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At least 145 records · Page 8
All sourcesNASA NTRSDOE OSTI
DOE OSTI2026

Codimension-two spiral spin liquid in the effective honeycomb-lattice compound Cs 3 ⁢Fe 2 ⁢Cl 9

A codimension-two spiral spin liquid is a correlated paramagnetic state with one-dimensional ground state degeneracy hosted within a three-dimensional lattice. Here, in this work, via neutron scattering experiments and numerical simulations, we establish the existence of a codimension-two spiral spin liquid in the effective honeycomb-lattice compound Cs 3 ⁢Fe 2⁢ Cl 9 , which demonstrates an alternate path to spiral spin liquids by overcoming the long-standing impediment of weak further-neighbor interactions. In the long-range ordered regime, competing spiral and spin density wave orders emerge as a function of applied magnetic field, among which a possible order-by-disorder transition is identified.

Monte Carlo methods↗
DOE OSTI2020

Spin Reversal of a Quantum Hall Ferromagnet at a Landau Level Crossing

When Landau levels (LLs) become degenerate near the Fermi energy in the quantum Hall regime, interaction effects can drastically modify the electronic ground state. Here, we study the quantum Hall ferromagnet formed in a two-dimensional hole gas around the LL filling factor v = 1 in the vicinity of a LL crossing in the heave-hole valence band. Cavity spectroscopy in the strong-coupling regime allows us to optically extract the spin polarization of the two-dimensional hole gas. By analyzing this polarization as a function of hole density and magnetic field, we observe a spin flip of the ferromagnet. Furthermore, the depolarization away from v = 1 accelerates close to the LL crossing. This is indicative of an increase in the size of skyrmion excitations as the effective Zeeman energy vanishes at the LL crossing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Defect Stability in CdTe Based on Formation Energies and Migration Barriers

Native point defects are thought to play a key role in CdTe, either as compensation centers in intentionally doped material, as a source of conductivity in nominally undoped material, or as electron–hole recombination centers. Here, the discussion of their concentration and impact has often centered only on formation energies and transition levels. Using hybrid density functional calculations, including the effects of spin–orbit coupling (SOC), we discuss the stability of native point defects in CdTe based on their formation energies and migration barriers. We show that although Cd interstitials are the lowest energy donor defects, they are unstable at room temperature due to a low migration barrier. They are important for maintaining charge neutrality during growth or annealing at high temperatures, but once the material is brought to room temperature, they are not frozen in as often assumed and are expected to anneal out, leaving the other more stable defects to determine the conductivity. Taking this into account in the solution of the charge neutrality equation, we are able to predict the conductivity type and carrier concentrations that are in good agreement with experimental observations.

14 SOLAR ENERGY↗
DOE OSTI2026

Non-Altermagnetic Origin of Exchange Bias Behaviors in Incoherent RuO 2 /Fe Bilayer Heterostructures

Initially identified as a promising altermagnetic (AM) candidate, rutile RuO 2 has since become embroiled in controversy due to contradictory findings of modeling and measurements of the magnetic properties of bulk crystals and thin films. For example, despite observations of a bulk nonmagnetic state using density functional theory, neutron scattering, and muon spin resonance measurements, patterned RuO 2 Hall bars and film heterostructures display magnetotransport signatures of magnetic ordering. Among the characteristics routinely cited as evidence for AM is the observation of exchange bias (EB) in an intimately contacted Fe-based ferromagnetic (FM) layer, which can arise due to interfacial coupling with a compensated antiferromagnet. Here, within this work, the origins of this EB coupling in Ru-capped RuO 2 /Fe bilayers are investigated using polarized neutron diffraction, polarized neutron reflectometry, cross-sectional transmission electron microscopy, and super conducting quantum interference device measurements. These experiments reveal that the EB behavior is driven by the formation of an iron oxide interlayer containing Fe 3 O 4 that undergoes a magnetic transition and pins interfacial moments within Fe at low temperature. These findings are confirmed by comparable measurements of Ni-based heterostructures, which do not display EB coupling, as well as magnetometry of additional Fe/Ru bilayers that display oxide-driven EB coupling despite the absence of the epitaxial RuO 2 layer. While these results do not directly refute the possibility of AM ordering in RuO 2 thin films, they reveal that EB, and related magnetotransport phenomena, cannot alone be considered evidence of this characteristic in the rutile structure due to interfacial chemical disorder.

