of the bulk bcc iron. We showed that it was capable of reproducing the equilibrium physical properties and the pressure-volume curve in good comparison with experiments. We then focused on the analysis of its local electronic correlations. By exploiting different local fluctuation-related physical quantities as measures of electronic correlation within target orbits, we elucidated the different roles of t 2g and e g states in both spin channels and presented compelling evidence to showcase this distinction in their electronic correlation.

3-dimensional systems↗
DOE OSTI2020

Proton form factor ratio μ p G E p / G M p from double spin asymmetry

We report the ratio of the electric and magnetic form factor of the proton, $\mu_p G_E^p/G_M^p$, has been measured for elastic electron-proton scattering with polarized beam and target up to four-momentum transfer squared, $Q^2=5.66$ (GeV/c)$^2$ using the double spin asymmetry for target spin orientation aligned nearly perpendicular to the beam momentum direction. This measurement of $\mu_p G_E^p/G_M^p$ agrees with the $Q^2$ dependence of previous recoil polarization data and reconfirms the discrepancy at high $Q^2$ between the Rosenbluth and the polarization-transfer method with a different measurement technique and systematic uncertainties uncorrelated to those of the recoil-polarization measurements. The form factor ratio at $Q^2$=2.06 (GeV/c)$^2$ has been measured as $\mu_p G_E^p/G_M^p = 0.720 \pm 0.176_{stat} \pm 0.039_{sys}$, which is in agreement with an earlier measurement with the polarized target technique at similar kinematics. The form factor ratio at $Q^2$=5.66 (GeV/c)$^2$ has been determined as $\mu_p G_E^p/G_M^p=0.244\pm0.353_{stat}\pm0.013_{sys}$, which represents the highest $Q^2$ reach with the double spin asymmetry with polarized target to date.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2019

Spin Glass Behavior in La{sub 0.7}Ca{sub 0.23}Sr{sub 0.07}MnO{sub 3} Nanofibers Obtained by Electrospinning

This work contributes to the development of new nanostructured mixed valence manganites and to explore and optimize their magnetic properties at 1-D level. Nanofibers of La{sub 0.7}Ca{sub 0.23}Sr{sub 0.07}MnO{sub 3} manganite were fabricated using the electrospinning method and three different heat treatments to determine how the nanostructure affects its thermomagnetic behavior. From scanning electron microscopy, nanofibers morphology was observed and average diameters of 75, 94, and 97 nm were identified after heat treatments of 973, 1073, and 1173 K, respectively. According to X-ray diffraction technique, a single-phase orthorhombic structure was defined for each sample. Average crystallite sizes were determined as 47, 49, and 58 nm. A ferromagnetic to paramagnetic transition with Curie temperatures of 297, 305, and 314 K were identified, respectively. Furthermore, a glassy state was induced by nanofibers agglomeration. The spin glass and irreversible temperatures diminished as the magnetic field was increased and a highly anisotropic state was evidenced for all samples. Thermomagnetic behavior in manganites showed to be significantly influenced by the one-dimensional structure and exposed how the dimensionality proportionated by the fabrication method can be used to adjust magnetic properties.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Magnetotransport properties of the topological nodal-line semimetal CaCdSn

Topological nodal-line semimetals support protected band crossings, which form nodal lines or nodal loops between the valence and conduction bands and exhibit novel transport phenomena. Here we address the topological state of the nodal-line semimetal candidate material CaCdSn, and report magnetotransport properties of its single crystals grown by the self-flux method. In this work, our first-principles calculations show that the electronic structure of CaCdSn harbors a single nodal loop around the Γ point in the absence of spin-orbit coupling effects. The nodal crossings in CaCdSn are found to lie above the Fermi level and yield a Fermi surface that consists of both electron and hole pockets. CaCdSn exhibits high mobility (μ ≈ 3.44 × 10 4 cm 2 V –1 s –1 ) and displays a field-induced metal-semiconductor-like crossover with a plateau in resistivity at low temperature. We observe an extremely large and quasilinear nonsaturating transverse as well as longitudinal magnetoresistance (MR) at low temperatures (≈ 7.44 × 10 3 % and ≈ 1.71 × 10 3 %, respectively, at 4 K). We also briefly discuss possible reasons behind such a large quasilinear magnetoresistance and its connection with the nontrivial band structure of CaCdSn.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Machine Learning Accelerates the Discovery of Design Rules and Exceptions in Stable Metal–Oxo Intermediate Formation

