Dilemma in All-optical Characterization of Single-layer NiI2 Multiferroics

Matters Arising in Nature on “Evidence for a single layer van der Waals multiferroic”. The search for two dimensional multiferroic materials is an exciting yet challenging endeavor. Recently, Song reported the exciting discovery of type II multiferroic order in an antiferromagnetic (AFM) NiI2 single layer and concluded the ferroelectric (FE) polarization induced by a helical magnetic order1. Their finding was presented from all optical experimental evidence, based on the methods of second harmonic generation (SHG) and linear dichroism (LD). However, the all optical characterizations cannot serve as unanimous evidence of the FE existence, particularly in conjunction with magnetic orders in a single layer NiI2 multiferroic. We have designed and built a Magneto-Optical-Electric Joint-measurement Scanning Imaging system (MOEJSI) for identification of two-dimensional vdW multiferroic.