Honeycomb or triangular lattices were extensively studied and thought to be proper platforms for realizing quantum anomalous Hall effect (QAHE), where magnetism is usually caused by d orbitals of transition metals. Here we propose that square lattice can host three magnetic topological states, including the fully spin polarized nodal loop semimetal, QAHE and topologically trivial ferromagnetic semiconductor, in terms of the symmetry and k$\cdot$p model analyses that are materials-independent. A phase diagram is presented. We further show that the above three magnetic topological states can be indeed implemented in two-dimensional (2D) materials ScLiCl5, LiScZ5 (Z=Cl, Br), and ScLiBr5, respectively. The ferromagnetism in these 2D materials is microscopically revealed from p electrons of halogen atoms. This present study opens a door to explore the exotic topological states as well as quantum magnetism from p-orbital electrons by means of the materials-independent approach.
We predict from first principles an entirely topological orbital magnetization in the noncoplanar bulk antiferromagnet $γ$-FeMn originating in the nontrivial topology of the underlying spin structure, without any reference to spin-orbit interaction. Studying the influence of strain, composition ratio, and spin texture on the topological orbital magnetization and the accompanying topological Hall effect, we promote the scalar spin chirality as key mechanism lifting the orbital degeneracy. The system is thus a prototypical topological orbital ferromagnet, the macroscopic orbital magnetization of…
Tuning the spin-orbit coupling strength via foreign element doping and/or modifying bonding strength via strain engineering are the major routes to convert normal insulators to topological insulators. We here propose an alternative strategy to realize topological phase transition by tuning the orbital level. Following this strategy, our first-principles calculations demonstrate that a topological phase transition in some cubic perovskite-type compounds CsGeBr$_3$ and CsSnBr$_3$ could be facilitated by carbon substitutional doping. Such unique topological phase transition predominantly results …
We address the importance of the modern theory of orbital magnetization for spintronics. Based on an all-electron first-principles approach, we demonstrate that the predictive power of the routinely employed "atom-centered" approximation is limited to materials like elemental bulk ferromagnets, while the application of the modern theory of orbital magnetization is crucial in chemically or structurally inhomogeneous systems such as magnetic thin films, and materials exhibiting non-trivial topology in reciprocal and real space,~e.g.,~Chern insulators or non-collinear systems. We find that the mo…
We explore via density functional calculations the magnetic doping of a topological ferroelectric as an unconventional route to multiferroicity. Vanadium doping of the layered perovskite La$_{2}$Ti$_{2}$O$_{7}$ largely preserves electric polarization and produces robust ferromagnetic order, hence proper multiferroicity. The marked tendency of dopants to cluster into chains results in an insulating character at generic doping. Ferromagnetism stems from the symmetry breaking of the multi-orbital V system via an unusual "antiferro"-orbital order, and from the host's low-symmetry layered structure…
Electrons which are slowly moving through chiral magnetic textures can effectively be described as if they where influenced by electromagnetic fields emerging from the real-space topology. This adiabatic viewpoint has been very successful in predicting physical properties of chiral magnets. Here, based on a rigorous quantum-mechanical approach, we unravel the emergence of chiral and topological orbital magnetism in one- and two-dimensional spin systems. We uncover that the quantized orbital magnetism in the adiabatic limit can be understood as a Landau-Peierls response to the emergent magnetic…
We reveal a class of three-dimensional $d$-orbital topological materials in the antifluorite Cu$_2$S family. Derived from the unique properties of low-energy $t_{2g}$ states, their phases are solely determined by the sign of spin-orbit coupling (SOC): topological insulator for negative SOC, whereas topological semimetal for positive SOC; both having Dirac-cone surface states but with contrasting helicities. With broken inversion symmetry, the semimetal becomes one with a nodal box consisting of butterfly-shaped nodal lines that are robust against SOC. Further breaking the tetrahedral symmetry …
We show that there is a fundamental difference between spin Hall current and orbital angular momentum Hall current in Rashba- Dresselhaus spin orbit coupling systems. The orbital angular momentum Hall current has a pure topological contribution which is originated from the existence of magnetic flux in momentum space while there is no such topological nature for the spin Hall current. Moreover, we show that the orbital Hall conductance is always larger than the spin Hall conductance in the presence of both couplings. The topological part is expected to be free from the effect of disorder due t…
Many materials crystallize in structure types that feature a square-net of atoms. While these compounds can exhibit many different properties, some members of this family are topological materials. Within the square-net-based topological materials, the observed properties are rich, ranging for example from nodal-line semimetals to a bulk half-integer quantum Hall effect. Hence, the potential for guided design of topological properties is enormous. Here we provide an overview of the crystallographic and electronic properties of these phases and show how they are linked, with the goal of underst…
