Chemical Composition Control at the Substrate Interface as the Key for FeSe Thin-Film Growth.

The strong fascination exerted by the binary compound of FeSe demands reliable engineering protocols and more effective approaches toward inducing superconductivity in FeSe thin films. Our study addresses the peculiarities in pulsed laser deposition that determine FeSe thin-film growth and focuses on the film/substrate interface, which has only been considered hypothetically in the past literature. The FeSe/MgO interface has been assumed (1) to be clean and (2) to obey lattice-matching epitaxy. Our studies reveal that both assumptions are misleading and demonstrate the tendency for domain-matching epitaxial growth, which accompanies the problem of chemical heterogeneity. We propose that homogenization of the film/substrate interface by an Fe buffer can improve the control of stoichiometry and nanostrain in a way that favors superconductivity even in ultrathin FeSe films. We will also show that on a chemically homogenized FeSe/Fe interface, the control of film texture with preparation conditions is still possible.