The discovery of high-temperature (Tc) superconductivity in monolayer FeSe on SrTiO3 raised a fundamental question whether high Tc is commonly realized in monolayer iron-based superconductors. Tetragonal FeS is a key material to resolve this issue because bulk FeS is a superconductor with Tc comparable to that of isostructural FeSe. However, difficulty in synthesizing tetragonal monolayer FeS due to its metastable nature has hindered further investigations. Here we report elucidation of band structure of monolayer FeS on SrTiO3, enabled by a unique combination of in-situ topotactic reaction and molecular-beam epitaxy. Our angle-resolved photoemission spectroscopy on FeS and FeSe revealed marked similarities in the electronic structure, such as heavy electron doping and interfacial electron-phonon coupling, both of which have been regarded as possible sources of high Tc in FeSe. However, surprisingly, high-Tc superconductivity is absent in monolayer FeS. This is linked to the weak superconducting pairing in electron-doped multilayer FeS in which the interfacial effects are absent. Our results strongly suggest that the cross-interface electron-phonon coupling enhances Tc only when it cooperates with the pairing interaction inherent to the superconducting layer. This finding provides a key insight to explore new heterointerface high-Tc superconductors.

We have performed angle-resolved photoemission spectroscopy on a heterostructure consisting of topological insulator Bi 2 Te 3 and iron chalcogenide FeTe fabricated on SrTiO 3 substrate by molecular-beam-epitaxy technique. This system was recently found to show superconductivity albeit non-superconducting nature of each constituent material. Upon interfacing FeTe with two quintuple layers of Bi 2 Te 3 , we found that the Dirac-cone surface state of Bi 2 Te 3 is shifted toward higher binding energy, while the holelike band at the Fermi level originating from FeTe moves toward lower binding energy. This suggests that electron charge transfer takes place from FeTe to Bi 2 Te 3 through the interface. The present result points to importance of hole-doped FeTe interface for the occurrence of unconventional superconductivity.