Off-Plane Dielectric Screening of Few-Layer Graphdiyne and Its Family

We performed first-principles calculations on few-layer graphdiyne (GDY) and its family, sp-sp(2) hybrid carbon atomic layers, for an off-plane, static dielectric screening. The vertical dielectric constants of semiconducting GDY structures are finite and independent of the thickness. However, unlike the widely accepted wisdom that the static metallic screening is infinite, those of metallic GDY structures are finite and dependent on their thickness. Furthermore, the vertical dielectric screening can be tuned by varying the interlayer distance. We also studied the dielectric properties of heterostructures of GDY/its family; the vertical dielectric constant has an equivalent value from the two distinct values of the two distinct monostructures. The dielectric screening behaviors are well described by the uniform dielectric slab model. In addition, the band gaps can be widely tuned from 0 to 0.8 eV, by varying the thickness and electric field. Our results provide a method for engineering the dielectric constant and band gap of GDY and its family for applications of supercapacitors and nanodevices.