Structures, Stabilities, and Electronic Properties of Small-Sized Zr₂Si _n (n=1–11) Clusters: A Density Functional Study

Abstract

Ab initio methods based on density functional theory at B3LYP level have been applied in investigating the equilibrium geometries, growth patterns, relative stabilities, and electronic properties of Zr 2 -doped Si n clusters. The optimisation results shown that the lowest-energy configurations for Zr 2 Si n clusters do not keep the corresponding silicon framework unchanged, which reflects that the doped Zr atoms dramatically affect the most stable structures of the Si n clusters. By analysing the relative stabilities, it is found that the doping of zirconium atoms reduces the chemical stabilities of silicon host. The Zr 2 Si 4 and Zr 2 Si 7 clusters are the magic numbers. The natural population and natural electronic configuration analyses indicated that the Zr atoms possess positive charge for n = 1-6 and negative charge for n = 7-11. In addition, the chemical hardness, chemical potential, infrared, and Raman spectra are also discussed.

Study on Structural Evolution, Thermochemistry and Electron Affinity of Neutral, Mono- and Di-Anionic Zirconium-Doped Silicon Clusters ZrSin0/-/2- (n = 6–16)

“…Wu et al studied the bond distances, vibrational frequencies, adiabatic electron affinities (AEAs), ionization potential, and dissociation energies of TMSi (TM = 3d, 4d, 5d elements) and their charged ions by using the B3LYP scheme [19]. Furthermore, the geometries and electronic properties of Zr 2 -doped silicon clusters were reported [20,21]. On the experimental aspect, Koyasu et al investigated the equilibrium configurations, electronic structures, and properties of MSi n (M = Zr, Sc, Y, Lu, Ti, Hf, V, Nb, and Ta, n = 6–20) by means of anion photoelectron spectroscopy (PES) and their reactivity to H 2 O adsorption, presented their AEAs and vertical detachment energies (VDEs), and discussed the cooperative effect between their geometric and electronic structures [22,23].…”