Based on the generalized valence bond picture, a Schwinger boson mean field theory is applied to the symmetric SU(4) spin-orbital systems. For a two-leg SU(4) ladder, the ground state is a spin-orbital liquid with a finite energy gap, in good agreement with recent numerical calculations. In two-dimensional square and triangle lattices, the SU(4) Schwinger bosons condense at (π/2,π/2) and (π/3,π/3), respectively. Spin, orbital, and coupled spin-orbital static susceptibilities become singular at the wave vectors, twice of which the bose condensation arises at. It is also demonstrated that there …
Relativistic spin-orbit coupling plays an essential role in the field of topological insulators and quantum spintronics. It gives rise to the topological non-trivial band structure and enables electric manipulation of the spin degree of freedom. Because of the spin-orbit coupling, rich spin-orbital coupled textures can exist both in momentum and in real space. For three dimensional topological insulators in the Bi$_2$Se$_3$ family, topological surface states with p$_z$ orbitals have a left-handed spin texture for the upper Dirac cone and a right-handed spin texture for the lower Dirac cone. In…
Using a semiclassical Green's function formalism, we discover the emergence of chiral and topological orbital magnetism in two-dimensional chiral spin textures by explicitly finding the corrections to the orbital magnetization, proportional to the powers of the gradients of the texture. We show that in the absence of spin-orbit coupling, the resulting orbital moment can be understood as the electronic response to the emergent magnetic field associated with the real-space Berry curvature. By referring to the Rashba model, we demonstrate that by tuning the parameters of surface systems the engin…
The orbital degrees of freedom play a pivotal role in understanding fundamental phenomena in solid-state materials as well as exotic quantum states of matter including orbital superfluidity and topological semimetals. Despite tremendous efforts in engineering synthetic cold-atom, electronic and photonic lattices to explore orbital physics, thus far high orbitals in an important class of materials, namely, the higher-order topological insulators (HOTIs), have not been realized. Here, we demonstrate p-orbital corner states in a photonic HOTI, unveiling their underlying topological invariant, sym…
Two-dimensional (2D) materials have attracted much recent attention because they exhibit various distinct intrinsic properties/functionalities, which are, however, usually not interchangeable. Interestingly, here we propose a generic approach to convert 2D semiconductors, which are amply abundant, to 2D topological insulators (TIs), which are less available, via selective atomic adsorption and strain engineering. The approach is underlined by an orbital design principle that involves introducing an extrinsic s-orbital state into the intrinsic sp-bands of a 2D semiconductor, so as to induce s-p…
We study the evolution of spin-orbital correlations in an inhomogeneous quantum system with an impurity replacing a doublon by a holon orbital degree of freedom. Spin-orbital entanglement is large when spin correlations are antiferromagnetic, while for a ferromagnetic host we obtain a pure orbital description. In this regime the orbital model can be mapped on spinless fermions and we uncover topological phases with zero energy modes at the edge or at the domain between magnetically inequivalent regions.
Searching for functional square lattices in layered superconductor systems offers an explicit clue to modify the electron behavior and find exotic properties. The trigonal SnAs3 structural units in SnAs-based systems are relatively conformable to distortion, which provides the possibility to achieve structurally topological transformation and higher superconducting transition temperatures. In the present work, the functional As square lattice was realized and activated in Li0.6Sn2As2 and NaSnAs through a topotactic structural transformation of trigonal SnAs3 to square SnAs4 under pressure, res…
One of the most important properties of topological insulators (TIs) is the helical spin texture of the Dirac surface states, which has been theoretically and experimentally argued to be left-handed helical above the Dirac point and right handed helical below. However, since the spin is not a good quantum number in these strongly spin-orbit coupled systems, this can not be a complete statement, and we must consider the total angular momentum J = L + S that is a contribution of the spin and orbital terms. Using a combination of orbital and spin-resolved angle-resolved photoemission spectroscopy…
We explore spin dynamics in Cu(1,3-bdc), a quasi-2D topological magnon insulator. The results show that the thermal evolution of Landé $g$-factor ($g$) is anisotropic: $g_\textrm{in-plane}$ reduces while $g_\textrm{out-plane}$ increases with increasing temperature $T$. Moreover, the anisotropy of the $g$-factor ($Δg$) and the anisotropy of saturation magnetization ($ΔM_\textrm{s}$) are correlated below 4 K, but they diverge above 4 K. We show that the electronic orbital moment contributes to the $g$ anisotropy at lower $T$, while the topological orbital moment induced by thermally excited spin…
