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At least 325 records · Page 18
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Charge self-consistent density functional theory plus ghost rotationally invariant slave-boson theory for correlated materials

We present a charge self-consistent density functional theory combined with the ghost rotationally invariant slave-boson (DFT+gRISB) formalism for studying correlated materials. Here, this method is applied to SrVO 3 and NiO, representing prototypical correlated metals and charge-transfer insulators. For SrVO 3 , we demonstrate that DFT+gRISB yields an accurate equilibrium volume and effective mass close to experimentally observed values. Regarding NiO, DFT+gRISB enables the simultaneous description of charge-transfer and Mott-Hubbard bands, significantly enhancing the accuracy of the original DFT+RISB approach. Furthermore, the calculated equilibrium volume and spectral function reasonably agree with experimental observations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Anisotropic c – f Hybridization in the Ferromagnetic Quantum Critical Metal CeRh 6 Ge 4

Heavy fermion compounds exhibiting a ferromagnetic quantum critical point have attracted considerable interest. Common to two known cases, i.e., CeRh 6 Ge 4 and YbNi 4 P 2 , is that the 4f moments reside along chains with a large interchain distance, exhibiting strong magnetic anisotropy that was proposed to be vital for the ferromagnetic quantum criticality. Here, we report an angle-resolved photoemission study on CeRh 6 Ge 4 in which we observe sharp momentum-dependent 4f bands and clear bending of the conduction bands near the Fermi level, indicating considerable hybridization between conduction and 4f electrons. The extracted hybridization strength is anisotropic in momentum space and is obviously stronger along the Ce chain direction.The hybridized 4f bands persist up to high temperatures, and the evolution of their intensity shows clear band dependence. Our results provide spectroscopic evidence for anisotropic hybridization between conduction and 4f electrons in CeRh 6 Ge 4 , which could be important for understanding the electronic origin of the ferromagnetic quantum criticality.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Unusual Exchange Couplings and Intermediate Temperature Weyl State in Co 3 Sn 2 S 2

Understanding magnetism and its possible correlations to topological properties has emerged to the forefront as a difficult topic in studying magnetic Weyl semimetals. Co 3 Sn 2 S 2 is a newly discovered magnetic Weyl semimetal with a kagome lattice of cobalt ions and has triggered intense interest for rich fantastic phenomena. In this study, we report the magnetic exchange couplings of Co 3 Sn 2 S 2 using inelastic neutron scattering and two density functional theory (DFT) based methods: constrained magnetism and multiple-scattering Green’s function methods. Co 3 Sn 2 S 2 exhibits highly anisotropic magnon dispersions and linewidths below T C , and paramagnetic excitations above T C . The spin-wave spectra in the ferromagnetic ground state is well described by the dominant third-neighbor “across-hexagon” J d model. Our density functional theory calculations reveal that both the symmetry-allowed 120° antiferromagnetic orders support Weyl points in the intermediate temperature region, with distinct numbers and the locations of Weyl points. Our study highlights the important role Co 3 Sn 2 S 2 can play in advancing our understanding of kagome physics and exploring the interplay between magnetism and band topology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Tuning the flat bands of the kagome metal CoSn with Fe, In, or Ni doping

We report CoSn is a Pauli paramagnet with relatively flat d bands centered about 100 meV below the Fermi energy, E F . Single crystals of CoSn lightly doped with Fe, In, or Ni are investigated using x-ray and neutron scattering, magnetic susceptibility and magnetization, AC susceptibility, specific heat, and resistivity measurements. Within the rigid-band approximation, hole doping with a few percent of Fe or In should move the flat bands closer to E F , whereas electron doping with Ni should move the flat bands further away from E F . We provide evidence that this indeed occurs. Fe and In doping drive CoSn toward magnetism, while Ni doping suppresses CoSn's already weak magnetic response. The resulting ground state is different for Fe versus In doping. For Fe-doped crystals, Co 1-x Fe x Sn, with 0.02< x <0.27, the magnetic and specific-heat data are consistent with the formation of a spin glass, with a glass temperature, T g , ranging from 1 K for x = 0.02 to 10 K for x = 0.27. Powder and single-crystal neutron diffraction found no evidence of long-range magnetic order below T g for samples with x ≈ 0.17. For In-doped crystals, CoSn 1-y In y , both the magnetic susceptibility and the Sommerfeld coefficient, γ, increase substantially relative to pure CoSn, but with no clear indication of a magnetic transition for 0.05< y <0.2. CoSn crystals doped with Ni (Co 0.93 Ni 0.07 Sn) have a significantly smaller magnetic susceptibility and γ than pure CoSn, consistent with flat bands further from E F .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
NASA NTRS1991

