Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “spin orbit coupling”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Resonant inelastic x-ray scattering investigation of Hund's and spin-orbit coupling in 5 d 2 double perovskites

𝐵 site ordered 5⁢𝑑 2 double perovskites (𝐴 2 ⁢𝐵⁢𝐵′⁢O 6 , 𝐵′ = 5⁢𝑑 2 ) display a remarkable range of physical properties upon variation of the chosen 𝐵 and 𝐵′ site ions. This sensitivity to chemical substitution reflects the delicate balance and profound impact of strong electronic correlation and spin-orbit coupling in such systems. Here, we present rhenium 𝐿 2 and 𝐿 3 resonant inelastic x-ray scattering (RIXS) measurements of two such physically dissimilar materials, Mott-insultating Ba 2⁢ Y⁢Re⁢O 6 and semiconducting Sr 2⁢ Cr⁢Re⁢O 6 . Despite these differences, our RIXS results reveal similar energy scales of Hund's (𝐽 𝐻 ) and spin-orbit coupling (𝜁) in the two materials, with both systems firmly in the intermediate Hund's coupling regime where 𝐽 𝐻 /𝜁∼1. However, there are clear differences in their RIXS spectra. The conductive character of Sr 2⁢ Cr⁢Re⁢O 6 broadens and obfuscates the atomic transitions within an electron-hole continuum, while the insulating character of Ba 2 ⁢Y⁢Re⁢O 6 results in sharp atomic excitations. This contrast in their RIXS spectra despite their similar energy scales reflects a difference in the itinerancy-promoting hopping integral and illustrates the impact of the local crystal environment in double perovskites. Finally, 𝐿 2 and 𝐿 3 edge analyses of the atomic excitations in Ba 2 ⁢Y⁢Re⁢O 6 reveal that the ordering of the low lying excited states is inverted compared to previous reports, such that the appropriate energy scales of Hund's and spin-orbit coupling are significantly modified. We present exact diagonalization calculations of the RIXS spectra at both edges which show good agreement with our results for new energy scales of 𝜁 = 0.290⁢(5)⁢eV and 𝐽 𝐻 = 0.38⁢(2)⁢eV [𝐽 𝐻 /𝜁 = 1.30⁢(5)].

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Topological Superconductivity Based on Antisymmetric Spin–Orbit Coupling

Topological superconductivity (TSC) has drawn much attention for its fundamental interest and application in quantum computation. An outstanding challenge is the lack of intrinsic TSC materials with a p-wave pairing gap, which has led to the development of an effective p-wave theory of coupling s-wave gap with Rashba spin–orbit coupling (RSOC). However, the RSOC-strict mechanism and materials pose still both fundamental and practical limitations. Here, we generalize this theory to antisymmetric SOC (ASOC). Using k·p perturbation theory, we demonstrate that 2D crystals, with point groups of C 2 , C 4 , C 6 , C 2v , C 4v , C 6v , D 2 , D 4 , D 6 , S 4 , or D 2d , can all facilitate the desired ASOC. Remarkably, this enables us to discover 314 TSC candidates by screening 2D material databases, which are further confirmed by first-principles calculations of Majorana boundary modes and the topological invariant of the superconducting gap. As a result, our work fundamentally enriches TSC theory and greatly expands the classes of TSC materials for experimental exploration.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Rashba spin-orbit coupling enhanced magnetoresistance in junctions with one ferromagnet

We explain how Rashba spin-orbit coupling (SOC) in a two-dimensional electron gas (2DEG), or in a conventional s-wave superconductor, can lead to a large magnetoresistance even with one ferromagnet. However, such enhanced magnetoresistance is not generic and can be nonmonotonic and change its sign with Rashba SOC. For an in-plane rotation of magnetization, it is typically negligibly small for a 2DEG and depends on the perfect transmission which emerges from a spin-parity-time symmetry of the scattering states, while this symmetry is generally absent from the Hamiltonian of the system. The key difference from considering the normal-state magnetoresistance is the presence of the spin-dependent Andreev reflection at superconducting interfaces. In the fabricated junctions of quasi-2D van der Waals ferromagnets with conventional s-wave superconductors (Fe 0.29 ⁢TaS 2 /NbN) we find another example of enhanced magnetoresistance where the presence of Rashba SOC reduces the effective interfacial strength and is responsible for an equal-spin Andreev reflection. The observed nonmonotonic trend in the out-of-plane magnetoresistance with the interfacial barrier is an evidence for the proximity-induced equal-spin-triplet superconductivity.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Spin-orbit coupling controlled ground states in the double perovskite iridates $\textit{A}_2\textit{B}$IrO$_6$ ($\textit{A}$ = Ba, Sr; $\textit{B}$ = Lu, Sc)

