Silver cluster doped graphyne (GY) with outstanding non-linear optical properties

This research study addresses the computational simulations of optical and nonlinear optical (NLO) characteristics of silver (Ag) cluster doped graphyne (GY) complexes. By precisely following DFT and TD-DFT hypothetical computations, in-depth characterization of GY@Ag_center, GY@Ag_side, GY@2Ag_{perpendicular}, GY@2Ag_above, and GY@3Ag_center is accomplished using CAM-B3LYP/LANL2DZ while the CAM-B3LYP/mixed basis set is used for study of 2GY@Ag_center, 2GY@Ag_side, 2GY@2Ag_{perpendicular}, 2GY@2Ag_above, and 2GY@3Ag_center. The effects of various graphyne surface based complexes on hyperpolarizabilities, frontier molecular orbitals (FMOs), density of states (DOS), absorption maximum (λ_max), binding energy (E_b), dipole moment (μ), electron density distribution map (EDDM), transition density matrix (TDM), electrostatic potential (ESP), vertical ionization energy (E_VI) and electrical conductivity (σ) have been investigated. Infrared (IR), non-covalent interaction (NCI) analysis accompanied by isosurface are performed to study the vibrational frequencies and type of interaction. Doping strategies in all complexes impressively reformed charge transfer characteristics such as narrowing band gap (E_g) in the range of 2.58–4.73 eV and enhanced λ_max lying in the range of 368–536 nm as compared to pure GY with 5.78 eV E_g and 265 nm λ_max for (GY@Ag_center–GY@3Ag_center). In the case of (2GY@Ag_center–2GY@3Ag_center), when compared to 2GY with 5.58 eV E_g and 275 nm absorption, maximum doping techniques have more effectively modified λ_max in the region of 400–548 nm and E_g, which is in the order of 2.55–4.62 eV. GY@3Ag_center and 2GY@3Ag_center reflected a noteworthy increment in linear polarizability α_O (436.90 au) and (586 au) and the first hyperpolarizability β_O (5048.77 au) and (17 270 au) because of their lowest excitation energy (ΔE) when studied in comparison with GY (α_O = 281.54 and β_O = 0.21 au) and 2GY surface (α_O = 416 and β_O = 0.06 au). Focusing on harmony between the tiny Ag clusters and graphyne surface as well as their influences on NLO properties, graphyne doping using its two-unit cells (2GY) is found to be expedient for the development of future nanoscale devices.

This research study addresses the computational simulations of optical and nonlinear optical (NLO) characteristics of silver (Ag) cluster doped graphyne complexes.