Probing the Structures, Stabilities and Electronic Properties of Neutral and Anionic PrSinλ (n=1-9, λ=0,-1) Clusters: Comparison with Pure Silicon Clusters

Silicon-based clusters have attracted particular attention because they are regard as building blocks for developing silicon-based nanomaterials. However, pure silicon clusters have low chemical stability owing to their dangling bonds. Doping with lanthanide atoms is a good way to form closed-shell of M@Si-n clusters and alter their electronic and magnetic properties. Here, we systematically study the lanthanide element Pr doped neutral and anionic silicon clusters by using density functional theory. Extensive searches for ground-state structures of Si-n+1(lambda) and PrSin lambda (n = 1-9, lambda = 0, - 1) clusters were carried out based on the comparison between experimental photoelectron spectroscopy and simulated spectra. Furthermore, the calculated AEA values of our obtained structures show good agreement with the experimental values. Based on averaged binding energies, fragmentation energies and HOMO-LUMO gaps, their relative stabilities were analyzed. Furthermore, the patterns of HOMOs for the most stable isomers were investigated to gain insight into the nature of bonding. The results show that some sigma-type and few pi-type bonds are formed among Si and Pr atoms. To achieve a insight into localization of charge and charge-transfer information, the Mulliken population are analyzed and discussed.

Automated summary

The study systematically investigates the lanthanide element Pr doped neutral and anionic silicon clusters using density functional theory, to alter the electronic and magnetic properties of the clusters. The results show that sigma-type and pi-type bonds are formed among the silicon and lanthanide atoms, providing insights into the nature of bonding. Additionally, the analysis of Mulliken population helps in understanding the localization of charge and charge-transfer information within the clusters.