Spin-orbital Entanglement Research Articles

Spin-orbit entanglement driven by the Jahn-Teller effect

Spin-orbit entanglement in 4d and 5d transition metal systems can enhance electronic correlations, leading to nontrivial ground states and the emergence of exotic excitations. There is also an interest to investigate spin-orbit entanglement in 3d compounds, though this is challenging due to their smaller spin-orbit coupling. Here we demonstrate that the Jahn-Teller effect in Mn3+ reduces the energy gap between high- and low- spin-orbital states that lead to enhanced spin-orbit entanglement. Our results show a rare example of synergistic effects of Jahn-Teller and spin-orbit interactions and provide a way to entangle different degrees of freedom in d-metal oxides, which may allow paths to explore the interplay of orbital, lattice and spins in 3d correlated systems.

Manipulation of anisotropic Zhang-Rice exciton in NiPS3 by magnetic field

The effect of external magnetic fields on the behavior of the Zhang-Rice exciton in NiPS3, which captures the physics of spin-orbital entanglement in 2D XY-type antiferromagnets, remains unclear. This study presents systematic study of angle-resolved and polarization-resolved magneto-optical photoluminescence spectra of NiPS3 in the Voigt geometry. We observed highly anisotropic, non-linear Zeeman splitting and polarization rotation of the Zhang-Rice exciton, which depends on the direction and intensity of the magnetic field and can be attributed to the spin-orbital coupling and field-induced spin reorientation. Furthermore, above the critical magnetic field, we detected additional splitting of the exciton peaks, indicating the coexistence of various orientations of Néel vector. This study characterizes orbital change of Zhang-Rice exciton and field-induced spin-reorientation phase transitions in a 2D hexagonal XY-type antiferromagnet, and it further demonstrates the continuous manipulation of the spin and polarization of the Zhang-Rice exciton.

G-factor symmetry and topology in semiconductor band states

The [Formula: see text] tensor, which determines the reaction of Kramers-degenerate states to an applied magnetic field, is of increasing importance in the current design of spin qubits. It is affected by details of heterostructure composition, disorder, and electric fields, but it inherits much of its structure from the effect of the spin-orbit interaction working at the crystal-lattice level. Here, we uncover interesting symmetry and topological features of [Formula: see text] for important valence and conduction bands in silicon, germanium, and gallium arsenide. For all crystals with high (cubic) symmetry, we show that large departures from the nonrelativistic value [Formula: see text] are guaranteed by symmetry. In particular, considering the spin part [Formula: see text], we prove that the scalar function [Formula: see text] must go to zero on closed surfaces in the Brillouin zone, no matter how weak the spin-orbit coupling is. We also prove that for wave vectors [Formula: see text] on these surfaces, the Bloch states [Formula: see text] have maximal spin-orbital entanglement. Using tight-binding calculations, we observe that the surfaces [Formula: see text] exhibit many interesting topological features, exhibiting Lifshitz critical points as understood in Fermi-surface theory.

Nonlinear Transverse Magnetic Susceptibility under Electric Toroidal Dipole Ordering

An electric toroidal dipole (ETD) moment is one of the fundamental dipole moments as well as electric and magnetic ones. Although it directly couples to neither an electric nor magnetic field due to its spatial inversion and time-reversal parities, its ordered state leads to unconventional transverse responses of the conjugate physical quantities. We here theoretically investigate nonlinear transverse magnetic susceptibility under the ETD ordering. By performing a self-consistent mean-field calculation for a five $d$-orbital model under a tetragonal crystalline electric field and using the nonlinear Kubo formula, we show that a third-order transverse magnetic susceptibility corresponding to a uniform magnetization perpendicular to the external magnetic field becomes nonzero once the ETD moment is ordered under tetragonal crystalline electric field. Moreover, we find that spin-orbital entanglement and a low-lying first excited crystal-field level are important for realizing large transverse responses.

Giant Magnetic Anisotropy in the Atomically Thin van der Waals Antiferromagnet FePS3

AbstractVan der Waals (vdW) magnets are an ideal platform for tailoring 2D magnetism with immense potential for spintronics applications and are intensively investigated. However, little is known about the microscopic origin of magnetic order in these antiferromagnetic systems. X‐ray photoemission electron microscopy is used to address the electronic and magnetic properties of the vdW antiferromagnet FePS3down to the monolayer. The experiments reveal a giant out‐of‐plane magnetic anisotropy of 22 meV per Fe ion, accompanied by unquenched magnetic orbital moments. Moreover, the calculations suggest that the Ising magnetism in FePS3is a visible manifestation of spin–orbit entanglement of the Fe 3delectron system.

