Observation of the Magnetic Ground State of the Two Smallest Triangular Nanographenes

[Image: see text] Fusion of three benzene rings in a triangular fashion gives rise to the smallest open-shell graphene fragment, the phenalenyl radical, whose π-extension leads to an entire family of non-Kekulé triangular nanographenes with high-spin ground states. Here, we report the first synthesis of unsubstituted phenalenyl on a Au(111) surface, which is achieved by combining in-solution synthesis of the hydro-precursor and on-surface activation by atomic manipulation, using the tip of a scanning tunneling microscope. Single-molecule structural and electronic characterizations confirm its open-shell S = 1/2 ground state that gives rise to Kondo screening on the Au(111) surface. In addition, we compare the phenalenyl’s electronic properties with those of triangulene, the second homologue in the series, whose S = 1 ground state induces an underscreened Kondo effect. Our results set a new lower size limit in the on-surface synthesis of magnetic nanographenes that can serve as building blocks for the realization of new exotic quantum phases of matter.