Topology as a Design Variable for Multiproperty Engineering in Synthesized 4-5-6-8 Carbon Nanoribbons

Abstract

Nonbenzenoid carbon frameworks expand low-dimensional material design via controlled asymmetry. Here, we show the experimentally realized 4-5-6-8 carbon nanoribbon establishes a topology-driven paradigm for multiproperty engineering, not just a graphene variant. Using hybrid DFT, tight-binding, and molecular dynamics in a multiscale framework, we demonstrate the symmetry-broken lattice stabilizes hierarchical bonds within standard energy ranges. This geometry produces a robust semiconducting state (hybrid gap >1 eV) and enables strain as a controllable modulation parameter. A tight-binding Hamiltonian fitted only at equilibrium accurately captures strain-dependent band evolution, proving the essential physics is topology-dominated. Mechanical analysis reveals high stiffness with fracture governed by the largest polygons, showing asymmetry redistributes stress without compromising integrity. Intrinsic phonon scattering suppresses thermal conductance, enabling favorable thermoelectric performance without extrinsic disorder. Optical response confirms non-equivalent ring connectivity reorganizes interband transitions, promoting strong visible absorption and efficient photocarrier generation. These results position topology as a governing parameter coupling elasticity, electronics, thermal transport, and optics, establishing the 4-5-6-8 nanoribbon as a unified platform for predictive design of multifunctional carbon materials.