Iridates with the 5$d^4$ electronic configuration have attracted recent interest due to reports of magnetically ordered ground states despite longstanding expectations that their strong spin-orbit coupling would generate a $\textit{J}$ = 0 electronic ground state for each Ir 5+ ion. The major focus of prior research has been on the double perovskite iridates Ba 2 YIrO 6 and Sr 2 YIrO 6 , where the nature of the ground states (i.e., ordered vs nonmagnetic) is still controversial. Here, in this work, we present neutron powder diffraction, high-energy-resolution fluorescence-detected x-ray absorption spectroscopy (HERFD-XAS), resonant inelastic x-ray scattering (RIXS), magnetic susceptibility, and muon spin relaxation data on the related double perovskite iridates Ba 2 LuIrO 6 , Sr 2 LuIrO 6 , Ba 2 ScIrO 6 , and Sr 2 ScIrO 6 that enable us to gain a general understanding of the electronic and magnetic properties for this family of materials. Our HERFD-XAS and RIXS measurements establish $\textit{J}$ = 0 electronic ground states for the Ir 5+ ions in all cases, with similar values for Hund's coupling $J_H$ and the spin-orbit coupling constant $λ_{\text{SOC}}$. Our bulk susceptibility and muon spin relaxation data find no evidence for long-range magnetic order or spin freezing, but they do exhibit weak magnetic signals that are consistent with extrinsic local moments. Our results indicate that the large $λ_{\text{SOC}}$ is the key driving force behind the electronic and magnetic ground states realized in the $5d^4$ double perovskite iridates, which agrees well with conventional wisdom.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Emergence of a Spin Microemulsion in Spin-Orbit Coupled Bose-Einstein Condensates

We report the first numerical prediction of a “spin microemulsion”—a phase with undulating spin domains resembling classical bicontinuous oil-water-surfactant emulsions—in two-dimensional systems of spinor Bose-Einstein condensates with isotropic Rashba spin-orbit coupling. Using field-theoretic numerical simulations, we investigated the melting of a low-temperature stripe phase with supersolid character and find that the stripes lose their superfluidity at elevated temperature and undergo a Kosterlitz-Thouless-like transition into a spin microemulsion. Momentum distribution calculations highlight a thermally broadened occupation of the Rashba circle of low-energy states with macroscopic and isotropic occupation around the ring. Here, we provide a finite-temperature phase diagram that positions the emulsion as an intermediate, structured isotropic phase with residual quantum character before transitioning at higher temperature into a structureless normal fluid.

Finite temperature field theory↗
DOE OSTI2026

Vibrational Spin-Orbit Coupling Contributions to Excited State Decay of Ligand-to-Ligand Charge Transfer States

Controlling excited state relaxation processes is important in a variety of photochemical and photophysical processes, including the generation of ground and excited state spin polarization for quantum information science applications. Here, we address how specific static distortions – based on vibrational spin-orbit active modes at C2v symmetry determined by group theory – in a series of low-symmetry ligand-to-ligand charge transfer complexes enable direct spin-orbit coupling contributions to T1 → S0 excited state decay. These results are used to address spin-vibronic coupling contributions to T1 → S0 decay in a high-symmetry (tBu2bpy)Pt(S,S) (tBu2bpy = 4,4’-di-tert-butyl-2,2’-bipyridine and S,S = benzene-1,2-dithiolate) ligand-to-ligand charge transfer complex with effective C2v symmetry, where T1 relaxation is both spin- and orbitally forbidden due to the direct spin-orbit coupling matrix element being zero by symmetry. Low-frequency vibrations that involve a pyridine-pyridine twisting motion within the bpy ligand generate large ∂/∂Qi values that will contribute significantly to T1 → S0 relaxation. The work advances ligand design strategies for the generation of tailored T1 → S0 relaxation rates, which can be utilized to optimize the generation of electron spin polarization in radical-elaborated ligand-to-ligand charge transfer complexes.

