Fe‐Intercalation Dominated Ferromagnetism of van der Waals Fe3GeTe2

Fe3 GeTe2 have proven to be of greatly intrigue. However, the underlying mechanism behind the varying Curie temperature (Tc ) values remains a puzzle. This study explores the atomic structure of Fe3 GeTe2 crystals exhibiting Tc values of 160, 210, and 230 K. The elemental mapping reveals a Fe-intercalation on the interstitial sites within the van der Waals gap of the high-Tc (210 and 230 K) samples, which are observed to have an exchange bias effect by electrical transport measurements, while Fe intercalation or the bias 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 interlayer exchange paths greatly contribute 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 Fe3 GeTe2 .