Layer-dependent magnetism and spin fluctuations in atomically thin van der Waals magnet CrPS4

Abstract: van der Waals (vdW) magnets, an emerging family of two-dimensional (2D) materials, have received tremendous attention due to their rich fundamental physics and significant potential for cutting-edge technological applications. In contrast to the conventional bulk counterparts, vdW magnets exhibit significant tunability of local material properties, such as stacking engineered interlayer coupling and layer-number dependent magnetic and electronic interactions, which promise to deliver previously unavailable merits to develop multifunctional microelectronic devices. As a further ingredient of this emerging topic, here we report nanoscale quantum sensing and imaging of atomically thin vdW magnet chromium thiophosphate CrPS4, revealing its characteristic layer-dependent 2D static magnetism and dynamic spin fluctuations. We also show a large tunneling magnetoresistance in CrPS4-based spin filter vdW heterostructures. The excellent material stability, robust strategy against environmental degradation, in combination with tailored magnetic properties highlight the potential of CrPS4 in developing state-of-the-art 2D spintronic devices for next-generation information technologies.