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

Novel phenomena in transition-metal oxide thin films and heterostructures with strong correlations and spin-orbit coupling

Transition-metal oxides have been a central subject of condensed matter physics for decades. In addition to novel electronic states driven by the influence of strong correlation, relativistic spin-orbit coupling effects have recently attracted much attention for their potential to explore topological phenomena. Here, in this article, we review various experimental and theoretical studies on transition-metal oxides with focus on thin films and heterostructures where their physics is much influenced by correlation effects and spin-orbit coupling. The combination of the heterostructure geometry together with correlation and topology leads to a variety of novel states here reviewed. We also discuss perspectives for future research in this broad promising area.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Comparison of state-interaction and spinor-representation calculations of spin-orbit coupling within exact two-component coupled-cluster theories

Here a benchmark study of state-interaction and spinor-representation calculations of spin-orbit coupling using the exact two-component Hamiltonians with atomic mean-field integrals (the X2CAMF schemes) at the equation-of-motion coupled-cluster singles and doubles level is reported. We adopt a version of the X2CAMF scheme with spin-orbit integrals correct to first order for the state-interaction calculations and a version correct to infinite order for the spinor-representation calculations. The differences between the state-interaction calculations with minimum active spaces to account for (quasi-)degeneracy and the spinor-representation calculations thus correspond to higher-order spin-orbit contributions. This state-interaction approach with scalar-relativistic effects accurately included in the reference functions and in the spin-orbit integrals is shown to exhibit robust performance for elements across the periodic table. On the other hand, the more rigorous spinor representation shows more rapid convergence with respect to the number of correlated electrons and is the preferred choice for accurate calculations for heavy elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Giant Orbital Anisotropy with Strong Spin–Orbit Coupling Established at the Pseudomorphic Interface of the Co/Pd Superlattice

Orbital anisotropy at interfaces in magnetic heterostructures has been key to pioneering spin–orbit-related phenomena. However, modulating the interface’s electronic structure to make it abnormally asymmetric has been challenging because of lack of appropriate methods. Here, the authors report that low-energy proton irradiation achieves a strong level of inversion asymmetry and unusual strain at interfaces in [Co/Pd] superlattices through nondestructive, selective removal of oxygen from Co3O4/Pd superlattices during irradiation. Structural investigations corroborate that progressive reduction of Co3O4into Co establishes pseudomorphic growth with sharp interfaces and atypically large tensile stress. The normal component of orbital to spin magnetic moment at the interface is the largest among those observed in layered Co systems, which is associated with giant orbital anisotropy theoretically confirmed, and resulting very large interfacial magnetic anisotropy is observed. All results attribute not only to giant orbital anisotropy but to enhanced interfacial spin–orbit coupling owing to the pseudomorphic nature at the interface. They are strongly supported by the observation of reversal of polarity of temperature-dependent Anomalous Hall signal, a signature of Berry phase. This work suggests that establishing both giant orbital anisotropy and strong spin–orbit coupling at the interface is key to exploring spintronic devices with new functionalities.

42 ENGINEERING↗
DOE OSTI2022

A comparison between the one- and two-step spin-orbit coupling approaches based on the ab initio Density Matrix Renormalization Group

The efficient and reliable treatment of both spin-orbit coupling (SOC) and electron correlation is essential for understanding f-element chemistry. Here, we analyze two approaches to the problem, the one-step approach where both effects are treated simultaneously, and the two-step state interaction approach. We report an implementation of the ab initio density matrix renormalization group(DMRG) with a one-step treatment of the SOC effect which can be compared to prior two-step treatments on an equal footing. Using a dysprosium octahedral complex and bridged dimer as benchmark systems, we identify characteristics of problems where the one-step approach is beneficial for obtaining the low-energy spectrum.

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

Two-component atomic Fermi superfluid with spin-orbital coupling in thin-spherical-shell geometry

We present a theory of two-component atomic Fermi superfluid with tunable pairing interaction in a thin spherical shell subject to spin-orbit coupling (SOC). By incorporating SOC into the Fermi superfluid in the BCS-Bose Einstein condensation (BEC) crossover, we obtain the energy spectrum and equations of state. While the order parameter and chemical potential are suppressed by SOC on the BCS side, the former remains positive but the latter may be pushed to negative values by SOC.Meanwhile, the compressibility exhibits kinks as the pairing interaction or SOC varies, indicating singular behavior of higher derivatives of the free energy despite the presence of the superfluid order parameter. The minimum of the energy dispersion indicates a decoupling of the energy gap from the order parameter, and the compressibility kinks occur when the energy gap approaches 0. We found the particle-hole mixing in the Fermi superfluid essential for the compressibility kinks since a Fermi gas with the same SOC but no pairing interaction only exhibits complicated dispersions but no singular behavior. Therefore, our results show that a combination of superfluid, SOC, and geometry can lead to interesting phenomena. Here, we also discuss possible experimental realizations and implications.