Microgravity Program strategic plan, 1991

The all encompassing objective of the NASA Microgravity Program is the use of space as a lab to conduct research and development. The on-orbit microgravity environment, with its substantially reduced buoyancy forces, hydrostatic pressures, and sedimentation, enables the conduction of scientific studies not possible on Earth. This environment allows processes to be isolated and controlled with an accuracy that cannot be obtained in the terrestrial environment. The Microgravity Science and Applications Div. has defined three major science categories in order to develop a program structure: fundamental science, including the study of the behavior of fluids, transport phenomena, condensed matter physics, and combustion science; materials science, including electronic and photonic materials, metals and alloys, and glasses and ceramics; and biotechnology, focusing on macromolecular crystal growth as well as cell and molecular science. Experiments in these areas seek to provide observations of complex phenomena and measurements of physical attributes with a precision that is enabled by the microgravity environment.

Source record↗
DOE OSTI2025

Anomalous elastic softening in ferroelectric hafnia under pressure

his study employs first-principles density-functional theory (DFT) calculations to explore the elastic and mechanical properties of ferroelectric hafnia (HfO 2 ) in its polar orthorhombic 𝑃⁢𝑐⁢𝑎⁢2 1 phase under varying hydrostatic pressure conditions up to 30 GPa. Utilizing a plane-wave basis set and Perdew-Burke-Ernzerhof generalized-gradient approximation for solids in our DFT calculations, we investigate both pure and yttrium-substituted HfO 2 . Our findings reveal an anomalous reduction in the 𝐶 33 component of the elastic tensor with increasing pressure, which becomes significant above 15 GPa and signals a potential pressure-driven structural phase transition at higher pressure. The analysis of atomic displacements under pressure sheds light on the unusual mechanical behavior and phase stability of this material. Additionally, we observe a transition from an indirect band gap to a direct band gap with increasing pressure, which could have significant implications for optical applications. Here, the effects of yttrium substitution on the mechanical and electronic properties are further examined, revealing that yttrium substitution softens the elastic response of this material and reduces the electronic band gap. These results enhance our understanding of elastic and mechanical responses of ferroelectric hafnia and its potential for applications in microelectronics, piezoelectric devices, and nonvolatile ferroelectric random-access memories. Further experimental validation is recommended to confirm our predictions and explore the practical implications of the observed phase transitions and electronic behavior of the ferroelectric hafnia under high-pressure conditions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Surface preparation method for investigating the three-dimensional electronic structure of perovskite nickelates

The investigation of the electronic structures on perovskite oxides using surface-sensitive spectroscopy techniques is often hindered by their “uncleavable” nature, typically requiring expensive and complex in situ experimental setups that integrate the capabilities of sample synthesis and spectroscopy measurement under ultrahigh vacuum condition. Here, we address this challenge by developing an ozone-annealing process that yields atomically flat surfaces on perovskite oxide thin films, making them suitable for high-resolution angle-resolved photoemission spectroscopy measurements. Using this method, we present a three-dimensional electronic structure study of Nd 1−𝑥 ⁢Sr 𝑥 ⁢NiO 3 (𝑥=0 and 0.175) thin films with unprecedented accuracy. The experimentally determined low-energy fermiology exhibits quantitative agreements with two-band tight-binding simulations, which is further validated by first-principles calculations considering the material's actual crystal structure. This work provides an accessible approach for ex situ ARPES measurements on perovskite oxides and other strongly correlated oxides, including the recently discovered high-𝑇 c nickelates.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Oxygen vacancy induced site-selective Mott transition in LaNiO 3

