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The recent discovery of two-dimensional (2D) magnets offers unique opportunities for the experimental exploration of low-dimensional magnetism4 and the magnetic proximity effects, and for the development of novel magnetoelectric, magnetooptic and spintronic devices. These advancements call for 2D materials with diverse magnetic structures as well as effective probes for their magnetic symmetries, which is key to understanding intralayer magnetic order and interlayer magnetic coupling. Here we apply second harmonic generation (SHG), a technique acutely sensitive to symmetry breaking, to probe the magnetic structure of a new 2D magnetic semiconductor, CrSBr. We find that CrSBr monolayers are ferromagnetically ordered below 146 K, an observation enabled by the discovery of a giant magnetic dipole SHG effect in the centrosymmetric 2D structure. In multilayers, the ferromagnetic monolayers are coupled antiferromagnetically, with the Neel temperature notably increasing with decreasing layer number. The magnetic structure of CrSBr, comprising spins co-aligned in-plane with rectangular unit cell, differs markedly from the prototypical 2D hexagonal magnets CrI3 and Cr2Ge2Te6 with out-of-plane moments. Moreover, our SHG analysis suggests that the order parameters of the ferromagnetic monolayer and the antiferromagnetic bilayer are the magnetic dipole and the magnetic toroidal moments, respectively. These findings establish CrSBr as an exciting 2D magnetic semiconductor and SHG as a powerful tool to probe 2D magnetic symmetry, opening the door to the exploration of coupling between magnetic order and excitonic/electronic properties, as well as the magnetic toroidal moment, in a broad range of applications.
Two-dimensional (2D) ferromagnets have recently drawn extensive attention, and here we study the electronic structure and magnetic properties of the bulk and monolayer of CrSBr, using first-principles calculations and Monte Carlo simulations. Our res
The recent discovery of magnetism within the family of exfoliatable van der Waals (vdW) compounds has attracted considerable interest in these materials for both fundamental research and technological applications. However current vdW magnets are lim
We investigate the dynamic nuclear polarization from the hyperfine interaction between nonequilibrium electronic spins and nuclear spins coupled to them in semiconductor nanostructures. We derive the time and position dependence of the induced nuclea
Recent claims of an experimental demonstration of spontaneous spin polarisation in dilute electron gases cite{young99} revived long standing theoretical discussions cite{ceper99,bloch}. In two dimensions, the stabilisation of a ferromagnetic fluid mi
Magnetic semiconductors are a powerful platform for understanding, utilizing and tuning the interplay between magnetic order and electronic transport. Compared to bulk crystals, two-dimensional magnetic semiconductors have greater tunability, as illu