Thermodynamic Perspective on the Oxidation of Layered Materials and Surface Oxide Amelioration in 2D Devices

Surface oxidation is an unneglectable problem for 2D semiconductors because it hinders the practical application of 2D material-based devices. In this research, the oxidation of layered materials is investigated by a thermodynamic approach to verify their oxidation tendency. It was found that almost all 2D materials are thermodynamically unstable in the presence of oxygen at room temperature. Two potential solutions for surface oxidation are proposed in this work: (i) the conversion of the surface oxides to functional oxides through the deposition of active metals and (ii) the recovery of original 2D materials from the surface oxides by 2D material heterostructure formation with the same chalcogen group. Supported by thermodynamic calculations, both approaches are feasible to ameliorate the surface oxides of 2D materials by the appropriate selection of metals for deposition or 2D materials for heterostructure formation. Thermodynamic data of 64 elements and 75 2D materials are included and compared in this research, which can improve gate insulator or electrode contact material selection in 2D devices to solve the surface oxidation issue. For instance, yttrium and titanium are good candidates for surface oxide conversion, while zirconium and hafnium chalcogenide can trigger the recovery of original 2D materials from their surface oxides. The systematic diagrams presented in this work can serve as a guideline for considering surface oxidation in future device fabrication from various 2D materials.