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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 397 records · Page 22
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Signatures of distinct impurity configurations in atomic-resolution valence electron-energy-loss spectroscopy: Application to graphene

The detection and identification of impurities and other point defects in materials is a challenging task. Signatures for point defects are typically obtained using spectroscopies without spatial resolution. Here in this paper, we demonstrate the power of valence electron-energy-loss spectroscopy (VEELS) in an aberration-corrected scanning transmission-electron microscope (STEM) to provide energy-resolved and atomically resolved maps of electronic excitations of individual impurities which, combined with theoretical simulations, yield unique signatures of distinct bonding configurations of impurities. We report VEELS maps for isolated Si impurities in graphene, which are known to exist in two distinct configurations. We also report simulations of the maps, based on density functional theory and dynamical scattering theory, which agree with and provide direct interpretation of observed features. We show that theoretical VEELS maps exhibit distinct and unambiguous signatures for the threefold- and fourfold-coordinated configurations of Si impurities in different energy-loss windows, corresponding to impurity-induced bound states, resonances, and antiresonances. With the advent of new monochromators and detectors with high energy resolution and low signal-to-noise ratio, the present work ushers an atomically resolved STEM-based spectroscopy of individual impurities as an alternative to conventional spectroscopies for probing impurities and defects.

36 MATERIALS SCIENCE↗
DOE OSTI2017

Alternative structure of TiO 2 with higher energy valence band edge

We introduce an alternative structure of TiO 2 anatase that has a higher energy oxygen p-like valence band maximum than pristine TiO 2 anatase and thus has a much better alignment with the water splitting levels. This alternative structure is unique when considering a large subspace of possible structural distortions of TiO 2 anatase. We propose two routes towards this state and believe that one of them might have been realized in the recently discovered so-called black TiO 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

Frustrated spin- 1 2 molecular magnetism in the mixed-valence antiferromagnets Ba 3 M Ru 2 O 9 ( M = In , Y, Lu)

We have performed magnetic susceptibility, heat capacity, muon spin relaxation, and neutron-scattering measurements on three members of the family Ba 3 MRu 2 O 9 , where M=In, Y, and Lu. These systems consist of mixed-valence Ru dimers on a triangular lattice with antiferromagnetic interdimer exchange. Although previous work has argued that charge order within the dimers or intradimer double exchange plays an important role in determining the magnetic properties, our results suggest that the dimers are better described as molecular units due to significant orbital hybridization, resulting in one spin-1/2 moment distributed equally over the two Ru sites. These molecular building blocks form a frustrated, quasi-two-dimensional triangular lattice. Our zero- and longitudinal-field μSR results indicate that the molecular moments develop a collective, static magnetic ground state, with oscillations of the zero-field muon spin polarization indicative of long-range magnetic order in the Lu sample. In conclusion, the static magnetism is much more disordered in the Y and In samples, but they do not appear to be conventional spin glasses.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Nonresonant valence-to-core x-ray emission spectroscopy of niobium

The valence-to-core (V2C) portion of x-ray emission spectroscopy (XES) measures the electron states close to the Fermi level. These states are involved in bonding, thus providing a measure of the chemistry of the material. For this paper, we show the V2C XES spectra for several niobium compounds. The Kβ" peak in the V2C XES results from the transition of a ligand 2s electron into the 1s core-hole of the niobium, a transition allowed by hybridization with the niobium 4p . This location in energy of this weak peak shows a strong ligand dependence, thus providing a sensitive probe of the ligand environment about the niobium.

