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Nonlinear electromagnetic response functions have reemerged as a crucial tool for studying quantum materials, due to recently appreciated connections between optical response functions, quantum geometry, and band topology. Most attention has been paid to responses to spatially uniform electric fields, relevant to low-energy optical experiments in conventional solid state materials. However, magnetic and magnetoelectric phenomena are naturally connected by responses to spatially varying electric fields due to Maxwell’s equations. Furthermore, in the emerging field of moiré materials, characteristic lattice scales are much longer, allowing spatial variation of optical electric fields to potentially have a measurable effect in experiments. In order to address these issues, we develop a formalism for computing linear and nonlinear responses to spatially inhomogeneous electromagnetic fields. Starting with the continuity equation, we derive an expression for the second-quantized current operator that is manifestly conserved and model independent. Crucially, our formalism makes no assumptions on the form of the microscopic Hamiltonian and so is applicable to model Hamiltonians derived from tight-binding or calculations. We then develop a diagrammatic Kubo formalism for computing the wave vector dependence of linear and nonlinear conductivities, using Ward identities to fix the value of the diamagnetic current order by order in the vector potential. We apply our formula to compute the magnitude of the Kerr effect at oblique incidence for a model of a moiré-Chern insulator and demonstrate the experimental relevance of spatially inhomogeneous fields in these systems. We further show how our formalism allows us to compute the (orbital) magnetic multipole moments and magnetic susceptibilities in insulators. Turning to nonlinear response, we use our formalism to compute the second-order transverse response to spatially varying transverse electric fields in our moiré-Chern insulator model, with an eye toward the next generation of experiments in these systems. Published by the American Physical Society 2024
We use symmetry analysis and density-functional theory to determine and characterize surface terminations that have a finite equilibrium magnetization density in antiferromagnetic materials. A nonzero magnetic dipole moment per unit area or “surface magnetization” can arise on particular surfaces of many antiferromagnets due to the bulk magnetic symmetries. Such surface magnetization underlies intriguing physical phenomena like interfacial magnetic coupling and can be used as a readout method of antiferromagnetic domains. However, a universal description of antiferromagnetic surface magnetization is lacking. We first introduce a classification system based on whether the surface magnetization is either sensitive or robust to roughness and on whether the magnetic dipoles at surface of interest are compensated or uncompensated when the bulk magnetic order is retained at the surface. We show that roughness-sensitive categories can be identified by a simple extension of a previously established group-theory formalism for identifying roughness-robust surface magnetization. We then map the group-theory method of identifying surface magnetization to a novel description in terms of bulk magnetic multipoles, which are already established as symmetry indicators for bulk magnetoelectric responses at both linear and higher orders. We use density-functional calculations to illustrate that nominally compensated surfaces in magnetoelectric Cr2O3 and centrosymmetric altermagnetic FeF2 develop a finite magnetization density at the surface, in agreement with our predictions based on both group theory and the ordering of the bulk multipoles. Our analysis provides a comprehensive basis for understanding the surface magnetic properties and their intimate correspondence to bulk magnetoelectric effects in antiferromagnets and has important implications for technologically relevant phenomena such as exchange-bias coupling. Published by the American Physical Society 2024
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