RuO2↗
DOE OSTI2023

Investigation of local distortion effects on X-ray absorption of ferroelectric perovskites from first principles simulations

Understanding the role of ferroelectric polarization in modulating the electronic and structural properties of crystals is critical for advancing these materials for overcoming various technological and scientific challenges. However, due to difficulties in performing experimental methods with the required resolution, or in interpreting the results of methods therein, the nanoscale morphology and response of these surfaces to external electric fields has not been properly elaborated. Here, in this work, we investigate the effect of ferroelectric polarization and local distortions in a BaTiO 3 perovskite, using two widely used computational approaches which treat the many-body nature of X-ray excitations using different philosophies, namely the many-body, delta-self-consistent-field determinant (mb-ΔSCF) and the Bethe–Salpeter equation (BSE) approaches. We show that in agreement with our experiments, both approaches consistently predict higher excitations of the main peak in the O–K edge for the surface with upward polarization. However, the mb-ΔSCF approach mostly fails to capture the L 2,3 separations at the Ti–L edge, due to the absence of spin–orbit coupling in Kohn–Sham density functional theory (KS-DFT) at the generalized gradient approximation level. On the other hand, and most promising, we show that application of the GW/BSE approach successfully reproduces the experimental XAS, both the relative peak intensities as well as the L 2,3 separations at the Ti–L edges upon ferroelectric switching. Thus simulated XAS is shown to be a powerful method for capturing the nanoscale structure of complex materials, and we underscore the need for many-body perturbation approaches, with explicit consideration of core-hole and multiplet effects, for capturing the essential physics in these systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2020

Controlling magnetic order, magnetic anisotropy, and band topology in the semimetals Sr(Mn 0.9 Cu 0.1 )Sb 2 and Sr(Mn 0.9 Zn 0.1 )Sb 2

Neutron diffraction and magnetic susceptibility studies show that orthorhombic single-crystals of topological semimetals Sr(Mn 0.9 Cu 0.1 ) Sb 2 and Sr(Mn 0.9 Zn 0.1 )Sb 2 undergo three-dimensional C-type antiferromagnetic (AFM) ordering of the Mn 2+ moments at T N = 200 ± 10 and 210 ± 12 K, respectively, significantly lower than that of the parent SrMnSb 2 with T N = 297 ± 3 K. Magnetization versus applied magnetic field (perpendicular to MnSb planes) below T N exhibits slightly modified de Haas van Alphen oscillations for the Zn-doped crystal as compared to that of the parent compound. By contrast, the Cu-doped system does not show de Haas van Alphen magnetic oscillations, suggesting that either Cu substitution for Mn changes the electronic structure of the parent compound substantially, or that the Cu sites are strong scatterers of carriers that significantly shorten their mean free path thus diminishing the oscillations. Density functional theory (DFT) calculations including spin-orbit coupling predict the C-type AFM state for the parent, Cu-, and Zn-doped systems and identify the a -axis (i.e., perpendicular to the Mn layer) as the easy magnetization direction in the parent and 12.5% of Cu or Zn substitutions. In contrast, 25% of Cu content changes the easy magnetization to the b-axis (i.e., within the Mn layer). Here, we find that the incorporation of Cu and Zn in SrMnSb 2 tunes electronic bands near the Fermi level resulting in different band topology and semimetallicity. The parent and Zn-doped systems have coexistence of electron and hole pockets with opened Dirac cone around the Y-point whereas the Cu-doped system has dominant hole pockets around the Fermi level with a distorted Dirac cone. The tunable electronic structure may point out possibilities of rationalizing the experimentally observed de Haas van Alphen magnetic oscillations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Phonon dispersion throughout the iron spin crossover in ferropericlase