Metal–oxo moieties are important catalytic intermediates in the selective partial oxidation of hydrocarbons and in water splitting. Stable metal–oxo species have reactive properties that vary depending on the spin state of the metal, complicating the development of structure–property relationships. To overcome these challenges, we train machine-learning (ML) models capable of predicting metal–oxo formation energies across a range of first-row metals, oxidation states, and spin states. Using connectivity-only features tailored for inorganic chemistry as inputs to kernel ridge regression or artificial neural network (ANN) ML models, we achieve good mean absolute errors (4–5 kcal/mol) on set-aside test data across a range of ligand orientations. Analysis of feature importance for oxo formation energy prediction reveals the dominance of nonlocal, electronic ligand properties in contrast to other transition metal complex properties (e.g., spin-state or ionization potential). We enumerate the theoretical catalyst space with an ANN, revealing expected trends in oxo formation energetics, such as destabilization of the metal–oxo species with increasing d-filling, as well as exceptions, such as weak correlations with indicators of oxidative stability of the metal in the resting state or unexpected spin-state dependence in reactivity. We carry out uncertainty-aware evolutionary optimization using the ANN to explore a >37 000 candidate catalyst space. New metal and oxidation state combinations are uncovered and validated with density functional theory (DFT), including counterintuitive oxo formation energies for oxidatively stable complexes. This approach doubles the density of confirmed DFT leads in originally sparsely populated regions of property space, highlighting the potential of ML-model-driven discovery to uncover catalyst design rules and exceptions.

transition metal catalysis↗
DOE OSTI2022

Interaction of Th with H 0/–/+ : Combined Experimental and Theoretical Thermodynamic Properties

In this work, high-level electronic structure calculations of the lowlying energy electronic states for ThH, ThH – , and ThH + are reported and compared to experimental measurements. The inclusion of spin–orbit coupling is critical to predict the ground-state ordering as inclusion of spin–orbit switches the coupled-cluster CCSD(T) ordering of the two lowest energy states for ThH and ThH + . At the multireference spin–orbit SO-CASPT2 level, the ground states of ThH, ThH – , and ThH + are predicted to be the 2 Δ 3/2 , 3 Φ 2 , and 3 Δ 1 states, respectively. The adiabatic electron affinity is calculated to be 0.820 eV, and the vertical detachment energy is calculated to be 0.832 eV in comparison to an experimental value of 0.87 ± 0.02 eV. The observed ThH – photoelectron spectrum has many transitions, which approximately correlate with excitations of Th + and/or Th. The adiabatic ionization energy of ThH including spin–orbit corrections is calculated to be 6.181 eV. The natural bond orbital results are consistent with a significant contribution of the Th + H – ionic configuration to the bonding in ThH. The bond dissociation energies for ThH, ThH – , and ThH + using the Feller–Peterson–Dixon approach were calculated to be similar for all three molecules and lie between 259 and 280 kJ/mol.

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

Thermal conductivity suppression in uranium-doped thorium dioxide due to phonon-spin interactions

In this work, impact of low level of uranium (U) atom substitution on thermal conductivity of thorium dioxide (ThO 2 ) is investigated. ThO 2 is an electronic insulator with a wide optical band-gap and no unpaired electrons whose thermal transport is governed by phonons. U-substitution introduces unpaired f-electrons resulting in paramagnetic behavior of U-ThO 2 at room temperature, which significantly suppresses its thermal conductivity. A single crystal of U-ThO 2 with graded composition of U is grown using a hydrothermal synthesis method, and thermal conductivity measurements are performed in regions with uniform composition of U at levels of 0%, 6%, 9% and 16%. Measured thermal conductivity profiles over 77–300 K temperature range are analyzed using an analytical expression for phonon-mediated thermal transport based on Klemens-Callaway model. Temperature dependent thermal conductivity is found to deviate significantly from the Rayleigh scattering trend expected for a simple substitutional point defect with a small perturbation to mass and interatomic forces. With the resonant scattering term, observed large suppression of thermal conductivity at low temperatures can be closely reproduced. Additionally, the extracted phonon-spin coupling constants imply a nonlinear relation of phonon-spin interaction intensity with respect to U doping percentage. Our study reveals how phonon-spin scattering contributed by unpaired f-electrons in U atoms influences thermal transport in the U-ThO 2 system.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Nucleon Structure Studies at Jefferson Lab and the Electron Ion Collider

