Strong Strong Spin-orbit Coupling Research Articles

Probing the Magnetic Ground State of Ba2YIrO6: Impact of Nonmagnetic Dopants and Spin-Orbit Coupling.

Strong spin-orbit coupling (SOC) in iridates has long been predicted to lead to exotic electronic and magnetic ground states. Ba2YIrO6 (BYIO) has attracted particular attention due to the expectation of a Jeff = 0 state for Ir5+ ions under the jj-coupling scheme. However, controversies surround the actual realization of this state, as finite magnetic moments are consistently observed experimentally. We present a multi-physics study of this system by progressively introducing nonmagnetic Sb5+ ions in place of Ir5+ (Ba2YIr​1-ySb​yO​6, BYISO). Despite similar charge and ionic radii, Sb​5+ doping appears highly inhomogeneous, coexisting with a fraction of nearly pure BYIO regions, as confirmed by X-ray diffraction (XRD). This aligns with observations in related compounds. While inhomogeneity creates uncertainty, the doped majority phases offer valuable insights. It is relevant that the inclusion of even small amounts of Sb​5+ (10-20%) leads to a rise in magnetization. This strengthens our previous suggestion that magnetic Ir ions form dynamic singlets in BYIO, resulting in a near-nonmagnetic background. The observed moment enhancement with nonmagnetic doping supports the breakdown of these singlets. Furthermore, the magnetization steadily increases with an increasing Sb​5+ content, contradicting the anticipated approach towards the Jeff = 0 state with increased SOC due to reduced hopping between Ir​5+ ions. This reinforces the presence of individual Ir​5+ moments. Overall, our findings suggest that Ba​2YIrO​6 might not possess sufficiently strong SOC to be solely described within the jj-coupling picture, paving the way for further investigation.

Atomic-Layer Controlled Transition from Inverse Rashba-Edelstein Effect to Inverse Spin Hall Effect in 2D PtSe2 Probed by THz Spintronic Emission.

2D materials, such as transition metal dichalcogenides, are ideal platforms for spin-to-charge conversion (SCC) as they possess strong spin-orbit coupling (SOC), reduced dimensionality and crystal symmetries as well as tuneable band structure, compared to metallic structures. Moreover, SCC can be tuned with the number of layers, electric field, or strain. Here, SCC in epitaxially grown 2D PtSe2 by THz spintronic emission is studied since its 1T crystal symmetry and strong SOC favor SCC. High quality of as-grown PtSe2 layers is demonstrated, followed by in situ ferromagnet deposition by sputtering that leaves the PtSe2 unaffected, resulting in well-defined clean interfaces as evidenced with extensive characterization. Through this atomic growth control and using THz spintronic emission, the unique thickness-dependent electronic structure of PtSe2 allows the control of SCC. Indeed, the transition from the inverse Rashba-Edelstein effect (IREE) in 1-3 monolayers (ML) to the inverse spin Hall effect (ISHE) in multilayers (>3 ML) of PtSe2 enabling the extraction of the perpendicular spin diffusion length and relative strength of IREE and ISHE is demonstrated. This band structure flexibility makes PtSe2 an ideal candidate to explore the underlying mechanisms and engineering of the SCC as well as for the development of tuneable THz spintronicemitters.

Highly Energy-Efficient Spin Current Generation in SrIrO3 by Manipulating the Octahedral Rotation.

Materials with strong spin-orbit coupling (SOC) have been continuously attracting intensive attention due to their promising application in energy-efficient, high-density, and nonvolatile spintronic devices. Particularly, transition-metal perovskite oxides with strong SOC have been demonstrated to exhibit efficient charge-spin interconversion. In this study, we systematically investigated the impact of epitaxial strain on the spin-orbit torque (SOT) efficiency in the SrIrO3(SIO)/Ni81Fe19(Py) bilayer. The results reveal that the SOT efficiency is strongly related to the octahedral rotation around the in-plane axes of the single-crystal SIO. By modulating the epitaxial strain using different substrates, the SOT efficiency can be remarkably improved from 0.15 to 1.45. This 10-fold enhancement of SOT efficiency suggests that modulating the epitaxial strain is an efficient approach to control the SOT efficiency in complex oxide-based heterostructures. Our work may have the potential to advance the application of complex oxides in energy-efficient spintronic devices.

