Abstract: Two-dimensional conjugated polymers (2DCPs)─organic 2D materials composed of arrays of carbon sp2 centers connected by π-conjugated linkers─are attracting increasing attention due to their potential applications in device technologies. This interest stems from the ability of 2DCPs to host a range of correlated electronic and magnetic states (e.g., Mott insulators). Substitution of all carbon sp2 centers in 2DCPs by nitrogen or boron results in diamagnetic insulating states. Partial substitution of C sp2 centers by B or N atoms has not yet been considered for extended 2DCPs but has been extensively studied in the analogous neutral mixed-valence molecular systems. Here, we employ accurate first-principles calculations to predict the electronic and magnetic properties of a new class of hexagonally connected neutral mixed-valence 2DCPs in which every other C sp2 nodal center is substituted by either a N or B atom. We show that these neutral mixed-valence 2DCPs significantly energetically favor a state with emergent superexchange-mediated antiferromagnetic (AFM) interactions between C-based spin-1/2 centers on a triangular sublattice. These AFM interactions are surprisingly strong and comparable to those in the parent compounds of cuprate superconductors. The rigid and covalently linked symmetric triangular AFM lattice in these materials thus provides a highly promising and robust basis for 2D spin frustration. As such, extended mixed-valence 2DCPs are a highly attractive platform for the future bottom-up realization of a new class of all-organic quantum materials, which could host exotic correlated electronic states (e.g., unusual magnetic ordering, quantum spin liquids).
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