Realization of Two‐Dimensional Intrinsic Polar Metal in a Buckled Honeycomb Binary Lattice

Abstract Structural topology and symmetry of a two‐dimensional (2D) network play pivotal roles in defining its electrical properties and functionalities. Here, a binary buckled honeycomb lattice with C 3v symmetry, which naturally hosts topological Dirac fermions and out‐of‐plane polarity, is proposed. It is successfully achieved in a group IV‐V compound, namely monolayer SiP epitaxially grown on Ag(111) surface. Combining first‐principles calculations with angle‐resolved photoemission spectroscopy, the degeneration of the Dirac nodal lines to points due to the broken horizonal mirror symmetry is elucidated. More interesting, the SiP monolayer manifests metallic nature, which is mutually exclusive with polarity in conventional materials. It is further found that the out‐of‐plane polarity is strongly suppressed by the metallic substrate. This study not only represents a breakthrough of realizing intrinsic polarity in 2D metallic material via ingenious design but also provides a comprehensive understanding of the intricate interplay of many exotic low‐dimensional quantum phenomena.