Abstract
In the pursuit of high-spin building blocks for the formation of covalently bonded 1D or 2D materials with controlled magnetic interactions, π -electron magnetism offers an ideal framework to engineer ferromagnetic interactions between nanographenes. As a first step in this direction, we explore the spin properties of ferromagnetically coupled triangulenes-triangular nanographenes with spin S = 1 . By combining in-solution synthesis of rationally designed molecular precursors with on-surface synthesis, we successfully achieve covalently bonded S = 2 triangulene dimers and S = 3 trimers on Au(111). Starting with the triangulene dimer, we meticulously characterize its low-energy magnetic excitations using inelastic electron tunneling spectroscopy (IETS). IETS reveals conductance steps corresponding to a quintet-to-triplet excitation, and a zero-bias peak resulting from higher-order spin-spin scattering of the five-fold degenerate ferromagnetic ground state. The Heisenberg model captures the key parameters of inter-triangulene ferromagnetic exchange, and its successful extension to the larger S = 3 system validates the model's accuracy. We anticipate that incorporating ferromagnetically coupled building blocks into the repertoire of magnetic nanographenes will unlock new possibilities for designing carbon nanomaterials with complex magnetic ground states.