The ability to engineer geometrically well-defined antidots in large triangulene homologues
allows for creating an entire family of triangulene quantum ring (TQR) structures with tunable high-spin
ground state and magnetic ordering, crucial for next-generation molecular spintronic devices. Herein, we
report the synthesis of an open-shell [7]triangulene quantum ring ([7]TQR) molecule on Au(111) through
the surface-assisted cyclodehydrogenation of a rationally-designed kekulene derivative. Bond-resolved
scanning tunneling microscopy (BR-STM) unambiguously imaged the molecular backbone of a single
[7]TQR with a triangular zigzag edge topology, which can be viewed as [7]triangulene decorated with a
coronene-like antidot in the molecular centre. Additionally, dI/dV mapping reveals that both inner and
outer zigzag edges contribute to the edge-localized and spin-polarized electronic states of [7]TQR. Both
experimental results and spin-polarized density functional theory calculations indicate that [7]TQR
retains its open-shell septuple ground-state (� = 3) on Au(111). This work demonstrates a new route for
the design of high-spin graphene quantum rings as the key components for future quantum devices.
Description of high-spin restricted open-shell molecules with the Piris natural orbital functional