Superconductivity in a ferroelectric-like topological semimetal SrAuBi

Given the rarity of metallic systems that exhibit ferroelectric-like transitions, it is apparently challenging to find a system that simultaneously possesses superconductivity and ferroelectric-like structural instability. Here, we report the observation of superconductivity at 2.4 K in a layered semimetal SrAuBi characterized by strong spin–orbit coupling (SOC) and ferroelectric-like lattice distortion. Single crystals of SrAuBi have been successfully synthesized and found to show a polar-nonpolar structure transition at 214 K, which is associated with the buckling of Au-Bi honeycomb lattice. On the basis of the band calculations considering SOC, we found significant Rashba-type spin splitting and symmetry-protected multiple Dirac points near the Fermi level. We believe that this discovery opens up new possibilities of pursuing exotic superconducting states associated with the semimetallic band structure without space inversion symmetry and the topological surface state with the strong SOC.

Strong Rashba parameter of two-dimensional electron gas at CaZrO3/SrTiO3 heterointerface

We synthesized a CaZrO3/SrTiO3 oxide heterostructure, which can serve as an alternative to LaAlO3/SrTiO3, and confirmed the generation of 2-dimensional electron gas (2-DEG) at the heterointerface. We analyzed the electrical-transport properties of the 2-DEG to elucidate its intrinsic characteristics. Based on the magnetic field dependence of resistance at 2 K, which exhibited Weak Anti-localization (WAL) behaviors, the fitted Rashba parameter values were found to be about 12–15 × 10–12 eV*m. These values are stronger than the previous reported Rashba parameters obtained from the 2-DEGs in other heterostructure systems and several layered 2D materials. The observed strong spin–orbit coupling (SOC) is attributed to the strong internal electric field generated by the lattice mismatch between the CaZrO3 layer and SrTiO3 substrate. This pioneering strong SOC of the 2-DEG at the CaZrO3/SrTiO3 heterointerface may play a pivotal role in the developing future metal oxide-based quantum nanoelectronics devices.

Spin-to-charge conversion in tantalum with structural phase transition

Tantalum (Ta), which is widely used as a spin sink material, especially for its β-phase with strong spin-orbit coupling (SOC) exhibits a high spin-charge interconversion efficiency. In this work, we investigate the spin-to-charge conversion (SCC) process of Ta/Permalloy (Ta/Py) bilayers with Ta having different crystalline phases. The structural phase transition of Ta film from tetragonal to body-centered cuboidal (BCC) which corresponds to β- and α-phases was obtained via high-temperature annealing in vacuum atmosphere. By applying ferromagnetic resonance (FMR) and inverse spin Hall effect (ISHE) measurements, the measured spin mixing conductance and SCC DC voltage show a strong correlation with the crystalline phase of Ta thin films in Ta/Py bilayers. A significant enhancement of spin mixing conductance in (β + α)-Ta/Py has been found and a higher SCC DC voltage was detected for α-phase Ta film with a weak SOC than β-phase Ta film with a strong SOC. These results reveal the significant role of the interfacial constitution in heavy metal/ferromagnet bilayers for spin current transportation, which can promote the development of high-efficiency spin-based devices through interfacial engineering.

Fluence and Temperature Dependences of Laser-Induced Ultrafast Demagnetization and Recovery Dynamics in L10-FePt Thin Film.

