First-principles study of the electronic structure and optical properties of two-dimensional $α$-graphdiyne

Abstract

The structural, electronic, and optical properties of monolayer $α$-graphdiyne ($α$-GDY) are systematically investigated using density-functional theory within the plane-wave pseudopotential formalism. The electronic band structure reveals a gapless Dirac crossing at the K point, demonstrating the Dirac semimetallic character of the monolayer. The calculated total and orbital-projected density of states show that the electronic states near the Fermi level are dominated by the carbon $2p$ orbitals, while the contribution of the $2s$ orbitals is comparatively weak. The optical response exhibits pronounced polarization dependence. The in-plane dielectric function displays a strong Drude-like response and negative values of the real dielectric function at low photon energies, whereas the out-of-plane component remains positive throughout the investigated energy range. Consistently, the absorption coefficient, extinction coefficient, reflectivity, and electron energy-loss spectra reveal a pronounced optical anisotropy. The calculated plasma frequencies are approximately $3.21$~eV for the in-plane polarization and $1.06$~eV for the out-of-plane polarization, indicating substantially stronger collective electronic excitations within the atomic plane. These findings demonstrate that $α$-GDY combines Dirac-like electronic behavior with highly anisotropic optical properties, highlighting its potential for polarization-sensitive optoelectronic, plasmonic, and nanoelectronic applications.