Thickness-dependent degradation and optical access in epitaxial 2H-MoTe2 protected by metallic capping layers

Abstract

We investigate degradation and surface protection of epitaxial 2H-MoTe2 films grown by molecular beam epitaxy on GaAs(111)B substrates. Using X-ray photoelectron spectroscopy (XPS), scanning tunneling microscopy, atomic force microscopy (AFM), Kelvin probe microscopy (KPM), Raman spectroscopy, and density functional theory (DFT), we examine the structural, chemical, and electronic evolution of MoTe2 protected by Co and Ni capping layers. XPS shows that the metallic caps effectively suppress oxidation during short-term air transfer, while revealing a pronounced Te-rich near-surface composition. With time, the caps become increasingly difficult to remove, suggesting gradual interfacial bonding promoted by excess tellurium and defect-rich MoTe2 interfaces. AFM and KPM reveal pronounced thickness-dependent ageing, with ultrathin regions showing markedly different contact-potential evolution from thicker films. DFT calculations support the sensitivity of work function and density of states to thickness and surface chemistry. Raman measurements through approximately 20 nm thick metallic caps demonstrate partial optical access to the protected material. Additional AFM and Raman observations suggest local formation of Te-rich nanostructures under laser illumination or near mechanically damaged regions. These results provide practical guidelines for protecting, transferring, delaminating, and optically characterizing air-sensitive MoTe2 and related van der Waals materials.