The fundamental mechanisms of ultrafast demagnetization and magnetization recovery processes in ferromagnetic materials remain incompletely understood. The investigation of different dynamic features which depend on various physical quantities requires a more systematic approach. Here, the femtosecond laser-induced demagnetization and recovery dynamics in L10-Fe0.5Pt0.5 alloy film are studied by utilizing time-resolved magneto-optical Kerr measurements, focusing on their dependences of excitation fluence and ambient temperature over broad ranges. Ultrafast demagnetization dominated by Elliott-Yafet spin-flip scattering, and two-step magnetization recovery processes are found to be involved in all observations. The fast recovery time corresponding to spin-lattice relaxation is much shorter than that of many ferromagnets and increase with excitation fluence. These can be ascribed to the strong spin-orbit coupling (SOC) demonstrated in FePt and the reduction of transient magnetic anisotropy, respectively. Surprisingly, the demagnetization time exhibits no discernible correlation with ambient temperature. Two competitive factors are proposed to account for this phenomenon. On the other hand, the spin-lattice relaxation accelerates as temperature decreases due to enhanced SOC at lower ambient temperature. A semiquantitative analysis is given to get a visualized understanding. These results offer a comprehensive understanding of the dynamic characteristics of ultrafast demagnetization and recovery processes in iron-based materials with strong SOC, highlighting the potential for regulating the magnetization recovery process through temperature and laser fluence adjustments.

Realizing a Superconducting Square-Lattice Bismuth Monolayer

Interplay of crystal symmetry, strong spin-orbit coupling (SOC), and many-body interactions in low-dimensional materials provides a fertile ground for the discovery of unconventional electronic and magnetic properties and versatile functionalities. Two-dimensional (2D) allotropes of group 15 elements are appealing due to their structures and controllability over symmetries and topology under strong SOC. Here, we report the heteroepitaxial growth of a proximity-induced superconducting 2D square-lattice bismuth monolayer on superconducting Pb films. The square lattice of monolayer bismuth films in a C4 symmetry together with a stripey moiré structure is clearly resolved by our scanning tunneling microscopy, and its atomic structure is revealed by density functional theory (DFT) calculations. A Rashba-type spin-split Dirac band is predicted by DFT calculations to exist at the Fermi level and becomes superconducting through the proximity effect from the Pb substrate. We suggest the possibility of a topological superconducting state in this system with magnetic dopants/field. This work introduces an intriguing material platform with 2D Dirac bands, strong SOC, topological superconductivity, and the moiré superstructure.

Substrate effects on spin relaxation in two-dimensional Dirac materials with strong spin-orbit coupling

Understanding substrate effects on spin dynamics and relaxation is of key importance for spin-based information technologies. However, the key factors that determine such effects, in particular for materials with strong spin-orbit coupling (SOC), have not been well understood. Here we performed first-principles real-time density-matrix dynamics simulations with SOC and the electron-phonon and electron-impurity scattering for spin lifetimes (τs) of supported/free-standing germanene, a prototypical strong SOC 2D Dirac material. We show that the effects of different substrates on τs can surprisingly differ by two orders of magnitude. We find that substrate effects on τs are closely related to substrate-induced modifications of the SOC-field anisotropy, which changes the spin-flip scattering matrix elements. We propose a new electronic quantity, named spin-flip angle θ↑↓, to characterize spin relaxation through intervalley spin-flip scattering. We find that {tau }_{s}^{-1} is approximately proportional to the averaged value of {sin }^{2}left({theta }^{uparrow downarrow }/2right), which serves as a guiding parameter of controlling spin relaxation.

Modulation of Spin-Orbit Torque and Large Enhancement of Perpendicular Magnetic Anisotropy in W/Co20Fe60B20/MgO by Ir Insertion Layer