The concepts of Weyl fermions and topological semimetals emerging in three-dimensional momentum space are extensively explored owing to the vast variety of exotic properties that they give rise to. On the other hand, very little is known about semimetallic states emerging in two-dimensional magnetic materials, which present the foundation for both present and future information technology. Here, we demonstrate that including the magnetization direction into the topological analysis allows for a natural classification of topological semimetallic states that manifest in two-dimensional ferromagn…
Nonlinear optical responses are often used as a probe for studying electronic properties of materials. For topological materials, studies so far focused on the photogalvanic electric current, which requires breaking inversion symmetry. In this work we present a theory of orbital current response in inversion-symmetric topological insulators. We find a symmetry-allowed orbital current response that occurs in centrosymmetric materials under illumination by linearly polarized light. The sign of the dc nonlinear conductivity reflects the $\mathbb{Z}_2$ index and the conductivity changes sign at th…
Crossed magnetic responses between spin and orbital angular momentum are studied in time-reversal symmetric topological insulators. Due to spin-orbit coupling in the quantum spin Hall systems and three-dimensional topological insulators, the magnetic susceptibility has crossed (intersectional) components between spin and orbital part of magnetism. In this study, the crossed susceptibility for the orbital magnetization is studied in two- and three-dimensional topological insulator models, in which an external magnetic field interacts with the electron spin by Zeeman coupling via distinct g-fact…
Orbital degrees of freedom can have pronounced effects on the fundamental properties of electrons in solids. In addition to influencing bandwidths, gaps, correlation strength and dispersion, orbital effects have also been implicated in generating novel electronic and structural phases, such as Jahn-Teller effect and colossal magnetoresistance. In this work, we show for the first time how the orbital nature of bands can result in non-trivial effects of strain on the band structure. We use scanning tunneling microscopy and quasiparticle interference imaging to study the effects of strain on the …
Recently, a new class of second-order topological insulators (SOTIs) characterized by an electronic dipole has been theoretically introduced and proposed to host topological corner states. As a novel topological state, it has been attracting great interest and experimentally realized in artificial systems of various fields of physics based on multi-sublattice models, e.g., breathing kagome lattice. In order to realize such kind of SOTI in natural materials, we proposed a symmetry-faithful multi-orbital model. Then, we reveal several familiar transition metal dichalcogenide (TMD) monolayers as …
Quantum spin Hall (QSH) systems hold promises of low-power-consuming spintronic devices, yet their practical applications are extremely impeded by the small energy gaps. Fabricating QSH materials with large gaps, especially under the guidance of design principles, is essential for both scientific research and practical applications. Here, we demonstrate that large on-site atomic spin-orbit coupling can be directly exploited via the intriguing substrate-orbital-filtering effect to generate large-gap QSH systems and experimentally realized on the epitaxially synthesized ultraflat bismuthene on A…
The search for large gap quantum spin Hall (QSH) and quantum anomalous Hall (QAH) insulators is important both for fundamental and practical interests. The degenerate multi-orbitals $p_x,p_y$ in honeycomb lattice provides a paradigm for QSH state with a boosted topological gap of the first order in atomic spin-orbit coupling. By using elementary band representation, we explore the feasibility of this mechanism for QSH in general two-dimensional lattices, and find that the biparticle lattices with $C_{3v}$ or $C_{4v}$ symmetry and degenerate multi-orbitals could work. We further provide concret…
Topological insulators are novel macroscopic quantum-mechanical phase of matter, which hold promise for realizing some of the most exotic particles in physics as well as application towards spintronics and quantum computation. In all the known topological insulators, strong spin-orbit coupling is critical for the generation of the protected massless surface states. Consequently, a complete description of the Dirac state should include both the spin and orbital (spatial) parts of the wavefunction. For the family of materials with a single Dirac cone, theories and experiments agree qualitatively…
Topological aspects of the geometry of DNA and similar chiral molecules have received a lot of attention, while the topology of their electronic structure is less explored. Previous experiments have revealed that DNA can efficiently filter spin-polarized electrons between metal contacts, a process called chiral-induced spin-selectivity (CISS). However, the underlying correlation between chiral structure and electronic spin remains elusive. In this work, we reveal an orbital texture in the band structure, a topological characteristic induced by the chirality. We find that this orbital texture e…
The discovery of intriguing properties related to the Dirac states in graphene has spurred huge interest in exploring its two-dimensional group-IV counterparts, such as silicene, germanene, and stanene. However, these materials have to be obtained via synthesizing on substrates with strong interfacial interactions, which usually destroy their intrinsic $π$($p_z$)-orbital Dirac states. Here we report a theoretical study on the existence of Dirac states arising from the $p_{x,y}$ orbitals instead of $p_z$ orbitals in silicene on 4H-SiC(0001), which survive in spite of the strong interfacial inte…
