Spin-orbit-enhanced magnetic surface second-harmonic generation in Sr₂IrO₄

Abstract

An anomalous optical second-harmonic generation (SHG) signal was previously reported in Sr₂IrO₄ and attributed to a hidden odd-parity bulk magnetic state. Here we investigate the origin of this SHG signal using a combination of bulk magnetic susceptibility, magnetic-field-dependent SHG rotational anisotropy, and overlapping wide-field SHG imaging and atomic force microscopy measurements. We find that the anomalous SHG signal exhibits a twofold rotational symmetry as a function of in-plane magnetic field orientation that is associated with a crystallographic distortion. We also show a change in SHG signal across step edges that tracks the bulk antiferromagnetic stacking pattern. While we do not rule out the existence of hidden order in Sr₂IrO₄, our results altogether show that the anomalous SHG signal in parent Sr₂IrO₄ originates instead from a surface-magnetization-induced electric-dipole process that is enhanced by strong spin-orbit coupling.