Structure and magnetic properties of icosahedral Pd(x)Ag(13−x) (x = 0–13) clusters

In this article, we present a modified Velocity-Verlet algorithm that makes cluster system converge rapidly and accurately. By combining it with molecular dynamics simulations, we develop an effective global sampling method for extracting isomers of bimetallic clusters. Using this method, we obtain the isomers of icosahedral Pd(x)Ag(13−x) (x = 0–13). Additionally, using the first-principle spin-polarized density functional theory approach, we find that each isomer still retains its icosahedral structure because of strong s-d orbital hybridization, and the cluster is more stable when a Pd atom is at the center of the cluster. With increasing x value, the magnetic moment decreases linearly from 5.0 μB at x = 0, until reaching zero at x = 5, and then increases linearly up to 8.0 μB at x = 13. By calculating the atom-projected density of states (PDOS), we reveal that the magnetic moment of Pd(x)Ag(13−x) mainly originates from s electrons of Ag when 0 ≤ x < 5, and d electrons of Pd when 5 < x ≤ 13. The PDOS results also show that the Pd(x)Ag(13−x) tends to transform from a semiconductor state to semi-metallic state when x gradually increases from 0 to 13.