36 MATERIALS SCIENCE↗
DOE OSTI2018

Valence, exchange interaction, and location of Mn ions in polycrystalline M n x G a 1 - x N ( x ≤ 0.04 )

In this paper, we present an experimental study for polycrystalline samples of the diluted magnetic semiconductor $\mathrm{M}{\mathrm{n}}_{x}\mathrm{G}{\mathrm{a}}_{1{-}x}\mathrm{N}(x{\le}0.04)$ in order to address some of the existing controversial issues. X-ray and neutron diffraction, x-ray absorption near-edge structure, and electron paramagnetic resonance experiments were used to characterize the structural, electronic, and magnetic properties of the samples, and inelastic neutron scattering was employed to determine the magnetic excitations associated with Mn monomers and dimers. Our main conclusions are as follows: (i) The valence of the Mn ions is $2+$. (ii) The $\mathrm{M}{\mathrm{n}}^{2+}$ ions experience a substantial single-ion axial anisotropy with parameter D = 0.027(3) meV. (iii) Nearest-neighbor $\mathrm{M}{\mathrm{n}}^{2+}$ ions are coupled antiferromagnetically. Finally, the exchange parameter $J={-}0.140(7)\mathrm{meV}$ is independent of the Mn content $x$; i.e., there is no evidence for hole-induced modifications of $J$ towards a potentially high Curie temperature postulated in the literature.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2018

Direct observation of strain-induced orbital valence band splitting in HfSe2 by sodium intercalation

By using angle-resolved photoemission spectroscopy (ARPES), the variation of the electronic structure of HfSe 2 has been studied as a function of sodium intercalation. We observe how this drives a band splitting of the p -orbital valence bands and a simultaneous reduction of the indirect band gap by values of up to 400 and 280 meV, respectively. Our calculations indicate that such behavior is driven by the band deformation potential, which is a result of our observed strain induced by sodium intercalation. The applied uniaxial strain calculations based on density functional theory agree strongly with the experimental ARPES data. Finally, these findings should assist in studying the physical relationship between intercalation and strain, as well as for large-scale two-dimensional straintronics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Systematics of E 2 strength in the s d shell with the valence-space in-medium similarity renormalization group

Recent developments in ab initio nuclear theory demonstrate promising results in medium- to heavy-mass nuclei. A particular challenge for many of the many-body methodologies, however, is an accurate treatment of the electric-quadrupole, E2, strength associated with collectivity. The valence-space in-medium similarity renormalization group (VS-IMSRG) is a particularly powerful method for accessing medium- and high-mass nuclei but has been found to underpredict E2 strengths. The purpose of this work is to evaluate the isospin dependence of this underprediction. We perform a systematic comparison of VS-IMSRG calculations with available literature. We make use of isoscalar and isovector contributions to the E2 matrix elements to assess isoscalar and isovector contributions to the missing strength. It is found that the E2 strength is consistent throughout T z =|12|, T z =|1|, T z =|32|, and T z =2 pairs within the sd shell. Furthermore, no isovector contribution to the deficiency is identified. A comparison with toy-models and coupled-cluster calculations is used to discuss potential origins of the missing strength, which arises from missing many-particle, many-hole excitations out of the model space. The absence of any significant isovector contribution to the missing E2 strength indicates that the E2 strength discrepancy, and therefore any correction, is largely independent of the isospin of the nuclei in question.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2017

Experimental study of the rearrangements of valence protons and neutrons amongst single-particle orbits during double- β decay in Mo 100

The rearrangements of protons and neutrons amongst the valence single-particle orbitals during double-beta decay of Mo-100 have been determined by measuring cross sections in (d, p), (p, d), (He-3, a), and (He-3, d) reactions on Mo-98,Mo-100 and Ru-100,Ru-102 targets. The deduced nucleon occupancies reveal significant discrepancies when compared with theoretical calculations; the same calculations have previously been used to determine the nuclear matrix element associated with the decay probability of double-beta decay of the Mo-100 system.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

Nucleon tomography and total angular momentum of valence quarks from synergy between lattice QCD and elastic scattering data

We present an exploratory work on integrating lattice-QCD results with experimental data for elastic scattering. Within the framework of generalized parton distributions, this approach allows for the extraction of detailed information about nucleon tomography and the total angular momentum carried by valence quarks. To accomplish this reliably, we introduce a new quantity, the “double ratio,” which significantly reduces the systematic uncertainties inherent in lattice QCD computations. Moreover, we introduce a “shadow” term in the extraction procedure, which is sensitive only to lattice-QCD results. This term allows us to investigate the model dependence of the extraction, providing a more flexible description of the nucleon that goes beyond the previously considered bell-shaped distribution.

