Strongly Compressed Few-Layered SnSe₂ Films Grown on a SrTiO₃ Substrate: The Coexistence of Charge Ordering and Enhanced Interfacial Superconductivity

Abstract

High pressure has been demonstrated to be a powerful approach of producing novel condensed-matter states, particularly in tuning the superconducting transition temperature (<i>T</i>_c) of the superconductivity in a clean fashion without involving the complexity of chemical doping. However, the challenge of high-pressure experiment hinders further in-depth research for underlying mechanisms. Here, we have successfully synthesized continuous layer-controllable SnSe₂ films on SrTiO₃ substrate using molecular beam epitaxy. By means of scanning tunneling microscopy/spectroscopy (STM/S) and Raman spectroscopy, we found that the strong compressive strain is intrinsically built in few-layers films, with a largest equivalent pressure up to 23 GPa in the monolayer. Upon this, unusual 2 × 2 charge ordering is induced at the occupied states in the monolayer, accompanied by prominent decrease in the density of states (DOS) near the Fermi energy (<i>E</i>_F), resembling the gap states of CDW reported in transition metal dichalcogenide (TMD) materials. Subsequently, the coexistence of charge ordering and the interfacial superconductivity is observed in bilayer films as a result of releasing the compressive strain. In conjunction with spatially resolved spectroscopic study and first-principles calculation, we find that the enhanced interfacial superconductivity with an estimated <i>T</i>_c of 8.3 K is observed only in the 1 × 1 region. Such superconductivity can be ascribed to a combined effect of interfacial charge transfer and compressive strain, which leads to a considerable downshift of the conduction band minimum and an increase in the DOS at <i>E</i>_F. Our results provide an attractive platform for further in-depth investigation of compression-induced charge ordering (monolayer) and the interplay between charge ordering and superconductivity (bilayer). Meanwhile, it has opened up a pathway to prepare strongly compressed two-dimensional materials by growing onto a SrTiO₃ substrate, which is promising to induce superconductivity with a higher <i>T</i>_c.