Broadband nonlinear Hall response and multiple wave mixing in a room temperature altermagnet

Abstract

Crystalline symmetries determine the linear and nonlinear response of materials to external stimuli such as mechanical pressure and electromagnetic fields, governing phenomena such as piezoelectricity, optical activity, and multiple wave mixing with wide ranging technological applications. Altermagnets present a new class of materials with magnetic crystalline order where specific crystal symmetry operations connect antiferromagnetic sublattices, leading to non-relativistic spin-splitting of the electronic band structure. Hence, the electric material properties of altermagnets should uniquely mirror these underlying symmetry properties, potentially giving rise to novel phenomena in response to external driving fields. Here, we report the discovery of a broadband third-order nonlinear anomalous Hall effect in altermagnetic CrSb at room temperature. The comparison of our observations with symmetry analyses and model calculations shows that this nonlinear Hall response is induced by the nonlinear electric susceptibility of a Berry curvature quadrupole, which exists within the spin-split band structure of CrSb and is characterized by the underlying crystalline and magnetic symmetries. We then utilize this third-order nonlinear electric susceptibility of CrSb to realize a multiple wave mixing device with pronounced four wave mixing output, which could, in principle, be extended to THz frequencies. Our study discovers that the crystalline magnetic order of altermagnets determines their nonlinear electric material properties, which could facilitate applications in high-frequency electronics, THz generation, communication networks, and energy harvesting.