Manipulation of Lateral Exchange Bias Via Ion Intercalation

Lateral exchange bias, arising between spatially adjacent ferromagnetic and antiferromagnetic regions, introduces a new dimension to the conventional exchange bias effect—a cornerstone of magnetic memory technologies. However, its realization has largely relied on uncontrolled thickness inhomogeneity formed during material synthesis, severely limiting active tunability. Here, we demonstrate the controllable manipulation of lateral exchange bias in CrSBr through ion intercalation. By modulating the concentration of organic ions, the interlayer magnetic coupling is continuously tuned from antiferromagnetic (AFM) to ferromagnetic (FM), enabling precise control over the phase fraction between coexisting AFM‐CrSBr and FM‐CrSBr phases. Consequently, the lateral exchange bias can be continuously regulated and directly mapped via spin‐filter tunneling magnetoresistance (sf‐TMR). Furthermore, our results suggest that the AFM‐CrSBr region exerts a pinning effect on the FM‐CrSBr matrix, stabilizing a metastable interlayer antiparallel configuration within the intercalated FM‐CrSBr. This emergent magnetic state gives rise to a distinct hysteresis loop absent in pristine CrSBr and generates a pronounced nonvolatile sf‐TMR signal. Micromagnetic simulations suggest that a reduction in domain wall density can help stabilize this metastable antiparallel state, providing a possible mechanism consistent with the experimental observations. Besides the fundamental significance, our finding highlights the promise of sf‐TMR for next‐generation nonvolatile antiferromagnetic memory.