While defects such as oxygen vacancies in correlated materials can modify their electronic properties dramatically, understanding the microscopic origin of electronic correlations in materials with defects has been elusive. Lanthanum nickelate with oxygen vacancies, LaNiO 3 - x , exhibits the metal-to-insulator transition as the oxygen vacancy level x increases from the stoichiometric LaNiO 3 . In particular, LaNiO 2.5 exhibits a paramagnetic insulating phase, also stabilizing an antiferromagnetic state below T N ≃ 152 K . Here, we study the electronic structure and energetics of LaNiO 3 - x using first principles. We find that LaNiO 2.5 exhibits a “site-selective” paramagnetic Mott insulating state at T ≃ 290 K as obtained using density functional theory plus dynamical mean field theory ( DFT + DMFT ). The Ni octahedron site develops a Mott insulating state with strong correlations as the Ni e g orbital is half-filled while the Ni square-planar site with apical oxygen vacancies becomes a band insulator. Overall, our oxygen vacancy results cannot be explained by the pure change of the Ni oxidation state alone within the rigid band-shift approximation. Our DFT + DMFT density of states explains that the peak splitting of unoccupied states in LaNiO 3 - x measured by the experimental x-ray absorption spectra originates from two nonequivalent Ni ions in the vacancy-ordered structure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Singly occupied 4⁢𝑓 antiferromagnetic insulators: CePO 4 and CeVO 4

Rare-earth containing wide band gap oxides, which provide spin-photon interface and narrow linewidth optical emission, are getting significant attention as the most promising candidate materials in advancing quantum transduction and memories. Here, in this work, from ab initio calculations, we identify antiferromagnetic ground states in structurally preferred monoclinic CePO 4 and tetragonal CeVO 4 exhibiting localized occupied and unoccupied Ce 4⁢𝑓 states with 4⁢𝑓−4⁢𝑓 transition characteristics. Interestingly, in CePO 4 , O 2⁢𝑝 and P 3⁢𝑝 states hybridize negligibly with Ce 4⁢𝑓 states, while in CeVO 4 , V 3⁢𝑑 and O 2⁢𝑝 states hybridize and appear as extended states in between the occupied and unoccupied Ce 4⁢𝑓 states. Here, phonon calculations and analysis identify and differentiate Raman active phonon modes along with the spin phonon coupling of Ce in both CePO 4 and CeVO 4 that ultimately lead to different 4⁢𝑓 ground-state crystal-field multiplets, which are critical to accurately describe electronic transitions for foundational quantum transduction and memories. Further, the identified 𝐶 1 site symmetry of Ce, lacking inversion symmetry in CePO 4 , is relevant for quantum memories and 𝐷 2⁢𝑑 site symmetry of Ce exhibiting inversion symmetry in CeVO 4 is relevant for quantum transduction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Two-level systems in nucleated and non-nucleated epitaxial alpha-tantalum films

Building usefully coherent superconducting quantum processors depends on reducing losses in their constituent materials. Tantalum, like niobium, has proven utility as the primary superconducting layer within highly coherent qubits. However, unlike Nb, high temperatures are typically used to stabilize the desirable body-centered-cubic phase, α-Ta, during thin film deposition. It has long been known that a thin Nb layer permits the room-temperature nucleation of α-Ta, but here we observe the epitaxial process and present few-photon microwave loss measurements in Nb-nucleated Ta films. We compare resonators patterned from Ta films grown at high temperature (500 °C) and films nucleated at room temperature, in order to understand the impact of the crystalline order on quantum coherence. In both cases, films grew with Al 2 O 3 (001) ∥ Ta (110), indicating that the epitaxial orientation is independent of temperature and is preserved across the Nb/Ta interface. We use conventional low-power spectroscopy to measure two level system (TLS) loss as well as an electric-field bias technique to measure the effective dipole moments of TLS in the surfaces of resonators. In our measurements, Nb-nucleated Ta resonators had greater loss tangent (1.5 ± 0.1 × 10 -5 ) than non-nucleated (5 ± 1× 10 -6 ) in approximate proportion to defect densities as characterized by x-ray diffraction (0.27° vs 0.18° [110] reflection width) and electron microscopy (30 vs 70 nm domain size). Furthermore, the dependence of the loss tangent on domain size indicates that the development of more ordered Ta films is likely to lead to improvements in qubit coherence times. Moreover, low-temperature α-Ta epitaxy may enable the growth of microstate-free heterostructures, which would not withstand high temperature processing.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Effect of the electronic charge gap on LO bond-stretching phonons in undoped La 2 CuO 4 calculated using LDA + U

