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

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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.