Basic formulation and first-principles implementation of nonlinear magneto-optical effects

Abstract

First-principles calculation of nonlinear magneto-optical effects has become an indispensable tool to reveal the geometric and topological nature of electronic states and to understand light-matter interactions. While intriguingly rich physics could emerge in magnetic materials, further methodological developments are required to deal with time-reversal symmetry breaking, due to the degeneracy and gauge problems caused by symmetry and the low-frequency divergence problem in the existing calculation formalism. Here we present a gauge-covariant and low-frequency convergent formalism for the first-principles computation. Remarkably, this formalism generally works for both non-magnetic and magnetic materials with or without band degeneracy. Reliability and capability of our method are demonstrated by studying example materials (i.e., bilayers of MnBi${}_2$Te${}_4$ and CrI${}_3$) and comparing with published results. Moreover, an importance correction term that ensures gauge covariance of degenerate states is derived, whose influence on physical responses is systematically checked. Our method enables computation of nonlinear magneto-optical effects in magnetic materials and paves the way for exploring rich physics created by the interplay of light and magnetism.

References in corpus (4)

• On A Proper Definition of Spin Current
• First-Principles Studies of Second-Order Nonlinear Optical Properties of Organic-Inorganic Hybrid Halide Perovskites
• Antiferromagnetism-induced second-order nonlinear optical responses of centrosymmetric bilayer CrI${}_3$
• Intrinsic Spin Photogalvanic Effect in Nonmagnetic Insulator

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• Spin-chirality-driven second-harmonic generation in two-dimensional magnet CrSBr
• Stacking-dependent Electronic and Topological Properties in van der Waals Antiferromagnet MnBi${}_2$Te${}_4$ Films
• Unidirectional valley-contrasting photo-current in strained transition metal dichalcogenide monolayers
• Skin Effect of Nonlinear Optical Responses in Antiferromagnets
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• TensorSymmetry: a package to get symmetry-adapted tensors disentangling spin-orbit coupling effect and establishing analytical relationship with magnetic order
• Magnetism-induced second-order nonlinear optical responses in multiferroic BiFeO${}_3$
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