Typical density-functional theory calculations that wrongly predict undoped cuprates to be metallic also predict Cu-O half- and full-breathing phonon energies that are significantly softer than observed, presumably because of weak on-site Coulomb repulsion on the Cu 3d orbitals. We used DFT+U calculations with antiferromagnetic supercells of La 2 CuO 4 to establish correlation between the on-site repulsion strength, tuned via adjusting the value of U, and phonon dispersions. Here, we find that breathing and half-breathing phonons reach experimental values when U is tuned to obtain the correct optical gap and magnetic moments. We demonstrate that using distorted supercells within DFT+U is a promising framework to model phonons in undoped cuprates and other perovskite oxides with complex, interrelated structural and electronic degrees of freedom.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Electronic structure of chromium trihalides beyond density functional theory

In this work, we explore the electronic band structure of freestanding monolayers of chromium trihalides Cr X 3 , X = Cl, Br, I, within an advanced ab initio theoretical approach based on the use of Green's function functionals. We compare the local density approximation with the quasiparticle self-consistent GW (QS GW ) approximation and its self-consistent extension ( QS G W ^ ) by solving the particle-hole ladder Bethe-Salpeter equations to improve the effective interaction W . We show that, at all levels of theory, the valence band consistently changes shape in the sequence Cl → Br → I , and the valence band maximum shifts from the M point to the Γ point. By analyzing the dynamic and momentum-dependent self-energy, we show that QS G W ^ adds to the localization of the systems in comparison with QS GW , thereby leading to a narrower band and reduced amount of halogens in the valence band manifold. Further analysis shows that X = Cl is most strongly correlated, and X = I is least correlated (most bandlike) as the hybridization between Cr d and X p enhances in the direction Cl → Br → I . For CrBr 3 and CrI 3 , we observe remarkable differences between the QS GW and QS G W ^ valence band structures, while their eigenfunctions are very similar. We show that weak perturbations, like moderate strain, weak changes to the d - p hybridization, and adding small U , can flip the valence band structures between these two solutions in these materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Quantum-limit phenomena and band structure in the magnetic topological semimetal EuZn 2 As 2

The interplay between magnetism and electronic topology in the quantum limit is a forefront subject of condensed matter physics. Here, we show the electronic and magnetic properties of layered antiferromagnet EuZn 2 As 2 in pulsed magnetic fields up to 60 T and temperatures down to 0.6 K. By analyzing the quantum oscillations observed in the magnetoresistance (MR) and proximity detector oscillator (PDO) frequency, we find that (1) the oscillation frequency F = 46 ± 6 T for H // c and 42 ± 2 T for H // ab; (2) the corresponding Berry phase is close to π for H // c, implying a nontrivial topology; and (3) the large linear MR occurs beyond the first Landau level, without any sign of saturation. From these observations, we conclude that the linear MR can be understood by considering diffusing cyclotron centers due to compressed Landau wavefunction, an emergent behavior in the quantum limit.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic correlation induced expansion of Fermi pockets in δ-plutonium