Fermi gases↗
DOE OSTI2024

Spin-orbit coupling in molecular complexes beyond van der Waals regime: Key factors for further splitting of 2 P 3/2 ground state

Here, we report a joint spectroscopic and theoretical study probing spin-orbit coupling (SOC) in a variety of molecular complexes between an iodine atom and a ligand (L) with L ranging from Ar, HF to formic/acetic acids, and glycine/N-methylated glycine derivatives. Cryogenic photoelectron spectroscopy of L·I - (L=HCOOH, CH 3 COOH) reveals three distinct peaks, identified as three SOC states, denoted as X(1/2), A(3/2), and B(l/2) for the corresponding neutrals. The X and A separation ΔE XA is measured to be 0.10 eV for both, whereas the X and B gap ΔE XB is 0.98 and 0.97 eV for formic and acetic acid, respectively. These new ΔE XA values are compared with the previously reported values for the molecular complexes L·I· with L=Ar, HF, glycine, and A-methylated glycines. All together these complexes encompass a diversity of intermolecular interactions, from van der Waals to weak and strong hydrogen bonding. While the ΔE XB remains similar, the ΔE XA is shown to be extremely sensitive to the type of ligands and interactions, spanning from 5 meV to 150 meV. High-level relativistic quantum calculations including explicit SOC formulism nicely reproduce all experimental SOC splitting. A direct correlation between the magnitude of ΔE XA with the intermolecular interaction strength or bond distance of the neutral complexes—the stronger interaction (shorter bond length), the greater splitting, is established.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Effects of spin-orbit coupling and very large supercells on the description of acceptors in CdTe

Predicting accurate shallow donor and acceptor levels in semiconductors has been quite challenging using periodic boundary conditions as implemented in current density functional theory codes. The reason is that the wave functions associated with the shallow centers are quite extended and are not fully contained in the supercell (typically with a few hundred atoms) so impurities in the periodically repeated image cells interact with each other. Errors of ~0.1 eV are expected, and these are of the same order of magnitude as the ionization energies themselves. In the case of acceptors in CdTe, this problem is exacerbated by the strong spin-orbit coupling that split the Te-related states at the top of the valence band, making the calculations at least 8 times more expensive. CdTe is an important solar-cell material with record high efficiency of 22%. One of the main limiting factors to increasing the efficiency towards the theoretical limit of ~30% is the often reported very low hole concentration. Pushing to the limit of computational capability by using very large supercells with spin-orbit coupling we report the results of hybrid functional calculations of group-V acceptors in CdTe. We show that extrapolation to the dilute limit leads to an interpretation of the experimental data that is qualitatively different from previous DFT and hybrid functional calculation reports. We find that the group-V impurities indeed behave as shallow acceptors and that the corresponding compensating AX-centers are unstable and do not limit p-type doping. We address the differences between our results and previous theoretical predictions and show that our calculated ionization energies predict hole concentrations that are in excellent agreement with recent temperature-dependent Hall measurements on high-quality single-crystal samples.

14 SOLAR ENERGY↗
DOE OSTI2024

Nodal fermions in the strongly spin-orbit coupled pyrochlore-lattice compound RbBi2

We explore the topological electronic band structure of the pyrochlore lattice in the strong spin-orbit coupling regime. Using angle-resolved photoemission spectroscopy, first-principles calculations, and symmetry analysis, we have investigated the bulk electronic structure of RbBi2, which has a Bi pyrochlore network. We observe the presence of 3D massless Dirac fermions enforced by nonsymmorphic symmetry, as well as a 3D quadratic band crossing protected by cubic crystalline symmetry. Furthermore, we identify an additional 3D linear Dirac dispersion associated with band inversion protected by threefold rotation symmetry. These observations reveal the rich band topology of itinerant pyrochlore lattice systems in the strong SOC limit and serve as a starting point to explore correlated topological phases in geometrically frustrated lattices.