Ferropericlase (Fp), (Mg 1– x Fex)O, is the second most abundant phase in the Earth's lower mantle. At relevant pressure-temperature conditions, iron in Fp undergoes a high spin (HS), $\textit{S}$ = 2, to low spin (LS), $\textit{S}$ = 0, state change. The nature of this phenomenon is quite well understood now, but there are still basic questions regarding the structural stability and the existence of soft phonon modes during this iron state change. General theories exist to explain the volume reduction, the significant thermoelastic anomalies, and the broad nature of this HS-LS crossover. These theories make extensive use of the quasiharmonic approximation. Therefore, dynamical and structural stability is essential to their validity. Here, we investigate the vibrational spectrum of Fp throughout this spin crossover using ab initio density-functional theory $+U_{sc}$ calculations. We address vibrational modes associated with isolated and (second-)nearest-neighbor iron ions undergoing the HS-LS state change. As expected, acoustic modes of this solid solution are resilient, while optical modes are the most affected. In this work, we show that there are no soft phonon modes across this HS-LS crossover, and Fp is dynamically stable at all relevant pressures.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

In-beam γ-ray and electron spectroscopy of 249,251 Md

The odd-Z 251 Md nucleus was studied using combined γ-ray and conversion-electron in-beam spectroscopy. Besides the previously observed rotational band based on the [521]1/2 - configuration, another rotational structure has been identified using γ-γ coincidences. The use of electron spectroscopy allowed the rotational bands to be observed over a larger rotational frequency range. Using the transition intensities that depend on the gyromagnetic factor, a [514]7/2 - single-particle configuration has been inferred for this band, i.e., the ground-state band. A physical background that dominates the electron spectrum with an intensity of ≃60% was well reproduced by simulating a set of unresolved excited bands. Moreover, a detailed analysis of the intensity profile as a function of the angular momentum provided a method for deriving the orbital gyromagnetic factor, namely g K = $0.69$ $^{+0.19}_{-0.16}$ for the ground-state band. The odd-Z 249 Md was studied using γ-ray in-beam spectroscopy. Evidence for octupole correlations resulting from the mixing of the Δl = Δ j = 3 [521]3/2 - and [633]7/2 + Nilsson orbitals were found in both 249,251 Md. Here, a surprising similarity of the 251 Md ground-state band transition energies with those of the excited band of 255 Lr has been discussed in terms of identical bands. Lastly, Skyrme-Hartree-Fock-Bogoliubov calculations were performed to investigate the origin of the similarities between these bands.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Starting-point-independent quantum Monte Carlo calculations of iron oxide

Quantum Monte Carlo (QMC) methods are useful for studies of strongly correlated materials because they are many body in nature and use the physical Hamiltonian. Typical calculations assume as a starting point a wave function constructed from single-particle orbitals obtained from one-body methods, e.g., density functional theory. However, mean-field-derived wave functions can sometimes lead to systematic QMC biases if the mean-field result poorly describes the true ground state. In this study, we examine the accuracy and flexibility of QMC trial wave functions using variational and fixed-node diffusion QMC estimates of the total spin density and lattice distortion of antiferromagnetic iron oxide (FeO) in the ground state B1 crystal structure. We found that for relatively simple wave functions the predicted lattice distortion was controlled by the choice of single-particle orbitals used to construct the wave function, rather than by subsequent wave function optimization techniques within QMC. By optimizing the orbitals with QMC, we then demonstrate starting-point independence of the trial wave function with respect to the method by which the orbitals were constructed by demonstrating convergence of the energy, spin density, and predicted lattice distortion for two qualitatively different sets of orbitals. The results suggest that orbital optimization is a promising method for accurate many-body calculations of strongly correlated condensed phases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Symmetry-correct bonding in density functional theory calculations for delta phase Pu

