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An anomalous optical second-harmonic generation (SHG) signal was previously reported in Sr$_2$IrO$_4$ 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 su sceptibility, 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 two-fold 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 Sr$_2$IrO$_4$, our results altogether show that the anomalous SHG signal in parent Sr$_2$IrO$_4$ originates instead from a surface-magnetization-induced electric-dipole process that is enhanced by strong spin-orbit coupling.
Understanding the complex phase diagram of cuprate superconductors is an outstanding challenge. The most actively studied questions surround the nature of the pseudogap and strange metal states and their relationship to superconductivity. In contrast , there is general agreement that the low energy physics of the Mott insulating parent state is well captured by a two-dimensional spin $S$ = 1/2 antiferromagnetic (AFM) Heisenberg model. However, recent observations of a large thermal Hall conductivity in several parent cuprates appear to defy this simple model and suggest proximity to a magneto-chiral state that breaks all mirror planes perpendicular to the CuO$_2$ layers. Here we use optical second harmonic generation to directly resolve the point group symmetries of the model parent cuprate Sr$_2$CuO$_2$Cl$_2$. We report evidence of an order parameter $Phi$ that breaks all perpendicular mirror planes and is consistent with a magneto-chiral state in zero magnetic field. Although $Phi$ is clearly coupled to the AFM order parameter, we are unable to realize its time-reversed partner ($-Phi$) by thermal cycling through the AFM transition temperature ($T_{textrm{N}}$ $approx$ 260 K) or by sampling different spatial locations. This suggests that $Phi$ onsets above $T_{textrm{N}}$ and may be relevant to the mechanism of pseudogap formation.
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