Oh, Dongjin↗
DOE OSTI2025

COLUMBUS─An Efficient and General Program Package for Ground and Excited State Computations Including Spin–Orbit Couplings and Dynamics

The COLUMBUS program system provides the tools for performing high-level multireference (MR) computations, including the multireference configuration interaction (MRCI) method and its multireference averaged quadratic coupled cluster (MR-AQCC) extension, allowing computations on a wide range of fascinating atomic and molecular systems, including the treatment of open-shells and complicated excited state phenomena. The inclusion of spin−orbit coupling (SOC) directly within the MRCI step enables the description of systems containing heavy elements, such as lanthanides and actinides, whose properties are strongly influenced by SOC. Analytic energy gradients and nonadiabatic couplings at the correlated MRCI level provide the foundation for a variety of dynamics studies, giving insight into ultrafast photochemistry. New and ongoing method developments in COLUMBUS include the computation of spin densities, improved descriptions of ionic states, enhancements to the AQCC method, and the porting of COLUMBUS to graphical processing units (GPUs). New external interfaces enable an enhanced description of electronic resonances and molecules in strong laser fields. This work highlights these new developments while providing a detailed account of the diverse applications of COLUMBUS in recent years.

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

Self-consistent quasiparticle G W and hybrid functional calculations for Al/InAs/Al heterojunctions: Band offset and spin-orbit coupling effects

The electronic structure of surfaces and interfaces plays a key role in the properties of quantum devices. Here, we study the electronic structure of realistic Al/InAs/Al heterojunctions using a combination of density functional theory with hybrid functionals and state-of-the-art quasiparticle G W (QSGW) calculations. We find a good agreement between QSGW calculations and hybrid functional calculations, which themselves compare favorably well with angle-resolved photoemission spectroscopy experiments. Our paper confirms the need for well-controlled quality of the interfaces to obtain the needed properties of InAs/Al heterojunctions. A detailed analysis of the effects of spin-orbit coupling on the spin splitting of the electronic states shows a linear scaling in k space, related to the two-dimensional nature of some interface states. The good agreement by QSGW and hybrid functional calculations opens the door towards trustable use of an effective approximation to QSGW for studying very large heterojunctions. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗
DOE OSTI2025

Microscopic origin of temperature-dependent magnetism in spin-orbit-coupled transition metal compounds

A few 4 d and 5 d transition metal compounds with various electron fillings were recently found to exhibit magnetic susceptibilities χ and magnetic moments that deviate from the well-established Kotani model. This model has been considered for decades to be the canonical expression for descriing the temperature dependence of magnetism in systems with nonnegligible spin-orbit coupling effects. In this paper, we uncover the origin of such discrepancies and determine the applicability and limitations of the Kotani model by calculating the temperature dependence of the magnetic moments of a series of 4 d (Ru-based) and 5 d (W-based) systems at different electron fillings. For this purpose, we perform exact diagonalization of -derived relativistic multiorbital Hubbard models on finite clusters and compute their magnetic susceptibilities. Comparison with experimentally measured magnetic properties indicates that contributions such as a temperature-independent χ 0 background, crystal field effects, Coulomb and Hund's couplings, and intersite interactions—not included in the Kotani model—are especially crucial for correctly describing the temperature dependence of χ and magnetic moments at various electron fillings in these systems. Based on our results, we propose a generalized approach beyond the Kotani model to accurately describe their magnetism. Published by the American Physical Society 2025

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Engineering infinite-range SU($\textit{n}$) interactions with spin-orbit-coupled fermions in an optical lattice

Here, we study multilevel fermions in an optical lattice described by the Hubbard model with on-site SU($\textit{n}$) -symmetric interactions. We show that in an appropriate parameter regime this system can be mapped onto a spin model with all-to-all SU($\textit{n}$)-symmetric couplings. Raman pulses that address internal spin states modify the atomic dispersion relation and induce spin-orbit coupling, which can act as a synthetic inhomogeneous magnetic field that competes with the SU($\textit{n}$) exchange interactions. We investigate the mean-field dynamical phase diagram of the resulting model as a function of $\textit{n}$ and different initial configurations that are accessible with Raman pulses. Consistent with previous studies for $\textit{n}$ = 2 , we find that for some initial states the spin model exhibits two distinct dynamical phases that obey simple scaling relations with $\textit{n}$. Moreover, for $\textit{n}$ > 2 we find that dynamical behavior can be highly sensitive to initial intraspin coherences. Our predictions are readily testable in current experiments with ultracold alkaline-earth-metal(-like) atoms.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