Robust Electric‐Field Control of Colossal Exchange Bias in CrI₃ Homotrilayer

Controlling exchange bias (EB) by electric fields is crucial for next-generation magnetic random access memories and spintronics with ultralow energy consumption and ultrahigh speed. Multiferroic heterostructures have been traditionally used to electrically control EB and interfacial ferromagnetism through weak/indirect coupling between ferromagnetic and ferroelectric films. However, three major bottlenecks (lattice mismatch, interface defects, and weak/indirect coupling in multiferroic heterostructures) remain, resulting in only a few tens of milli-tesla EB field. Here, this study reports a robust electric-field control recipe to dynamically tailor the EB effect in a pure CrI₃ homotrilayer on a ferroelectric Y-doped HfO₂ (HYO) substrate, and demonstrate a colossal and tunable EB field (H_E) from -0.15 to +0.33 T, giving rise to an EB modulation of 0.48 T. The charge doping due to ferroelectric HYO film divides a homo-configuration of CrI₃ homotrilayer into one antiferromagnetic (AFM) bilayer CrI₃ and one ferromagnetic (FM) monolayer CrI₃, favoring direct exchange coupling. The synergies of charge doping and electric field induce a transition of magnetic orders from AFM to FM phase in bilayer CrI₃, which is also supported by first-principles calculations, leading to the robust electric control of colossal EB effect. The results therefore open numerous opportunities for exploring 2D spintronics, memories, and braininspired in-memory computing.