Exchange Bias in Molecule/Fe3GeTe2 van der Waals Heterostructures via Spinterface Effects

The exfoliation of layered magnetic materials generates atomically thin flakes characterized by an ultrahigh surface sensitivity, which makes their magnetic properties tunable via external stimuli, such as electrostatic gating and proximity effects. Another powerful approach to engineer magnetic materials is molecular functionalization, generating hybrid interfaces with tailored magnetic interactions, called spinterfaces. However, spinterface effects have not yet been explored on layered magnetic materials. Here, the emergence of spinterface effects is demonstrated at the interface between flakes of the prototypical layered magnetic metal Fe3GeTe2 and thin films of Co‐phthalocyanine. Magnetotransport measurements show that the molecular layer induces a magnetic exchange bias in Fe3GeTe2, indicating that the unpaired spins in Co‐phthalocyanine develop antiferromagnetic ordering and pin the magnetization reversal of Fe3GeTe2 via magnetic proximity. The effect is strongest for a Fe3GeTe2 thickness of 20 nm, for which the exchange bias field reaches −840 Oe at 10 K and is measurable up to ≈110 K. This value compares very favorably with previous exchange bias fields reported for Fe3GeTe2 in all‐inorganic van der Waals heterostructures, demonstrating the potential of molecular functionalization to tailor the magnetism of van der Waals layered materials. Spinterface effects are demonstrated in a hybrid van der Waals heterostructure composed of a CoPc film interfaced with a layered ferromagnet Fe3GeTe2. The interface interactions introduce an exchange bias field in Fe3GeTe2, which is among the strongest reported for layered magnetic materials. The results demonstrate the potential of molecular functionalization for tailoring the magnetic properties of layered materials.