Anomalous Tunneling Magnetoresistance Oscillation and Electrically Tunable Tunneling Anisotropic Magnetoresistance in Few‐Layer CrPS₄

Abstract 2D van der Waals (vdW) magnets with layer‐dependent magnetic states and/or diverse magnetic interactions and anisotropies have attracted extensive research interest. Despite the advances, a notable challenge persists in effectively manipulating the tunneling anisotropic magnetoresistance (TAMR) of 2D vdW magnet‐based magnetic tunnel junctions (MTJs). Here, this study reports the novel and anomalous tunneling magnetoresistance (TMR) oscillations and pioneering demonstration of bias and gate voltage controllable TAMR in 2D vdW MTJs, utilizing few‐layer CrPS 4 . This material, inherently an antiferromagnet, transitions to a canted magnetic order upon application of external magnetic fields. Through TMR measurements, this work unveils the novel layer‐dependent oscillations in the tunneling resistance for few‐layer CrPS 4 devices under both out‐of‐plane and in‐plane magnetic fields, with a pronounced controllability via gate voltage. Intriguingly, this study demonstrates that both the polarity and magnitude of TAMR in CrPS 4 can be effectively tuned through either a bias or gate voltage. The mechanism behind this electrically tunable TAMR is further elucidated through first‐principles calculations. The implications of the findings are far‐reaching, providing new insights into 2D magnetism and opening avenues for the development of innovative spintronic devices based on 2D vdW magnets.