Wafer-Scale Growth of 2D PtTe₂ with Layer Orientation Tunable High Electrical Conductivity and Superior...

Platinum ditelluride (PtTe₂) is an emerging semimetallic two-dimensional (2D) transition-metal dichalcogenide (TMDC) crystal with intriguing band structures and unusual topological properties. Despite much devoted efforts, scalable and controllable synthesis of large-area 2D PtTe₂ with well-defined layer orientation has not been established, leaving its projected structure-property relationship largely unclarified. Herein, we report a scalable low-temperature growth of 2D PtTe₂ layers on an area greater than a few square centimeters by reacting Pt thin films of controlled thickness with vaporized tellurium at 400 °C. We systematically investigated their thickness-dependent 2D layer orientation as well as its correlated electrical conductivity and surface property. We unveil that 2D PtTe₂ layers undergo three distinct growth mode transitions, i.e., horizontally aligned holey layers, continuous layer-by-layer lateral growth, and horizontal-to-vertical layer transition. This growth transition is a consequence of competing thermodynamic and kinetic factors dictated by accumulating internal strain, analogous to the transition of Frank-van der Merwe (FM) to Stranski-Krastanov (SK) growth in epitaxial thin-film models. The exclusive role of the strain on dictating 2D layer orientation has been quantitatively verified by the transmission electron microscopy (TEM) strain mapping analysis. These centimeter-scale 2D PtTe₂ layers exhibit layer orientation tunable metallic transports yielding the highest value of ∼1.7 × 10⁶ S/m at a certain critical thickness, supported by a combined verification of density functional theory (DFT) and electrical measurements. Moreover, they show intrinsically high hydrophobicity manifested by the water contact angle (WCA) value up to ∼117°, which is the highest among all reported 2D TMDCs of comparable dimensions and geometries. Accordingly, this study confirms the high material quality of these emerging large-area 2D PtTe₂ layers, projecting vast opportunities employing their tunable layer morphology and semimetallic properties from investigations of novel quantum phenomena to applications in electrocatalysis.