Lattice QCD↗
DOE OSTI2020

Triplet Resonating Valence Bond State and Superconductivity in Hund’s Metals

A central idea in strongly correlated systems is that doping a Mott insulator leads to a superconductor by transforming the resonating valence bonds (RVBs) into spin-singlet Cooper pairs. Here, we argue that a spin-triplet RVB (tRVB) state, driven by spatially, or orbitally anisotropic ferromagnetic interactions can provide the parent state for triplet superconductivity. We apply this idea to the iron-based superconductors, arguing that strong on site Hund’s interactions develop intra-atomic tRVBs between the $t_{2_g}$ orbitals. On doping, the presence of two iron atoms per unit cell allows these interorbital triplets to coherently delocalize onto the Fermi surface, forming a fully gapped triplet superconductor. In this work, this mechanism gives rise to a unique staggered structure of on site pair correlations, detectable as an alternating π phase shift in a scanning Josephson tunneling microscope.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Excitonic Condensate in Flat Valence and Conduction Bands of Opposite Chirality

Excitonic Bose-Einstein condensation (EBEC) has drawn increasing attention recently with the emergence of 2D materials. A general criterion for EBEC, as expected in an excitonic insulator (EI) state, is to have negative exciton formation energies in a semiconductor. Here, using exact diagonalization of a multiexciton Hamiltonian modeled in a diatomic kagome lattice, we demonstrate that the negative exciton formation energies are only a prerequisite but insufficient condition for realizing an EI. By a comparative study between the cases of both conduction and valence flat bands (FBs) versus that of a parabolic conduction band, we further show that the presence and increased FB contribution to exciton formation provide an attractive avenue to stabilize the excitonic condensate, as confirmed by calculations and analyses of multiexciton energies, wave functions, and reduced density matrices. In conclusion, our results warrant a similar many-exciton analysis for other known and/or new candidates of EIs and demonstrate the FBs of opposite parity as a unique platform for studying exciton physics, paving the way to material realization of spinor BEC and spin superfluidity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

XMCD study of magnetism and valence state in iron-substituted strontium titanate

Room-temperature ferromagnetism was characterized for thin films of SrTi 0.6 Fe 0.4 O 3–δ grown by pulsed laser deposition on SrTiO 3 and Si substrates under different oxygen pressures and after annealing under oxygen and vacuum conditions. X-ray magnetic circular dichroism demonstrated that the magnetization originated from Fe 2+ cations, whereas Fe 3+ and Ti 4+ did not contribute. Films with the highest magnetic moment (0.8 μ B per Fe) had the highest measured Fe 2+ :Fe 3+ ratio of 0.1 corresponding to the largest concentration of oxygen vacancies (δ = 0.19). Postgrowth annealing treatments under oxidizing and reducing conditions demonstrated quenching and partial recovery of magnetism respectively, and a change in Fe valence states. In conclusion, the study elucidates the microscopic origin of magnetism in highly Fe-substituted SrTi 1–x Fe x O 3–δ perovskite oxides and demonstrates that the magnetic moment, which correlates with the relative content of Fe 2+ and Fe 3+ , can be controlled via the oxygen content, either during growth or by postgrowth annealing.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Complex transport and magnetism in inhomogeneous mixed valence Ce 3 Ir 4 Ge 13

