Direct evidence of a charge depletion region at the interface of Van der Waals monolayers and dielectric oxides: The case of superconducting FeSe/STO

Abstract

The discovery of two dimensional Van der Waals materials has opened up several possibilities for designing novel devices. Yet a more promising way of designing exotic heterostutures with improved physical properties is to grow a monolayer of these materials on a substrate. For example, in the field of superconductivity it has been demonstrated that the superconducting transition temperature of a monolayer of FeSe grown on some oxide substrates e.g., strontium titanate (STO) is by far higher than its bulk counterpart. Although the system has been considered as a model system for understanding the phenomenon of high-temperature superconductivity, the physical mechanism responsible for this high transition temperature is still highly under debate. Here using momentum and energy resolved high-resolution electron energy-loss spectroscopy we probe the dynamic charge response of the FeSe/STO(001) system and demonstrate that the frequency- and momentum-dependent dynamic charge response is not compatible with a simple film/substrate model. Our analysis reveals the existence of a depletion region at the interface between this Van der Waals monolayer and the substrate. The presence of the depletion layer, accompanied with a considerably large charge transfer from STO into the FeSe monolayer, leads to a strong renormalization of the STO energy bands and a substantial band bending at the interface. Our results shed light on the electronic complexities of the FeSe/oxide interfaces and pave the way of designing novel low-dimensional high-temperature superconductors through interface engineering. We anticipate that the observed phenomenon is rather general and can take place in many two dimensional Van der Waals monolayers brought in contact with dielectric oxides or semiconducting substrates.