Role of double TiO2 layers at the interface of FeSe/SrTiO3 superconductors

We determine the surface reconstruction of SrTiO3 used to achieve superconducting FeSe films in experiments, which is different from the 1 x 1 TiO2-terminated SrTiO3 assumed by most previous theoretical studies. In particular, we identify the existence of a double TiO2 layer at the FeSe/SrTiO3 interface that plays two important roles. First, it facilitates the epitaxial growth of FeSe. Second, ab initio calculations reveal a strong tendency for electrons to transfer from an oxygen deficient SrTiO3 surface to FeSe when the double TiO2 layer is present. The double layer helps to remove the hole pocket in the FeSe at the Gamma point of the Brillouin zone and leads to a band structure characteristic of superconducting samples. The characterization of the interface structure presented here is a key step towards the resolution of many open questions about this superconductor.