Jahn-Teller states mixed by spin-orbit coupling in an electromagnetic field

Spin-orbit coupling plays a pivotal role in condensed matter physics. For instance, spin-orbit interactions affect the magnetization and transport dynamics in solids, while spins and momenta are locked in topological matter. Alternatively, spin-orbit entanglement may play an important role in exotic phenomena, like quantum spin liquids in 4d and 5d systems. An interesting question is how electronic states mixed by spin orbit coupling interact with electromagnetic fields, which may hold potential to tune their properties and reveal interesting physics. Motivated by our recent discovery of large gyrotropic signals in some Jahn-Teller manganites, here we explore the interaction of light with spin-mixed states in a d4 transition metal. We show that spin-orbit mixing enables electronic transitions that are sensitive to circularly polarized light, giving rise to a gyrotropic response that increases with spin-orbit coupling. Interestingly, photoexcited transitions that involve spin reversal are behind such gyrotropic resonances. Additionally, we find that the interaction with the electromagnetic field depends strongly on the relative orientation of the propagation of light with respect to Jahn-Teller distortions and spin quantization. We suggest that such interactions offer the opportunity to use electromagnetic waves at optical wavelengths to entangle orbital and spin degrees of freedom. Our approach, which includes a group-theoretical treatment of spin-orbit coupling, has wide applicability and provides a versatile tool to explore the interaction of electromagnetic fields with electronic states in transition metals with arbitrary spin-orbit coupling strength and pointgroup symmetries.

Constraints on the two-dimensional pseudospin- 12 Mott insulator description of Sr2IrO4

${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$ has often been described via a simple, one-band pseudospin-$\frac{1}{2}$ model subject to electron-electron interactions on a square lattice, fostering analogies with cuprate superconductors believed to be well described by a similar model. In this work we argue---based on a detailed study of the low-energy electronic structure by circularly polarized spin and angle-resolved photoemission spectroscopy combined with dynamical mean-field theory calculations---that a pseudospin-$\frac{1}{2}$ model fails to capture the full complexity of the system. We show instead that a realistic multiband Hubbard Hamiltonian, accounting for the full correlated ${t}_{2g}$ manifold, provides a detailed description of the interplay between spin-orbital entanglement and electron-electron interactions and yields quantitative agreement with experiments. Our analysis establishes that the ${j}_{3/2}$ states make up a substantial percentage of the low-energy spectral weight, i.e., approximately 74% as determined from the integration of the $j$-resolved spectral function in the 0 to $\ensuremath{-}1.64\phantom{\rule{0.16em}{0ex}}\mathrm{eV}$ energy range. The results in our work are of relevance not only to Ir-based materials but also more generally to multiorbital materials with closely spaced energy scales.

Interpretation of Ir L -edge isotropic x-ray absorption spectra across the pressure-induced dimerization transition in hyperhoneycomb β−Li2IrO3

The extended nature of atomic $5d$ orbitals, together with a relatively short $\ensuremath{\sim}3\phantom{\rule{0.16em}{0ex}}\AA{}$ Ir-Ir distance across edge-shared octahedra in honeycomb iridate lattices, leads to a tendency to disrupt the local, spin-orbit-entangled ${j}_{\mathrm{eff}}=\frac{1}{2}$ moments of ${\mathrm{Ir}}^{4+}$ ions in favor of dimerization and the formation of molecular orbitals, especially upon lattice compression. The sensitivity of Ir $L$-edge spectroscopy to both spin-orbit entanglement in ${j}_{\mathrm{eff}}$ states and the quenching of orbital degrees of freedom in dimerized states results in a peculiar evolution of x-ray absorption spectra across dimerization transitions, including energy shifts in the opposite direction for ${L}_{3}$ and ${L}_{2}$ leading absorption edges and substantial changes in their isotropic branching ratio. We present a theoretical description of the evolution of $5d$ electronic states, and related x-ray absorption spectra, in going from the single ion to the dimerized limit. The calculations reproduce the experimental results for hyper-honeycomb $\ensuremath{\beta}\text{\ensuremath{-}}{\mathrm{Li}}_{2}{\mathrm{IrO}}_{3}$ [L. Veiga et al., Phys. Rev. B 100, 064104 (2019); L. Veiga et al., Phys. Rev. B 96, 140402(R) (2017)] and shed light into the weakening of the coupling between spin and orbital degrees of freedom as the strength of dimerization increases. The results provide a basis for the interpretation of $L$-edge x-ray absorption spectra in $5d$ systems where competition between the formation of local ${j}_{\mathrm{eff}}$ states and molecular orbitals is at play.