Iridium ($\mathrm{Ir}$) is a 5d heavy metal with strong spin-orbit coupling (SOC), which introduces various intriguing phenomena when interacting with a ferromagnetic layer. In this study, we utilize $\mathrm{Ir}$ as an insertion layer in $\mathrm{W}/\mathrm{Ir}({t}_{\mathrm{Ir}})/{\mathrm{Co}}_{20}{\mathrm{Fe}}_{60}{\mathrm{B}}_{20}/\mathrm{Mg}\mathrm{O}$ heterostructures to tune SOC and study its influence on the spin-orbit torque (SOT), perpendicular magnetic anisotropy (PMA), and Dzyaloshinskii-Moriya interaction (DMI). The SOT efficiency decreases first and then increases with an increase of $\mathrm{Ir}$ insertion layer thickness because of the opposite spin Hall angle between $\mathrm{W}$ and $\mathrm{Ir}$, and the sign changes when the thickness of $\mathrm{Ir}$ is 1.5 nm, which is close to the spin diffusion length of $\mathrm{Ir}$ of 1.35 nm. Importantly, a 0.25-nm-thick $\mathrm{Ir}$ layer enhances largely the effective PMA by 140%--350% under different annealing temperatures compared with that of a sample without insertion. Meanwhile, the DMI constant is also enhanced. The enhancement of PMA and DMI is likely due to the enhancement of interfacial SOC when $\mathrm{Ir}$ diffuses into ${\mathrm{Co}}_{20}{\mathrm{Fe}}_{60}{\mathrm{B}}_{20}$ and leads to the formation of ${\mathrm{Fe}}_{1\ensuremath{-}x}{\mathrm{Ir}}_{x}$. These results provide an effective method to tune SOC by inducing a dusting layer with strong SOC to meet different requirements in spintronic devices like small magnetic tunnel junctions.

Anisotropic spin-to-charge conversion in bismuth

Many intriguing physical phenomena have emerged from the Bi-containing materials due to the interplay of band topology and strong spin-orbit coupling (SOC). In this work, we report anisotropic spin-to-charge conversion in Bi, a semimetal endowed with highly anisotropic Fermi surfaces in addition to strong SOC. The value of spin Hall angle ${\ensuremath{\theta}}_{\mathrm{SH}}$ in Bi, that measures the spin-to-charge conversion efficiency, varies from ${\ensuremath{\theta}}_{\mathrm{SH}}\ensuremath{\approx}0$ to ${\ensuremath{\theta}}_{\mathrm{SH}}\ensuremath{\approx}2.6%$ for two predominant crystal orientations. In addition, the propensity of oxidation and interface quality also affect the spin-to-charge conversion in Bi. The highly anisotropic spin-to-charge conversion between Bi(003) and Bi(012) provide significant insights into the exploration and development of Bi-based topological quantum materials and spintronics.

J=0 nonmagnetic insulating state in K2OsX6 (X=F,Cl,andBr)

In $4d/5d$ transition-metal systems, many interesting physical properties arise from the interplay of bandwidth, electronic correlations, and spin-orbit interactions. Here, using {\it ab initio} density functional theory, we systematically study the double-perovskite-like system K$_2$Os$X_6$ (X = F, Cl, and Br) with a $5d^4$ electronic configuration. Our main result is that the $J = 0$ nonmagnetic insulating state develops in this system, induced by strong spin-orbital coupling. Specifically, the well-separated Os$X_6$ octahedra lead to the cubic crystal-field limit and result in dramatically decreasing hoppings in nearest neighbor Os-Os sites. In this case, the three degenerate $t_{2g}$ orbitals are reconstructed into two ``effective'' $j_{\rm eff}$ ($j_{\rm eff} = 1/2$ and $j_{\rm eff} = 3/2$ states) states separated by the strong SOC, opening a gap with four electrons occupying the $j_{\rm eff} = 3/2$ orbitals. Furthermore, the hybridization between the Os $5d$ orbitals and the $X$ ($X$ = F, Cl, and Br) $p$ 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.

