Large enhancement of Curie temperature in Fe3GeTe2 by Fe intercalation in the van der Waals gap

Abstract The magnetic and electrical transport properties of the two-dimensional ferromagnetic Fe3GeTe2 have proven to be a subject of intrigue, with a broad range of Curie temperatures (Tc) observed in recent studies, ranging from 160 K to 230 K, and even reaching room temperature by ionic gating. Despite these discoveries, the underlying mechanism behind the varying Tc values remains a puzzle. Here, we employed scanning transmission electron microscopy to explore the atomic structure of Fe3GeTe2 crystals exhibiting Tc values of 160, 210, and 230 K. The results of the elemental mapping reveal that Fe intercalation on the interstitial sites within the van der Waals gap is present in the high- Tc (210 and 230 K) samples. The electrical transport measurements demonstrate the presence of an exchange bias effect in these high- Tc samples, owing to the existence of ferromagnetic and antiferromagnetic interfaces, while this effect is absent in the low-Tc (160 K) samples. First-principles calculations further suggest that the Fe-intercalation layer may be responsible for the local antiferromagnetic coupling that gives rise to the exchange bias effect, and that the introduction of interlayer exchange paths greatly contributes to the enhancement of Tc. This discovery of the Fe-intercalation layer elucidates the mechanism behind the hidden antiferromagnetic ordering that underlies the enhancement of Tc in Fe3GeTe2.