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The interface between transition metal compounds provides a rich playground for emergent phenomena. Recently, significantly enhanced superconductivity has been reported for single-layer FeSe on Nb-doped SrTiO
3
substrate. Yet it remains mysterious how the interface affects the superconductivity. Here we use
in situ
angle-resolved photoemission spectroscopy to investigate various FeSe-based heterostructures grown by molecular beam epitaxy, and uncover that electronic correlations and superconducting gap-closing temperature (
T
g
) are tuned by interfacial effects.
T
g
up to 75 K is observed in extremely tensile-strained single-layer FeSe on Nb-doped BaTiO
3
, which sets a record high pairing temperature for both Fe-based superconductor and monolayer-thick films, providing a promising prospect on realizing more cost-effective superconducting device. Moreover, our results exclude the direct correlation between superconductivity and tensile strain or the energy of an interfacial phonon mode, and highlight the critical and non-trivial role of FeSe/oxide interface on the high
T
g
, which provides new clues for understanding its origin.
Individual layers of FeSe grown on SrTiO3 superconduct at far higher temperatures than in bulk, but the effect of the film-substrate interface is poorly understood. Peng
et al
. find that modifying this interface has a significant non-trivial effect on the superconducting characteristics of FeSe films.