Surface Diffusion and Epitaxial Self‐Planarization for Wafer‐Scale Single‐Grain Metal Chalcogenide Thin Films

Abstract Although wafer‐scale single‐grain thin films of 2D metal chalcogenides (MCs) have been extensively sought after during the last decade, the grain size of the MC thin films is still limited in the sub‐millimeter scale. A general strategy of synthesizing wafer‐scale single‐grain MC thin films by using commercial wafers (Si, Ge, GaAs) both as metal source and epitaxial collimator is presented. A new mechanism of single‐grain thin‐film formation, surface diffusion, and epitaxial self‐planarization is proposed, where chalcogen elements migrate preferentially along substrate surface and the epitaxial crystal domains flow to form an atomically smooth thin film. Through synchrotron X‐ray diffraction and high‐resolution scanning transmission electron microscopy, the formation of single‐grain Si 2 Te 3 , GeTe, GeSe, and GaTe thin films on (111) Si, Ge, and (100) GaAs is verified. The Si 2 Te 3 thin film is used to achieve transfer‐free fabrication of a high‐performance bipolar memristive electrical‐switching device.