Interfacial Polarons in van der Waals Heterojunction of Monolayer SnSe₂ on SrTiO₃ (001)

Abstract

Interfacial polarons have been demonstrated to play important roles in heterostructures containing polar substrates. However, most of polarons found so far are diffusive large polarons; the discovery and investigation of small polarons at interfaces are scarce. Herein, we report the emergence of interfacial polarons in monolayer SnSe₂ epitaxially grown on Nb-doped SrTiO₃ (STO) surface using angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). ARPES spectra taken on this heterointerface reveal a nearly flat in-gap band correlated with a significant charge modulation in real space as observed with STM. An interfacial polaronic model is proposed to ascribe this in-gap band to the formation of self-trapped small polarons induced by charge accumulation and electron-phonon coupling at the van der Waals interface of SnSe₂ and STO. Such a mechanism to form interfacial polaron is expected to generally exist in similar van der Waals heterojunctions consisting of layered 2D materials and polar substrates.