The long-held conclusion that magnetic order in delta phase Pu makes the structure mechanically unstable in density functional theory calculations is incorrect if the magnetic order is allowed to be non-collinear. The non-collinear 3Q spin structure is intrinsically cubic and makes all structurally equivalent bonds equivalent in their bonding character. Applied to density functional theory calculations on delta phase Pu, the 3Q spin structure results in elastic constants and phonons with the correct symmetry. Finally, the calculated phonon dispersion agrees better with experiment than previous calculations, and the calculated thermal expansion shows the unique behavior seen experimentally: it is negative.

36 MATERIALS SCIENCE↗
DOE OSTI2022

$\textit{J}$ = 0 nonmagnetic insulating state in K 2 OsX 6 ($\textit{X}$ = F, Cl, and Br)

In 4$\textit{d}$ /5$\textit{d}$ transition-metal systems, many interesting physical properties arise from the interplay of bandwidth, electronic correlations, and spin-orbit interactions. Here, using ab initio density functional theory, we systematically study the double-perovskite-like system K 2 OsX6 ($\textit{X}$ = F, Cl, and Br) with a $5d^4$ electronic configuration. In this work, our main result is that the $\textit{J}$ = 0 nonmagnetic insulating state develops in this system, induced by strong spin-orbit coupling (SOC). Specifically, the well-separated OsX 6 octahedra lead to the cubic crystal-field limit and result in dramatically decreasing hoppings among nearest neighbor Os-Os sites. In this case, the three degenerate $t_{2g}$ orbitals are reconstructed into two “effective” $j_{\text{eff}}$ ($j_{\text{eff}}$ = 1/2 and $j_{\text{eff}}$ = 3/2 states) states separated by the strong SOC, opening a gap with four electrons occupying the$j_{\text{eff}}$ = 3/2 orbitals. Furthermore, the hybridization between the Os 5$\textit{d}$ orbitals and the $\textit{X}$ ($\textit{X}$ = F, Cl, and Br) $\textit{p}$ orbitals increases from F to Br, leading the electrons in K 2 OsF 6 to be more localized than in K 2 OsCl 6 and K 2 OsBr 6 , resulting in a smaller bandwidth for K 2 OsF 6 than in the Cl- or Br-cases. Our results provide guidance to experimentalists and theorists working on this interesting family of osmium halides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Strongly anisotropic electronic and magnetic structures in oxide dichlorides RuOCl 2 and OsOCl 2

The van der Waals oxide dichlorides MOX 2 (M=V, Ta, Nb, Ru, and Os; X=halogen element), with different electronic densities, are attracting considerable attention. Ferroelectricity, spin-singlet formation, and orbital-selective Peierls phases were reported in this family with d 1 or d 2 electronic configurations, all believed to be caused by the strongly anisotropic electronic orbital degree of freedom. Here, using density functional theory and density matrix renormalization group methods, we investigate the electronic and magnetic properties of RuOCl 2 and OsOCl 2 with d 4 electronic configurations. Different from a previous study using VOI 2 with d 1 configuration, these systems with 4d4 or 5d4 do not exhibit a ferroelectric instability along the a axis. Due to the fully occupied dxy orbital in RuOCl 2 and OsOCl 2 , the Peierls instability distortion disappears along the b axis, leading to an undistorted Immm phase (No. 71). Furthermore, we observe strongly anisotropic electronic and magnetic structures along the a axis. For this reason, the materials of our focus can be regarded as “effective one-dimensional” systems even when they apparently have a dominant two-dimensional lattice geometry. The large crystal-field splitting energy (between dxz/yz and dxy orbitals) and large hopping between nearest-neighbor Ru and Os atoms suppresses the J = 0 singlet state in MOCl 2 (M=Ru or Os) with electronic density n = 4, resulting in a spin-1 system. Moreover, we find staggered antiferromagnetic order with π wave vector along the M-O chain direction (a axis) while the magnetic coupling along the b axis is weak. Based on Wannier functions from first-principles calculations, we calculated the relevant hopping amplitudes and crystal-field splitting energies of the t 2g orbitals for the Os atoms to construct a multiorbital Hubbard model for the M-O chains. Staggered AFM with ↑|-|↓-↑|-|↓ spin structure dominates in our density matrix renormalization group calculations, in agreement with density functional theory calculations. Our results for RuOCl 2 and OsOCl 2 provide guidance to experimentalists and theorists working on this interesting family of oxide dichlorides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

