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Topological defects in graphene materials introduce exotic properties whichare absent in their defect-free counterparts with both fundamental importanceand technological implications. Although individual topological defects havebeen widely studied, collective magnetic behaviors originating fromwell-organized multiple topological defects remain a great challenge. Here, westudied the collective magnetic properties originating from three pentagontopological defects in truxene-based molecular graphenoids by using scanningtunneling microscopy and non-contact atomic force microscopy. Unpaired $\pi$electrons are introduced into the aromatic topology of truxene moleculargraphenoids one by one by dissociating hydrogen atoms at the pentagon defectsvia atom manipulation. Scanning tunneling spectroscopy measurements togetherwith density functional theory calculations suggest that the unpaired electronsare ferromagnetically coupled, forming a collective high-spin quartet state ofS=3/2. Our work demonstrates that the collective spin ordering can be realizedthrough engineering regular patterned topological defects in moleculargraphenoids, providing a new platform for designer one-dimensionalferromagnetic spin chains and two-dimensional ferromagnetic networks.

Topological Defects Induced High-Spin Quartet State in Truxene-Based Molecular Graphenoids