Quantum Correlations in Jahn-Teller Molecular Systems Simulated with Superconducting Circuits

We explore quantum correlations, in particular, quantum entanglement, among vibrational phonon modes as well as between electronic and vibrational degrees of freedom in molecular systems, described by Jahn-Teller mechanism. Specifically, to isolate and simplify the phonon- electron interactions in a complex molecular system, the basis of our discussions is taken to be the proposal of simulating two-frequency Jahn- Teller systems using superconducting circuit quantum electrodynamics systems (circuit QED) by Tekin Dereli and co-workers in 2012. We evaluate the quantum correlations, in particular entanglement between the vibrational phonon modes, and present analytical explanations using a single privileged Jahn-Teller mode picture. Furthermore, spin-orbit entanglement or quantum correlations between electronic and vibrational degrees of freedom are examined. We conclude by discussing experimental feasibility to detect such quantum correlations, considering the dephasing and decoherence in state-of-the-art superconducting two-level systems (qubits).

Yb delafossites: Unique exchange frustration of4fspin-12moments on a perfect triangular lattice

While the Heisenberg model for magnetic Mott insulators on planar lattice structures is comparatively well understood in the case of transition metal ions, the intrinsic spin-orbit entanglement of $4f$ magnetic ions on such lattices shows fascinating new physics largely due to corresponding strong anisotropies both in their single-ion and their exchange properties. We show here that the Yb delafossites, containing perfect magnetic ${\mathrm{Yb}}^{3+}$ triangular lattice planes with pseudospin $s=\frac{1}{2}$ at low temperatures, are an ideal platform to study these phenomena. Competing frustrated interactions may lead to an absence of magnetic order associated to a gapless spin liquid ground state with a huge linear specific heat exceeding that of many heavy fermions, whereas the application of a magnetic field induces anisotropic magnetic order with successive transitions into different long-range ordered structures. In this comparative study, we discuss our experimental findings in terms of a unified crystal-field and exchange model. We combine electron paramagnetic resonance (EPR) experiments and results from neutron scattering with measurements of the magnetic susceptibility, isothermal magnetization up to full polarization, and specific heat to determine the relevant model parameters. The impact of the crystal field is discussed as well as the symmetry-compatible form of the exchange tensor, and we give explicit expressions for the anisotropic $g$ factor, the temperature dependence of the susceptibility, the exchange-narrowed EPR linewidth, and the saturation field.

Topological charge, spin, and heat transistor

Spin pumping consists in the injection of spin currents into a non-magnetic material due to the precession of an adjacent ferromagnet. In addition to the pumping of spin the precession always leads to pumping of heat, but in the presence of spin-orbital entanglement it also leads to a charge current. We investigate the pumping of charge, spin and heat in a device where a superconductor and a quantum spin Hall insulator are in proximity contact with a ferromagnetic insulator. We show that the device supports two robust operation regimes arising from topological effects. In one regime, the pumped charge, spin and heat are quantized and related to each other due to a topological winding number of the reflection coefficient in the scattering matrix formalism -- translating to a Chern number in the case of Hamiltonian formalism. In the second regime, a Majorana zero mode switches off the pumping of currents owing to the topologically protected perfect Andreev reflection. We show that the interplay of these two topological effects can be utilized so that the device operates as a robust charge, spin and heat transistor.

Spin-memory loss induced by bulk spin–orbit coupling at ferromagnet/heavy-metal interfaces

A spin current through a ferromagnet/heavy-metal interface may shrink due to the spin-flip at the interface, resulting in the spin-memory loss. Here, we propose a mechanism of the spin-memory loss. In contrast to other mechanisms based on interfacial spin–orbit coupling, our mechanism is based on the bulk spin–orbit coupling in a heavy metal. We demonstrate that the bulk spin–orbit coupling induces the entanglement between the spin and orbital degrees of freedom and this spin-orbital entanglement can give rise to sizable spin-flip at the interface even when the interfacial spin–orbit coupling is weak. Our mechanism emphasizes crucial roles of the atomic orbital degree of freedom and induces the strong spin-memory loss near band crossing points between bands of different orbital characters.

