Nearly Flat Conduction Bands from Bond-Centered Orbital Networks in Dense C<sub>3</sub>N<sub>4</sub>.

Chen, JianJia; Liao, Yujie; He, Chaoyu; Zhong, Jianxin; Tang, Chao · Nano Lett · 2026

basic_science · Level V

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Abstract

Nearly flat electronic bands are highly sought after for emergent quantum phenomena yet remain difficult to realize in three-dimensional covalent materials. Here we show that such bands can arise in dense C<sub>3</sub>N<sub>4</sub> through bond-centered orbital networks. A systematic crystal-structure search identifies 110 previously unknown C<sub>3</sub>N<sub>4</sub> frameworks, including two low-energy phases that are dynamically stable and exhibit weakly dispersive band-edge states. In particular, the 176-10-56-0 phase hosts an ultraflat conduction band on the <i>k</i><sub><i>z</i></sub> = 0 plane with an in-plane bandwidth of only 4 meV, located just 0.06 eV above the true conduction-band minimum. Real-space analysis and effective bond-centered lattices reveal a connectivity-controlled mechanism for dispersion suppression. Moreover, very small strains can directly tune this low-lying flat band into the true conduction-band minimum while preserving weak dispersion, enhancing its experimental relevance. Our results establish bonding topology as a promising route to flat-band engineering in light-element covalent frameworks beyond conventional interference-based scenarios.