4 d element induced improvement of structural disorder and development of weakly reentrant spin-glass behavior in NiRuMnSn

The pursuit of efficient spin polarization in quaternary Heusler alloys with the general formula XX'YZ (where X, X', and Y are transition metals and Z is a p-block element) has been a subject of significant scientific interest. While previous studies showed that isoelectronic substitution of a 4d element in place of a 3d element in quaternary Heusler alloys improves the half-metallic ferromagnetic characteristics, our research here, on the quaternary Heusler alloy NiRuMnSn, reveals a strikingly different scenario. In this study, we present a detailed structural analysis of the material using x-ray absorption fine structure and neutron diffraction techniques which confirms the formation of a single-phase compound with 50:50 site disorder between Ni and Ru atoms at 4c and 4d sites. Contrary to expectations, our density functional theory calculations suggest a considerable decrease in spin polarization even in the ordered structure. Additionally, we report on the compound's exceptional behavior, displaying a rare reentrant spin-glass property below ~ 60 K, a unique and intriguing feature for quaternary Heusler-type compounds.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Zero-Field Splitting Calculations by Multiconfiguration Pair-Density Functional Theory

Zero-field splitting (ZFS) is a fundamental molecular property that is especially relevant for single-molecule magnets (SMMs), electron paramagnetic resonance spectra, and quantum computing. Developing a method that can accurately predict ZFS parameters can be very powerful for designing new SMMs. One of the challenges is to include external correlation in an inherently multiconfigurational open-shell species for the accurate prediction of magnetic properties. Previously available methods depend on expensive multireference perturbation theory calculations to include external correlation. In this paper, we present spin-orbit-inclusive multiconfiguration and multistate pair-density functional theory (MC-PDFT) calculations of ZFSs; these calculations have a cost comparable to complete-active-space self-consistent field (CASSCF) theory, but they include correlation external to the active space. We found that combining a multistate formulation of MC-PDFT, namely, compressed-state multistate pair-density functional theory, with orbitals optimized by weighted-state-averaged CASSCF, yields reasonably accurate ZFS results

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

Spin qubit properties of the boron-vacancy/carbon defect in the two-dimensional hexagonal boron nitride

Spin qubit defects in two-dimensional materials have a number of advantages over those in three-dimensional hosts including simpler technologies for defect creation and control, as well as qubit accessibility. In this work, we select the V B C B defect in the hexagonal boron nitride (hBN) as a possible optically controllable spin qubit and explain its triplet ground state and neutrality. In this defect a boron vacancy is combined with a carbon dopant substituting the closest boron atom to the vacancy. Our density-functional-theory calculations confirmed that the system has dynamically stable spin triplet and singlet ground states. As revealed from our linear response GW calculations, the spin-sensitive electronic states are localized around the three undercoordinated N atoms and make local peaks in the density of electronic states within the bandgap. Using the triplet and singlet ground state energies, as well as the energies of the optically excited states, obtained from solution to the Bethe–Salpeter equation, we construct the spin-polarization cycle, which is found to be favorable for the spin qubit initialization. The calculated zero-field splitting parameters ensure that the splitting energy between the spin projections in the triplet ground state is comparable to that of the known spin qubits. We thus propose the V B C B defect in hBN as a promising spin qubit.