We propose new two-dimensional (2D) topological insulators (TIs) in functionalized germanenes (GeX, X=H, F, Cl, Br or I) using first-principles calculations. We find GeI is a 2D TI with a bulk gap of about 0.3 eV, while GeH, GeF, GeCl and GeBr can be transformed into TIs with sizeable gaps under achievable tensile strains. A unique mechanism is revealed to be responsible for large topologically-nontrivial gap obtained: owing to the functionalization, the $σ$ orbitals with stronger spin-orbit coupling (SOC) dominate the states around the Fermi level, instead of original $π$ orbitals with weaker…
Research on graphene has revealed remarkable phenomena arising in the honeycomb lattice. However, the quantum spin Hall effect predicted at the K point could not be observed in graphene and other honeycomb structures of light elements due to an insufficiently strong spin-orbit coupling. Here we show theoretically that 2D honeycomb lattices of HgTe can combine the effects of the honeycomb geometry and strong spin-orbit coupling. The conduction bands, experimentally accessible via doping, can be described by a tight-binding lattice model as in graphene, but including multi-orbital degrees of fre…
The newly discovered topological crystalline insulators (TCIs) harbor a complex band structure involving multiple Dirac cones. These materials are potentially highly tunable by external electric field, temperature or strain and could find future applications in field-effect transistors, photodetectors, and nano-mechanical systems. Theoretically, it has been predicted that different Dirac cones, offset in energy and momentum-space, might harbor vastly different orbital character, a unique property which if experimentally realized, would present an ideal platform for accomplishing new spintronic…
Manganites are famous mostly for the colossal magnetoresistive effect, which involves the phase separation between ferromagnetic phase and charge-ordered CE-type antiferromagnetic phases. Furthermore, manganites contain some typical magnetic ferroelectrics, e.g. E-type antiferromagnetic $o$-HoMnO$_3$. Here we re-examined these zigzag-winding antiferromagnetic phases (CE-type and E-type antiferromagnets) from the topological perspective. Our theoretical analysis proved that the E-type phase is a weak topological insulator belonging to the $\mathbb{Z}$ class. In momentum space, we classify the s…
Topological magnon modes are expected to be useful for novel applications such as robust information propagation, since they are immune to backscattering and robust against disorder. Although there are several of theoretical proposals for topological magnon modes and growing experimental efforts for realizing them by now, it is still desirable to add complementary insights on this important phenomenon. Here, we propose a new scheme to achieve topological magnon where only nearest-neighbour exchange couplings on honeycomb lattice are necessary. In both ferromagnets and antiferromagnets, tuning …
Metamaterials made of periodic arrangements of electric permittivity and magnetic permeability and arrays of resonators can provide optic properties unexperienced in conventional materials, such as negative refractive index which can be used to achieve superlensing and cloaking. Developing new simpler structures with richer electromagnetic (EM) properties and wider working frequency bands is highly demanded for fast light-based information transfer and information processing. In the present work, we propose theoretically that a honeycomb-structured LC circuit with short-range textures in induc…
Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi$_4$Te$_7$ and MnBi$_6$Te$_{10}$, the $n=$~1 and 2 members of a modular (Bi$_2$Te$_3$)$_n$(MnBi$_2$Te$_4$) series, which have attracted recent interest as intrinsic magnetic topological insulators. Combining circular dichroic, spin-resolved and photon-energy-dependent ARPES measurements with calculations based on density functional theory, we unveil complex momentum-dependent orbital and spin textures in the surface electronic structure and disent…
We study Bi2Se3 by polarization-dependent angle-resolved photoemission spectroscopy (ARPES) and density-functional theory slab calculations. We find that the surface state Dirac fermions are characterized by a layer-dependent entangled spin-orbital texture, which becomes apparent through quantum interference effects. This explains the discrepancy between the spin polarization from spin-resovled ARPES - ranging from 20 to 85% - and the 100% value assumed in phenomenological models. It also suggests a way to probe the intrinsic spin texture of topological insulators, and to continuously manipula…
Topological Insulators are a novel state of matter where spectral bands are characterized by quantized topological invariants. This unique quantized non-local property commonly manifests through exotic bulk phenomena and corresponding robust boundary effects. In our work, we report a new type of topological insulator exhibiting spectral bands with non-quantized topological properties, but with a quantization that arises in a corresponding system where the square of the Hamiltonian is taken. We provide a thorough theoretical analysis as well as an experimental demonstration based on photonic Ah…
