TY - JOUR
T1 - Charge Conservation beyond Uniformity
T2 - Spatially Inhomogeneous Electromagnetic Response in Periodic Solids
AU - McKay, Robert C.
AU - Mahmood, Fahad
AU - Bradlyn, Barry
N1 - The authors thank G. Monteiro, P. Rao, and M. Trigo for helpful discussions. The theoretical work of R. C. M. and B. B. in the development of the response theory formalism was supported by the Alfred P. Sloan Foundation and the National Science Foundation under Grant No. DMR-1945058. The numerical computation of response functions and the development of experimental proposals was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, Energy Frontier Research Center for Quantum Sensing and Quantum Materials through Grant No. DE-SC0021238. This work made use of the Illinois Campus Cluster, a computing resource that is operated by the Illinois Campus Cluster Program (ICCP) in conjunction with the National Center for Supercomputing Applications (NCSA) and which is supported by funds from the University of Illinois at Urbana-Champaign.
PY - 2024/1
Y1 - 2024/1
N2 - 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 ab initio 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.
AB - 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 ab initio 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.
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U2 - 10.1103/PhysRevX.14.011058
DO - 10.1103/PhysRevX.14.011058
M3 - Article
AN - SCOPUS:85188958754
SN - 2160-3308
VL - 14
JO - Physical Review X
JF - Physical Review X
IS - 1
M1 - 011058
ER -