2D BN↗
DOE OSTI2021

Engineering local strain for single-atom nuclear acoustic resonance in silicon

Mechanical strain plays a key role in the physics and operation of nanoscale semiconductor systems, including quantum dots and single-dopant devices. In this report we describe the design of a nanoelectronic device, where a single nuclear spin is coherently controlled via nuclear acoustic resonance (NAR) through the local application of dynamical strain. The strain drives spin transitions by modulating the nuclear quadrupole interaction. We adopt an AlN piezoelectric actuator compatible with standard silicon metal–oxide–semiconductor processing and optimize the device layout to maximize the NAR drive. We predict NAR Rabi frequencies of order 200 Hz for a single 123Sb nucleus in a wide region of the device. Spin transitions driven directly by electric fields are suppressed in the center of the device, allowing the observation of pure NAR. Using electric field gradient-elastic tensors calculated by the density-functional theory, we extend our predictions to other high-spin group-V donors in silicon and to the isoelectronic 73Ge atom.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Orbital selective spin waves in detwinned NaFeAs

The existence of orbital-dependent electronic correlations has been recognized as an essential ingredient to describe the physics of iron-based superconductors. NaFeAs, a parent compound of iron-based superconductors, exhibits a tetragonal-to-orthorhombic lattice distortion below T s ≈ 60 K, forming an electronic nematic phase with two 90° rotated (twinned) domains, and orders antiferromagnetically below T N ≈ 42 K. We use inelastic neutron scattering to study spin waves in uniaxial pressure-detwinned NaFeAs. By comparing the data with combined density functional theory and dynamical mean-field theory calculations, we conclude that spin waves up to an energy scale of E crossover ≈ 100 meV are dominated by d yz -d yz intraorbital scattering processes, which have the twofold (C 2 ) rotational symmetry of the underlying lattice. On the other hand, the spin wave excitations above E crossover , which have approximately fourfold (C 4 ) rotational symmetry, arise from the d xy -d xy intraorbital scattering that controls the overall magnetic bandwidth in this material. In addition, we find that the low-energy (E ≈ 6 meV) spin excitations change from approximate C 4 to C 2 rotational symmetry below a temperature T* (>T s ), while spin excitations at energies above E crossover have approximate C 4 rotational symmetry and are weakly temperature dependent. Here, these results are consistent with angle-resolved photoemission spectroscopy measurements, where the presence of a uniaxial strain necessary to detwin NaFeAs also raises the onset temperature T* of observable orbital-dependent band splitting to above T s , thus supporting the notion of orbital selective spin waves in the nematic phase of iron-based superconductors.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Tuning spin–orbit coupling in (6,5) single-walled carbon nanotube doped with sp 3 defects

Single-walled carbon nanotubes (SWCNTs) containing sp 3 defects are a promising class of optoelectronic materials with bright photoluminescence and demonstrated single-photon emission. Using density functional theory simulations, complemented by measurements, we investigate the electronic structure of a series of quantum defects attached to (6,5) SWCNT with the goal of tuning the spin–orbit coupling by introduction of a heavy atom in the defect structure. We characterize the ground state electronic and spin properties of four synthesized and three potential defects on the tube and find that all of the synthesized defects considered introduce a localized midgap defect-centered state containing a single electron, ≈0.2–0.3 eV above the valence band. The spin density is located at the sp 3 defect site with negligible spin–orbit coupling even with the presence of a Pd atom. Three additional functional groups were tested via computation to increase spin localization near the metal, thereby increasing spin–orbit coupling. We predict that only the chlorodiphosphanepalladium(II)– [Cl(PH 3 ) 2 Pd(II)–] defect results in increased spin–orbit splitting of the defect state and the conduction band associated with the pristine-like SWCNT, a measure of the spin–orbit coupling of excited state transitions. This study suggests that for unpassivated sp 3 defects in (6,5) SWCNT, forming a direct bond between a heavy atom and the sp 3 carbon allows for tuning of spin–orbit coupling.

74 ATOMIC AND MOLECULAR PHYSICS↗