We report the discovery of Ce 3 Ir 4 Ge 13 , a Remeika phase with a complex array of structural, electronic, and magnetic properties. In this work, our single crystal x-ray diffraction measurements show that Ce 3 Ir 4 Ge 13 forms in the tetragonally distorted $I4_1/amd$ space group, which has three distinct rare earth sites. The electrical resistivity is almost temperature independent over three decades in temperature, from 0.4 K to 400 K, while the Hall coefficient measurements are consistent with a low-carrier semimetal. Magnetic susceptibility measurements reveal an effective moment, $μ^\text{exp}_\text{eff} = 1.87μ_B/$Ce, that falls significantly short of the expected value for Ce 3+ , suggesting that two of the rare earth sites are occupied by magnetic Ce 3+ while the third is occupied by nonmagnetic Ce 4+ . Upon cooling, Ce 3 Ir 4 Ge 13 first enters a short range magnetically ordered state below $T_\text{SRO}$ = 10 K, marked by a deviation from Curie-Weiss behavior in susceptibility and a broad field-independent heat capacity anomaly. At lower temperatures, we observe a second, sharper peak in the heat capacity at $T^\ast$ = 1.7 K, concurrent with a splitting of the field-cooled and zero-field-cooled susceptibilities. A small resistivity drop at $T^\ast$ suggests a loss of spin disorder scattering consistent with a magnetic ordering or spin freezing transition. Ce 3 Ir 4 Ge 13 is therefore a rare example of an inhomogeneous mixed valence compound with a complex array of thermodynamic and transport properties.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Topological Mixed Valence Model for Twisted Bilayer Graphene

Song and Bernevig (SB) have recently proposed a topological heavy-fermion description of the physics of magic angle twisted bilayer graphene (MATBG), involving the hybridization of flat-band electrons with a relativistic conduction sea. Here, we explore the consequences of this model, seeking a synthesis of understanding drawn from heavy-fermion physics and MATBG experiments. Our work identifies a key discrepancy between measured and calculated on-site Coulomb interactions, implicating renormalization effects that are not contained in the current model. With these considerations in mind, we consider a SB model with a single, renormalized on-site interaction between the f electrons, containing a phenomenological heavy-fermion binding potential on the moiré A A sites. This feature allows the simplified model to capture the periodic reset of the chemical potential with filling and the observed stability of local moment behavior. We argue that a two-stage Kondo effect will develop in MATBG as a consequence of the relativistic conduction band: Kondo I occurs at high temperatures, establishing a coherent hybridization at the Γ points and a non-Fermi liquid of incoherent fermions at the moiré K points; at much lower temperatures, Kondo II leads to a Fermi liquid in the flat band. Utilizing an auxiliary-rotor approach, we formulate a mean-field treatment of MATBG that captures this physics, describing the evolution of the normal state across a full range of filling factors. By contrasting the relative timescales of phonons and valence fluctuations in bulk heavy-fermion materials with that of MATBG, we are led to propose a valley-polaron origin to the Coulomb renormalization and the heavy-fermion binding potential identified from experiment. We also discuss the possibility that the two-fluid, non-Fermi liquid physics of the relativistic Kondo lattice is responsible for the strange-metal physics observed in MATBG. Published by the American Physical Society 2025

Lau, Liam L. H. (ORCID:0000000166039088)↗
DOE OSTI2015

Analysis of orbital occupancy of valence neutron in {sup 15}C through Coulomb breakup reactions

The Coulomb breakup reactions {sup 208}Pb({sup 15}C, {sup 14}C + n){sup 208}Pb and {sup 181}Ta({sup 15}C, {sup 14}C + n){sup 181}Ta have been studied at 68 and 85 A MeV beam energies, respectively, within the framework of the eikonal approximation to investigate the orbital occupancy of valence neutron in the {sup 15}C nucleus. The outcomes of the present work favor 0{sup +} ⊗ 2s{sub 1/2} as the core-neutron coupling for the ground-state structure with 0.91 as a spectroscopic factor.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Probing Ultrafast Electron (De)localization Dynamics in Mixed Valence Complexes Using Femtosecond X-ray Spectroscopy (Final Report)

The central goal of this proposal was to directly visualize and quantify how electronic correlations, vibronic couplings, and local solute-solvent interactions control intramolecular electron motion on the femtosecond time scale. The proposed research program focused on solvated Ruthenium (Ru) based mixed-valence complexes, a prototypical class of transition-metal complexes, which are of significant interest for their potential applications in photochemical energy conversion. Electron movements following photochemical excitation are closely coupled with atomic/vibrational and solvent motion. To disentangle these various components requires tools designed to directly probe electron correlations and vibronic coupling (coherently coupled motions of electronic and vibrational coordinates) on the timescale of electron motion in the solution phase.

36 MATERIALS SCIENCE↗