Plutonium is a critically important material as the behavior of its 5f electrons stands midway between the metalliclike itinerant character of the light actinides and localized atomic-core-like character of the heavy actinides. The δ phase of plutonium (δ-Pu), whereas still itinerant, has a large coherent Kondo peak and strong electronic correlations coming from its near-localized character. Here, using sophisticated Gutzwiller wave function and dynamical mean-field theory correlated theories, we study the Fermi surface and associated mass renormalizations of δ-Pu together with calculations of the de Haas–van Alphen frequencies. We find a large (~200%) correlation induced volume expansion in both the hole and the electron pockets of the Fermi surface in addition to an intermediate mass enhancement. All of the correlated electron theories predict, approximately, the same hole pocket placement in the Brillouin zone, which is different from that obtained in conventional density-functional band-structure theory, whereas the electron pockets from all theories are in, roughly, the same place.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Electronic structure of Humble defects in Ge and Ge 0.8⁢ Si 0.2

The group-IV diamond-structure elements are known to host a variety of planar defects, including {001} planar defects in C and {001}, {111}, and {113} planar defects in Si and Ge. Among the {001} planar defects, the Humble defect, known for some time to occur in Ge, has recently also been observed in Si-Ge alloys, but the details of its electronic structure remain poorly understood. Here, in this work, we perform first-principles density-functional calculations to study Humble defects in both Ge and Ge 0.8⁢ Si 0.2 . We also measure the Si L 2,3 -edge electron energy-loss spectra both at the defect and in a bulk-like region far from the defect and compare with theoretical calculations on corresponding Si sites in our first-principles calculations. We find that inclusion of core-hole effects in the theory is essential for reproducing the observed L 2,3 edge spectra, and that once they are included, the results provide a set of fingerprints for different types of local atomic bonding environments in Ge 0.8⁢ Si 0.2 . Our first-principles calculations reveal that the Humble defects have a tendency to enlarge the electronic band gap, which may have potential uses in band engineering. The use of hybrid functionals for an improved description of the band gap in these systems is also discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

The Li–F–H ternary system at high pressures

Evolutionary crystal structure prediction searches have been employed to explore the ternary Li-F-H system at 300 GPa. Metastable phases were uncovered within the static lattice approximation, with LiF 3 H 2 , LiF 2 H, Li 3 F 4 H, LiF 4 H 4 , Li 2 F 3 H and LiF 3 H lying within 50 meV/atom of the 0 K convex hull. All of these phases contain H n F¯ n+1 (n = 1; 2) anions, and Li + cations. Other structural motifs such as LiF slabs, $H$ $^{+}_{3}$ molecules and F δ- ions are present in some of the low enthalpy Li-F-H structures. The bonding within the H n F¯ n+1 molecules, which may be bent or linear, symmetric or asymmetric, is analyzed. The five phases closest to the hull are insulators, while LiF 3 H is metallic and predicted to have a vanishingly small superconducting critical temperature. Li 3 F 4 H is predicted to be stable at zero pressure. Furthermore, this study lays the foundation for future investigations of the role of temperature and anharmonicity on the stability and properties of compounds and alloys in the Li-F-H ternary system.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Photoluminescence, photophysics, and photochemistry of the V B - defect in hexagonal boron nitride

Extensive photochemical and spectroscopic properties of the V B - defect in hexagonal boron nitride are calculated, concluding that the observed photoemission associated with recently observed optically detected magnetic resonance is most likely of (1) 3 E'' → (1) 3 A' 2 origin. Rapid intersystem crossing from the defect's triplet to singlet manifolds explains the observed short excited-state lifetime and very low quantum yield. New experimental results reveal smaller intrinsic spectral bandwidths than previously recognized, interpreted in terms of spectral narrowing and zero-phonon-line shifting induced by the Jahn-Teller effect. Different types of computational methods are applied to map out the complex triplet and singlet defect manifolds, including the doubly ionized formulation of the equation-of-motion coupled-cluster theory that is designed to deal with the open-shell nature of defect states, and mixed quantum-mechanics/molecular-mechanics schemes enabling 5763-atom simulations. Finally, two other energetically feasible spectral assignments from among the singlet and triplet manifolds are considered, but ruled out based on inappropriate photochemical properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