Spin-orbital polarization of Majorana edge states in oxide nanowires

We investigate a paradigmatic case of topological superconductivity in a one-dimensional nanowire with $d-$orbitals and a strong interplay of spin-orbital degrees of freedom due to the competition of orbital Rashba interaction, atomic spin-orbit coupling, and structural distortions. We demonstrate that the resulting electronic structure exhibits an orbital dependent magnetic anisotropy which affects the topological phase diagram and the character of the Majorana bound states (MBSs). The inspection of the electronic component of the MBSs reveals that the spin-orbital polarization generally occurs along the direction of the applied Zeeeman magnetic field, and transverse to the magnetic and orbital Rashba fields. The competition of symmetric and antisymmetric spin-orbit coupling remarkably leads to a misalignment of the spin and orbital moments transverse to the orbital Rashba fields, whose manifestation is essentially orbital dependent. The behavior of the spin-orbital polarization along the applied Zeeman field reflects the presence of multiple Fermi points with inequivalent orbital character in the normal state. Additionally, the response to variation of the electronic parameters related with the degree of spin-orbital entanglement leads to distinctive evolution of the spin-orbital polarization of the MBSs. These findings unveil novel paths to single-out hallmarks relevant for the experimental detection of MBSs.

Spin-orbit coupling effects on spin-phonon coupling in Cd2Os2O7

Spin-orbit coupling (SOC) is essential in understanding the properties of 5d transition metal compounds, whose SOC value is large and almost comparable to other key parameters. Over the past few years, there have been numerous studies on the SOC-driven effects of the electronic bands, magnetism, and spin-orbit entanglement for those materials with a large SOC. However, it is less studied and remains an unsolved problem in how the SOC affects the lattice dynamics. We, therefore, measured the phonon spectra of 5d pyrochlore Cd2Os2O7 over the full Brillouin zone to address the question by using inelastic x-ray scattering (IXS). Our main finding is a visible mode-dependence in the phonon spectra, measured across the metal-insulator transition at 227 K. We examined the SOC strength dependence of the lattice dynamics and its spin-phonon (SP) coupling, with first-principle calculations. Our experimental data taken at 100 K are in good agreement with the theoretical results obtained with the optimized U = 2.0 eV with SOC. By scaling the SOC strength and the U value in the DFT calculations, we demonstrate that SOC is more relevant than U to explaining the observed mode-dependent phonon energy shifts with temperature. Furthermore, the temperature dependence of the phonon energy can be effectively described by scaling SOC. Our work provides clear evidence of SOC producing a non-negligible and essential effect on the lattice dynamics of Cd2Os2O7 and its SP coupling.

Honeycomb rare-earth magnets with anisotropic exchange interactions

We study the rare-earth magnets on a honeycomb lattice, and are particularly interested in the experimental consequences of the highly anisotropic spin interaction due to the spin-orbit entanglement. We perform a high-temperature series expansion using a generic nearest-neighbor Hamiltonian with anisotropic interactions, and obtain the heat capacity, the parallel and perpendicular spin susceptibilities, and the magnetic torque coefficients. We further examine the electron spin resonance linewidth as an important signature of the anisotropic spin interactions. Due to the small interaction energy scale of the rare-earth moments, it is experimentally feasible to realize the strong-field regime. Therefore, we perform the spin-wave analysis and study the possibility of topological magnons when a strong field is applied to the system. The application and relevance to the rare-earth Kitaev materials are discussed.

Evolution of Spin-Orbital Entanglement with Increasing Ising Spin-Orbit Coupling

Several realistic spin-orbital models for transition metal oxides go beyond the classical expectations and could be understood only by employing the quantum entanglement. Experiments on these materials confirm that spin-orbital entanglement has measurable consequences. Here, we capture the essential features of spin-orbital entanglement in complex quantum matter utilizing 1D spin-orbital model which accommodates SU(2)⊗SU(2) symmetric Kugel-Khomskii superexchange as well as the Ising on-site spin-orbit coupling. Building on the results obtained for full and effective models in the regime of strong spin-orbit coupling, we address the question whether the entanglement found on superexchange bonds always increases when the Ising spin-orbit coupling is added. We show that (i) quantum entanglement is amplified by strong spin-orbit coupling and, surprisingly, (ii) almost classical disentangled states are possible. We complete the latter case by analyzing how the entanglement existing for intermediate values of spin-orbit coupling can disappear for higher values of this coupling.