Zoo of silicon-based quantum bits

Zoo of silicon-based quantum bits

Spin pumping from antiferromagnetic insulator spin-orbit-proximitized by adjacent heavy metal: a first-principles Floquet-nonequilibrium Green function study

Motivated by the recent experiment (Vaidya et al 2020 Science 368 160) on spin pumping from sub-THz radiation-driven uniaxial antiferromagnetic insulator (AFI) MnF2 into heavy metal (HM) Pt hosting strong spin-orbit (SO) coupling, we compute and compare pumped spin currents in Cu/MnF2/Cu and Pt/MnF2/Cu heterostructures. Recent theories of spin pumping by AFI have relied on simplistic Hamiltonians (such as tight-binding) and the scattering approach to quantum transport yielding the so-called interfacial spin mixing conductance (SMC), but the concept of SMC ceases to be applicable when SO coupling is present directly at the interface. In contrast, we use a more general first-principles quantum transport approach which combines noncollinear density functional theory with Floquet-nonequilibrium Green’s functions in order to take into account: SO-proximitized AFI as a new type of quantum material, different from isolated AFI and brought about by AFI hybridization with adjacent HM layer; strong SO coupling at the interface; and evanescent wavefunctions penetrating from Pt or Cu into AFI layer to make its interfacial region conducting rather than insulating as in the isolated AFI. The DC component of pumped spin current vs. precession cone angle of the Néel vector l of AFI does not follow putative , except for very small angles for which we define an effective SMC from the prefactor and find that it doubles from MnF2/Cu to MnF2/Pt interface. In addition, the angular dependence differs for opposite directions of precession of the Néel vector, leading to twice as large SMC for the right-handed than for the left-handed chirality of the precession mode.

Magnetization-driven Lifshitz transition and charge-spin coupling in the kagome metal YMn6Sn6

The Fermi surface (FS) is essential for understanding the properties of metals. It can change under both conventional symmetry-breaking phase transitions and Lifshitz transitions (LTs), where the FS, but not the crystal symmetry, changes abruptly. Magnetic phase transitions involving uniformly rotating spin textures are conventional in nature, requiring strong spin-orbit coupling (SOC) to influence the FS topology and generate measurable properties. LTs driven by a continuously varying magnetization are rarely discussed. Here we present two such manifestations in the magnetotransport of the kagome magnet YMn6Sn6: one caused by changes in the magnetic structure and another by a magnetization-driven LT. The former yields a 10% magnetoresistance enhancement without a strong SOC, while the latter a 45% reduction in the resistivity. These phenomena offer a unique view into the interplay of magnetism and electronic topology, and for understanding the rare-earth counterparts, such as TbMn6Sn6, recently shown to harbor correlated topological physics.

Electron–Electron Interaction and Weak Antilocalization Effect in a Transition Metal Dichalcogenide Superconductor

In disordered transition‐metal dichalcogenide (TMD) superconductor, both the strong spin‐orbit coupling (SOC) and the disorder show remarkable effects on superconductivity. However, the features of SOC and disorder are rarely detected directly. Herein, the quantum transport behaviors arising from the interplay of SOC and disorder in the TMD superconductor 1T‐NbSeTe are reported. Before entering the superconducting state, the single crystal at low temperature shows a resistivity upturn, which is T 1/2 dependent and insensitive to the applied magnetic fields. The magnetoresistance (MR) at low temperatures shows an H 1/2 dependence at high magnetic fields. The characteristics are in good agreement with the electron–electron interaction (EEI) in a disordered conductor. In addition, the upturn changes and MR at low magnetic fields suggest the contribution of the weak antilocalization (WAL) effect arising from the strong SOC in the material. Moreover, the quantitative analyses of the transport features in different samples imply anomalous disorder‐enhanced superconductivity that needs to be further understood. The results reveal the disorder‐enhanced EEI and the strong SOC‐induced WAL effect in 1T‐NbSeTe, which illustrates the resistivity minimum in the widely studied doped superconductors. The work also provides insights into the disorder effect on superconductivity.

Giant Topological Hall Effect in van der Waals Heterostructures of CrTe2/Bi2Te3.

