Superconducting Two-Dimensional FeSe Grown on the Fe-Enriched Interface

Two-dimensional (2D) tetragonal FeSe has sparked extensive research interest owing to its tunable superconductivity, providing valuable insights into the design of high-temperature superconductors. Currently, the intricate Fe–Se phase diagram poses a challenge to the controlled synthesis of superconducting 2D FeSe in a pure tetragonal phase. Here, we exploit the ion-exchange property of fluorophlogopite mica to devise a straightforward approach for the phase-controlled synthesis of tetragonal FeSe on an Fe-enriched mica surface within a molten salt environment. This method successfully produces highly crystalline FeSe in a pure tetragonal phase with adjustable thickness. We investigated the surface composition of the postgrowth mica substrate using various microscopic and spectroscopic characterizations to highlight the importance of the Fe-enriched growth interface in the phase-selective synthesis of 2D tetragonal FeSe. The obtained 2D FeSe exhibited 2D superconductivity, comparable to that of FeSe mechanically exfoliated from bulk crystals, confirming the high quality of our samples. Beyond tetragonal FeSe, 2D antiferromagnetic FeTe and superconducting FeS x Se y Te 1– x – y have been phase-selectively synthesized via this approach. Our study elucidates the significance of the growth interface on the phase-selective synthesis of 2D materials and presents potential opportunities for the phase-controlled synthesis of 2D multiphase materials via the rational design of the growth interface.