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Register a new userRole of Berry phase theory for describing orbital magnetism: From magnetic heterostructures to topological orbital ferromagnets
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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 modern theory is particularly crucial for describing magnetism in a class of materials that we suggest here $-$ topological orbital ferromagnets.
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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 field. Our central result is that the spin-orbit interaction in interfacial skyrmions and domain walls can be used to tune the orbital magnetism over orders of magnitude by merging the real-space topology with the topology in reciprocal space. Our findings point out the route to experimental engineering of orbital properties of chiral spin systems, thereby paving the way to the field of chiral orbitronics.
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 use symmetry analysis and first principles calculations to show that the linear magnetoelectric effect can originate from the response of orbital magnetic moments to the polar distortions induced by an applied electric field. Using LiFePO4 as a model compound we show that spin-orbit coupling partially lifts the quenching of the 3d orbitals and causes small orbital magnetic moments ($mu_{(L)}approx 0.3 mu_B$) parallel to the spins of the Fe$^{2+}$ ions. An applied electric field $mathbf{E}$ modifies the size of these orbital magnetic moments inducing a net magnetization linear in $mathbf{E}$.
We derive a quantum-mechanical formula of the orbital magnetic quadrupole moment (MQM) in periodic systems by using the gauge-covariant gradient expansion. This formula is valid for insulators and metals at zero and finite temperature. We also prove a direct relation between the MQM and magnetoelectric (ME) susceptibility for insulators at zero temperature. It indicates that the MQM is a microscopic origin of the ME effect. Using the formula, we quantitatively estimate these quantities for room-temperature antiferromagnetic semiconductors BaMn$_2$As$_2$ and CeMn$_2$Ge$_{2 - x}$Si$_x$. We find that the orbital contribution to the ME susceptibility is comparable with or even dominant over the spin contribution.
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 band inversion for a TI phase, as demonstrated by tight-binding model analyses. Remarkably, based on first-principles calculations, we apply this approach to convert the semiconducting monolayer CuS and CuTe into a TI by adsorbing Na and K respectively with a proper s-level energy, and CuSe into a TI by adsorbing a mixture of Na and K with a tuned s-level energy or by adsorbing either Na or K on a strained CuSe with a tuned p-level valence band edge. Our findings open a new door to the discovery of TIs by a predictive materials design, beyond finding a preexisting 2D TI.
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