Two-dimensional conjugated
polymers (2DCPs)organic 2D materials
composed of arrays of carbon sp2 centers connected by π-conjugated
linkersare 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).