Polarity‐Reversal of Exchange Bias in van der Waals FePS3/Fe3GaTe2 Heterostructures

Exchange bias (EB) in antiferromagnetic (AFM)/ferromagnetic heterostructures is crucial for the advancement of spintronic devices and has attracted significant attention. The common EB effect in van der Waals heterostructures features a low blocking temperature (Tb) and a single polarity. In this work, a significant EB effect with a Tb up to 150 K is observed in FePS3/Fe3GaTe2 heterostructures, and in particular, the EB exhibits an unusual temperature‐dependent polarity‐reversal behavior. Under a high positive field‐cooling condition (e.g., μ0H ≥ 0.5 T), a negative EB field (HEB) is observed at low temperatures, and with increasing temperature, the HEB crosses zero at ≈20 K, subsequently becomes positive and later approaches zero again at Tb. A model composed of a top FePS3/interfacial FePS3/Fe3GaTe2 sandwich structure is proposed. The charge transfer from Fe3GaTe2 to FePS3 at the interface induces net magnetic moments (∆M) in FePS3. The interface favors AFM coupling, and thus the reversal of ∆M of the interfacial FePS3 leads to the polarity‐reversal of EB. Moreover, the EB can be extended to the bare Fe3GaTe2 region of the Fe3GaTe2 flake partially covered by FePS3. This work provides opportunities for a deeper understanding of the EB effect and opens a new route toward constructing novel spintronic devices. A significant EB effect with temperature‐dependent polarity‐reversal behavior is observed in FePS3/Fe3GaTe2 heterostructures under high cooling fields (e.g., μ0H ≥ 0.5 T). A model composed of a top FePS3/interfacial FePS3/Fe3GaTe2 sandwich structure is proposed. Charge transfer from Fe3GaTe2 to FePS3 induces net magnetic moments (∆M) in FePS3, and the reversal of ∆M of interfacial FePS3 leads to the polarity‐reversal of EB.