Discoveries of the interfacial topological Hall effect (THE) provide an ideal platform for exploring the physics arising from the interplay between topology and magnetism. The interfacial topological Hall effect is closely related to the Dzyaloshinskii-Moriya interaction (DMI) at an interface and topological spin textures. However, it is difficult to achieve a sizable THE in heterostructures due to the stringent constraints on the constituents of THE heterostructures, such as strong spin-orbit coupling (SOC). Here, we report the observation of a giant THE signal of 1.39 μΩ·cm in the van der Waals heterostructures of CrTe2/Bi2Te3 fabricated by molecular beam epitaxy, a prototype of two-dimensional (2D) ferromagnet (FM)/topological insulator (TI). This large magnitude of THE is attributed to an optimized combination of 2D ferromagnetism in CrTe2, strong SOC in Bi2Te3, and an atomically sharp interface. Our work reveals CrTe2/Bi2Te3 as a convenient platform for achieving large interfacial THE in hybrid systems, which could be utilized to develop quantum science and high-density information storage devices.

Efficient Optical Orientation and Slow Spin Relaxation in Lead-Free CsSnBr3 Perovskite Nanocrystals

Spin properties of lead halide perovskites have recently received considerable research attention, because the strong spin–orbit coupling (SOC) enables facile optical orientation of spin-polarized states, a property particularly useful for information science and spintronics. The strong SOC, however, also limits the spin relaxation lifetime. Herein, we study optical orientation and spin relaxation in lead-free CsSnBr3 perovskite nanocrystals. The SOC of CsSnBr3 (∼0.43 eV) is 3.5-fold weaker than that of lead halide perovskites but is still strong enough to ensure efficient optical orientation. Meanwhile, the room-temperature spin lifetime is prolonged to 18 ± 2 ps, longer than the reported lifetimes of various lead halide perovskites, and it is likely limited by electron–hole exchange rather than SOC. These results demonstrate the strong potential of nontoxic tin halide perovskites for spin-related applications.

Spin-orbit coupling effect on the electronic structure of Sr2FeHfO6 alloy for spintronics application

Strong spin–orbit coupling (SOC) in Sr2FeHfO6 (SFHO) alloy has been predicted by means of full-potential linear augmented plane wave method in order to study the effect on electronic structure. The tetragonal (I4/mmm) SFHO with SOC has an up-spin energy of ~1.2 eV and a total magnetic moment of ~2.03 μB mainly coming from the Fe (1.63 μB), and the SOC effect was prominent in SFHO due to the magnetic moment of 3d-Fe orbitals. The XAFS spectroscopy technique was used in order to analyze the electronic structure and optical properties of SFHO. The absorption spectra with Fe as a source atom shows a peak appearing around 7118 eV. SFHO with SOC falls within the half metallic state in the up-spin direction resulting significant increase of the total magnetic moment. This half-metallicity strong SOC in SFHO demonstrate much spin polarized electrons around the Fermi level, hence, this material is very potential in future memory devices and spintronic applications.

Ferrimagnetic Skyrmions in Topological Insulator/Ferrimagnet Heterostructures.

Magnetic skyrmions are topologically nontrivial chiral spin textures that have potential applications in next-generation energy-efficient and high-density spintronic devices. In general, the chiral spins of skyrmions are stabilized by the noncollinear Dzyaloshinskii-Moriya interaction (DMI), originating from the inversion symmetry breaking combined with the strong spin-orbit coupling (SOC). Here, the strong SOC from topological insulators (TIs) is utilized to provide a large interfacial DMI in TI/ferrimagnet heterostructures at room temperature, resulting in small-size (radius ≈ 100 nm) skyrmions in the adjacent ferrimagnet. Antiferromagnetically coupled skyrmion sublattices are observed in the ferrimagnet by element-resolved scanning transmission X-ray microscopy, showing the potential of a vanishing skyrmion Hall effect and ultrafast skyrmion dynamics. The line-scan spin profile of the single skyrmion shows a Néel-type domain wall structure and a 120 nm size of the 180° domain wall. This work demonstrates the sizable DMI and small skyrmions in TI-based heterostructures with great promise for low-energy spintronic devices.