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Interfacial exchange coupling between antiferromagnets (AFMs) and ferromagnets (FMs) crucially makes it possible to shift the FM hysteresis, known as exchange bias, and to switch AFM states. Two-dimensional magnets unlock opportunities to combine AFM and FM materials; however, the buried AFM–FM interfaces obtained by stacking remains challenging to understand. Here we demonstrate interfacial control via intralayer exchange coupling in the layered AFM CrPS4, where connected even and odd layers realize pristine lateral interfaces between AFM-like and FM-like regions. We distinguish antiphase even-layer states by scanning nitrogen-vacancy centre (NV) magnetometry due to a weak surface magnetization. This surface magnetization enables control over the even-layer state, with different regions switching at distinct fields due to their own lateral couplings. We toggle three AFM domains adjacent to a FM-like region and demonstrate a tunable multilevel exchange bias. Our nanoscale visualization unveils the microscopic origins of exchange bias and advances single two-dimensional crystals for hybrid AFM–FM technologies. 

Abstract Since their first observation in 2017, atomically thin van der Waals (vdW) magnets have attracted significant fundamental, and application-driven attention. However, their low ordering temperatures,T_c, sensitivity to atmospheric conditions and difficulties in preparing clean large-area samples still present major limitations to further progress, especially amongst van der Waals magnetic semiconductors. The remarkably stable, high-T_cvdW magnet CrSBr has the potential to overcome these key shortcomings, but its nanoscale properties and rich magnetic phase diagram remain poorly understood. Here we use single spin magnetometry to quantitatively characterise saturation magnetization, magnetic anisotropy constants, and magnetic phase transitions in few-layer CrSBr by direct magnetic imaging. We show pristine magnetic phases, devoid of defects on micron length-scales, and demonstrate remarkable air-stability down the monolayer limit. We furthermore address the spin-flip transition in bilayer CrSBr by imaging the phase-coexistence of regions of antiferromagnetically (AFM) ordered and fully aligned spins. Our work will enable the engineering of exotic electronic and magnetic phases in CrSBr and the realization of novel nanomagnetic devices based on this highly promising vdW magnet.