Intrinsic Grain Boundary Structure and Enhanced Defect States in Air‐Sensitive Polycrystalline 1T’‐WTe2 Monolayer

Abstract

AbstractMonolayer WTe2 has attracted significant attention for its unconventional superconductivity and topological edge states. However, its air sensitivity poses challenges for studying intrinsic defect structures. This study addresses this issue using a custom‐built inert gas interconnected system, and investigate the intrinsic grain boundary (GB) structures of monolayer polycrystalline 1T’ WTe2 grown by nucleation‐controlled chemical vapor deposition (CVD) method. These findings reveal that GBs in this system are predominantly governed by W‐Te rhombi with saturated coordination, resulting in three specific GB prototypes without dislocation cores. The GBs exhibit anisotropic orientations influenced by kinks formed from these fundamental units, which in turn affect the distribution of grains in various shapes within polycrystalline flakes. Scanning tunneling microscopy/spectroscopy (STM/S) analysis further reveals metallic states along the intrinsic 120° twin grain boundary (TGB), consistent with computed band structures. This systematic exploration of GBs in air‐sensitive 1T’ WTe2 monolayers provides valuable insights into emerging GB‐related phenomena.