The research programs of Thomas Jefferson Laboratory (JLab) and the future Electron- Ion Collider (EIC) focus on one of the main goals of strong interaction studies : understanding the structure of nucleons in terms of the quarks and gluons composing them. Their structure is encoded in functions such as Generalized Parton Distributions (GPDs), which describe how quarks and gluons’ transverse position and longitudinal momentum are distributed inside nucleons. GPDs allow to obtain three-dimensional pictures of nucleons and to understand some of their fundamental properties, such as their internal pressure or the emergence of their spin from the dynamics of the partons composing them. At JLab and the EIC, electron beams are used to probe nucleons. Measurement of reactions such as Deeply Virtual Compton Scattering (DVCS) allows access to GPDs. The first longitudinally polarized-target experiment of the CLAS12 program at Jlab took place in 2022-2023. Combining polarized electron beams and nucleon targets, this experiment offers unique access to observables that allow the measurement of different types of GPDs. In particular, the DVCS beam- and target-spin asymmetries for protons and neutrons in deuterium will be measured for the first time. They give access to kinds of GPDs that are still poorly known, and the comparison between proton and neutron data will allow the extraction of the flavor dependence of the structure of nucleons. Specific analysis methods have been implemented to work with a polarized nuclear target and are presented in this thesis. These methods allow to obtain preliminary results for the asymmetries, waiting for the complete statistics to be available. In the long term, the experimental program for the EIC has been established with a strong emphasis on the measurement of the structure of nucleons at high energy. Measurements of reactions such as DVCS impose strict requirements on the electromagnetic calorimeter that will allow to measure the energy of the scattered electrons and photons. This calorimeter, which is under development, will be based on scintillating crystals read by Silicon Photomultipliers (SiPMs). A new type of glass-based scintillating material was tested, evaluating the possibilities to meet the technical requirements concerning their light yield and resistance to radiation damage in particular. Several models of SiPMs have been characterized, demonstrating they can operate over the vast energy range necessary to address the physics case at the EIC and providing guidelines for developing their readout electronics.

Pilleux, Noemie↗
DOE OSTI2022

Spinor $GW$ Bethe-Salpeter calculations in BerkeleyGW: Implementation, symmetries, benchmarking, and performance

Computing the GW quasiparticle band structure and Bethe-Salpeter equation (BSE) absorption spectra for materials with spin-orbit coupling have commonly been done by treating GW corrections and spin-orbit coupling (SOC) as separate perturbations to density-functional theory. However, accurate treatment of materials with strong spin-orbit coupling (such as many topological materials of recent interest, and thermoelectrics) often requires a nonperturbative approach using spinor wave functions in the Kohn-Sham equation and GW/BSE. Such calculations have only recently become available, in particular for the BSE. Here, we have implemented this approach in the plane-wave pseudopotential GW/BSE code BerkeleyGW, which is highly parallelized and widely used in the electronic-structure community. We present reference results for quasiparticle band structures and optical absorption spectra of solids with different strengths of spin-orbit coupling, including Si, Ge, GaAs, GaSb, CdSe, Au, and Bi 2 Se 3 . The calculated quasiparticle band gaps of these systems are found to agree with experiment to within a few tens of meV. SOC splittings are found to be generally in better agreement with experiment, including quasiparticle corrections to band energies. The absorption spectrum of GaAs is not significantly impacted by the inclusion of spin-orbit coupling due to its relatively small value (0.2 eV) in the Λ direction, while the absorption spectrum of GaSb calculated with the spinor GW/BSE captures the large spin-orbit splitting of peaks in the spectrum. For the prototypical topological insulator Bi 2 Se 3 , we find a drastic change in the low-energy band structure compared to that of DFT, with the spinorial treatment of the GW approximation correctly capturing the parabolic nature of the valence and conduction bands after including off-diagonal self-energy matrix elements. We present the detailed methodology, approach to spatial symmetries for spinors, comparison against other codes, and performance compared to spinless GW/BSE calculations and perturbative approaches to SOC. This work aims to spur further development of spinor GW/BSE methodology in excited-state research software and enables a more accurate and detailed exploration of electronic and optical properties of materials containing elements with large atomic numbers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