Tunable Flat Bands and magnetism in Triangulene-based Superatomic Graphene

Abstract

Superatomic graphene platforms host a rich portfolio of flat-band-driven exotic quantum properties, yet their experimental realization remains challenging. Here, we report the bottom-up on-surface synthesis of superatomic graphene using phosphorus-doped triangulene as building blocks. Scanning tunneling microscopy and spectroscopy measurements resolve the well-defined honeycomb lattice of as-fabricated superatomic graphene and demonstrate the characteristic Dirac band and flat band electronic structures. Density functional theory calculations reveal that the flat bands originate from the in-plane p$_x,_y$-like frontier orbitals of the phosphorus-doped triangulene units, leading to intrinsic half-metallic behavior. Furthermore, oxygen functionalization of the molecular precursor enables deterministic modulation of the electronic structure and magnetic ordering. This work establishes a general platform for designing correlated quantum materials with tunable flat band properties.