Unconventional Band Structure via Combined Molecular Orbital and Lattice Symmetries in a Surface‐Confined Metallated Graphdiyne Sheet

• DOI: 10.1002/adma.202405178
• Publication Date: 2024-05-19T12:10:17Z
• Authors: Ignacio Piquero‐Z...; Wenqi Hu; Ari Paavo Seitsonen; Felix Haag; Johannes Küchle; Francesco Allegretti; Yuanhao Lyu; Lan Chen; Kehui Wu; Zakaria M. Abd El...; Ethem Aktürk; Svetlana Klyatskaya; Mario Ruben; Matthias Muntwiler; Johannes V. Barth; Yi‐Qi Zhang
• Keywords: Graphyne; Bilayer graphene

Graphyne (GY) and graphdiyne (GDY)-based monolayers represent the next generation 2D carbon-rich materials with tunable structures properties surpassing those of graphene. However, detection band formation in atomically thin GY/GDY analogues has been challenging, as both long-range order atomic precision have to be fulfilled system. The present work reports direct evidence on-surface synthesized metallated Ag-GDY sheets mesoscopic (≈1 µm) regularity. Employing scanning tunneling angle-resolved photoemission spectroscopies, energy-dependent transitions real-space electronic states above Fermi level valence are respectively observed. Furthermore, density functional theory (DFT) calculations corroborate observations reveal that doubly degenerate frontier molecular orbitals on a honeycomb lattice give rise flat, Dirac Kagome bands close level. DFT modeling also indicates an intrinsic gap for pristine sheet material, which is retained bilayer h-BN, whereas adsorption-induced in-gap evolve at synthesis platform decorating (111) facet silver. These results illustrate tremendous potential engineering novel via orbital symmetries precise carbon materials.