Enhanced Interfacial Properties of Metal–Bilayer TMD Heterostructures

High contact resistance at metal/semiconductor interfaces remains a critical bottleneck in realizing high‐performance devices based on 2D transition metal dichalcogenides (TMDs), primarily due to large Schottky barrier heights (SBH). In this work, we employ first‐principles calculations to systematically investigate the interfacial properties of various metals (Au, Ag, Pd, Ti, Pt) in contact with van der Waals (vdW) bilayer TMD heterostructures, specifically ‐ and ‐. Our results reveal a substantial reduction in SBHs in TMD heterostructures compared to the monolayers due to significant bandgap narrowing. Notably, Ti and Ag contacts yield nearly ohmic behavior with negligible SBHs, attributed to weaker orbital overlap and reduced Fermi‐level pinning, while Pd and Pt induce stronger metallization and higher SBHs. These findings demonstrate that vdW bilayer TMD heterostructures, when paired with suitable metal contacts, provide a promising route to minimize contact resistance, thereby advancing the design of efficient optoelectronic devices.