We study the electronic and structural properties of substitutional impurities of graphenelike nanoporous materials C$_2$N, $tg$-, and $hg$-C$_3$N$_4$ by means of density functional theory calculations. We consider four types of impurities; boron substitution on carbon sites (B(C)), carbon substitution on nitrogen sites (C(N)), nitrogen substitution on carbon sites (N(C)), and sulfur substitution on nitrogen sites (S(N)). From cohesive energy calculations, we find that the C(N) and B(C) substitutions are the most energetically favorable and induce small bond modifications in the vicinity of the impurity, while the S(N) induces strong lattice distortions. Though all of the studied impurities induce defect levels inside the band gap of these materials, their electronic properties are poles apart depending on the behavior of the impurity as an acceptor or a donor. It is also observed that acceptor (donor) wavefunctions are composed only of $sigma$ ($pi$) orbitals from the impurity itself and/or neighboring sites. Consequently, acceptor wavefunctions are directed towards the pores and donor wavefunctions are more extended throughout the neighboring atoms, a property that could further be explored to modify the interaction between these materials and adsorbates. Moreover, impurity properties display a strong site sensitivity and ground state binding energies ranging from $0.03$ to $1.13$ eV, thus offering an interesting route for tuning the optical properties of these materials. Finally, spin-polarized calculations reveal that all impurity configurations have a magnetic ground state that rises from the spin splitting of the impurity levels. In a few configurations, more than one impurity level can be found inside the gap and two of them could potentially be explored as two-level systems for single-photon emission, following similar proposals recently made on defect complexes on TMDCs.
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