Observation of tunable chiral spin textures with nonlinear optics.

Chiral spin textures, such as spin spirals and skyrmions, are key to advancing spintronics by enabling ultrathin, energy-efficient memory, and high-density data storage and processing. However, their realization remains hindered by the scarcity of suitable host materials and the formidable experimental challenges associated with the characterization of these intricate chiral magnetic states. Here, we report the observation of tunable chiral magnetic textures in van der Waals magnet CrPS4 with nonlinear optics. These tunable textures exhibit strong chiral third-order nonlinear optical responses, driven by interlayer and intralayer spin couplings under varying magnetic fields and temperatures. These pronounced chiral nonlinear optical responses highlight the potency and high sensitivity of the nonlinear optical readout for probing non-collinear magnetic orders. Moreover, our findings position van der Waals magnets and their heterostructures as an exceptional platform for reconfigurable spin-photonics and spintronics, unifying optical, electrical, and magnetic properties through unique intralayer and interlayer spin coupling properties and effective spin interaction between photons and electrons.