How spin-orbital entanglement depends on the spin-orbit coupling in a Mott insulator

The concept of the entanglement between spin and orbital degrees of freedom plays a crucial role in understanding various phases and exotic ground states in a broad class of materials, including orbitally ordered materials and spin liquids. We investigate how the spin-orbital entanglement in a Mott insulator depends on the value of the spin-orbit coupling of the relativistic origin. To this end, we numerically diagonalize a 1D spin-orbital model with the 'Kugel-Khomskii' exchange interactions between spins and orbitals on different sites supplemented by the on-site spin-orbit coupling. In the regime of small spin-orbit coupling w.r.t. the spin-orbital exchange, the ground state to a large extent resembles the one obtained in the limit of vanishing spin-orbit coupling. On the other hand, for large spin-orbit coupling the ground state can, depending on the model parameters, either still show negligible spin-orbital entanglement, or can evolve to a highly spin-orbitally entangled phase with completely distinct properties that are described by an effective XXZ model. The presented results suggest that: (i) the spin-orbital entanglement may be induced by large on-site spin-orbit coupling, as found in the 5d transition metal oxides, such as the iridates; (ii) for Mott insulators with weak spin-orbit coupling of Ising-type, such as e.g. the alkali hyperoxides, the effects of the spin-orbit coupling on the ground state can, in the first order of perturbation theory, be neglected.

Robust weak antilocalization due to spin-orbital entanglement in Dirac material Sr3SnO

The presence of both inversion (P) and time-reversal (T) symmetries in solids leads to a double degeneracy of the electronic bands (Kramers degeneracy). By lifting the degeneracy, spin textures manifest themselves in momentum space, as in topological insulators or in strong Rashba materials. The existence of spin textures with Kramers degeneracy, however, is difficult to observe directly. Here, we use quantum interference measurements to provide evidence for the existence of hidden entanglement between spin and momentum in the antiperovskite-type Dirac material Sr3SnO. We find robust weak antilocalization (WAL) independent of the position of EF. The observed WAL is fitted using a single interference channel at low doping, which implies that the different Dirac valleys are mixed by disorder. Notably, this mixing does not suppress WAL, suggesting contrasting interference physics compared to graphene. We identify scattering among axially spin-momentum locked states as a key process that leads to a spin-orbital entanglement.

Lattice distortion in the spin-orbital entangled state in RVO3 perovskites

We report a thorough study of Y$_{0.7}$La$_{0.3}$VO$_3$ single crystals by measuring magnetic properties, specific heat, thermal conductivity, x-ray and neutron diffraction with the motivation of revealing the lattice response to the spin-orbital entanglement in \textit{R}VO$_3$. Upon cooling from room temperature, the orbitally disordered paramagnetic state changes around T*$\sim$220\,K to spin-orbital entangled state which is then followed by a transition at T$_N$=116\,K to C-type orbital ordered (OO) and G-type antiferromagnetic ordered (AF) ground state. In the temperature interval T$_N<T<T^*$, the VO$_{6/2}$ octahedra have two comparable in-plane V-O bonds which are longer than the out-of-plane V-O1 bond. This local structural distortion supports the spin-orbital entanglement of partially filled and degenerate yz/zx orbitals. However, this distortion is incompatible with the steric octahedral site distortion intrinsic to orthorhombic perovskites. Their competition induces a second order transition from the spin-orbital entangled state to C-OO/G-AF ground state where the long range OO suppresses the spin-orbital entanglement. Our analysis suggests that the spin-orbital entangled state and G-OO are comparable in energy and compete with each other. Rare earth site disorder favors the spin-orbital entanglement rather than a cooperative Jahn-Teller distortion. The results also indicate for LaVO$_3$ a C-OO/G-AF state in T$_t$\,$\leq$\,T\,$\leq$T$_N$ and an orbital flipping transition at T$_t$.

Octahedral tilting induced isospin reorientation transition in iridate heterostructures

Iridate heterostructures are gaining interest as their magnetic properties are much more sensitive to structural distortion compared to pure spin systems due to spin-orbital entanglement induced by strong spin-orbit coupling. While bulk monolayer and bilayer iridates show $ab$-plane canted and $c$-axis antiferromagnetic (AFM) order, recent experiments on layered iridate superlattices (SL) have revealed striking properties, especially in the bilayer SL. A spin model is presented including the tilting induced Kitaev type interactions, which illustrates the proclivity towards $ab$-plane canted AFM order. A realistic Hubbard model including spin-dependent hopping terms arising from octahedral rotation and tilting is constructed for the bilayer SL in isospin space, and magnetic excitations are investigated in the self-consistently determined magnetic state. The Hubbard model analysis confirms the spin model results and shows strongly reduced magnon energy gap and an isospin reorientation transition from $c$-axis to $ab$-plane canted AFM order with increasing tilting.