Structural growth pattern of neutral and negatively charged yttrium-doped silicon clusters YSi_n^0/− (n=6–20): from linked to encapsulated structures

Abstract

A global search for the low energy of neutral and anionic doped Si clusters YSi n 0/À (n ¼ 6-20) was performed using the ABCluster global search technique coupled with a hybrid density functional method (mPW2PLYP). In light of the calculated energies and the measured photoelectron spectroscopy values, the true minima of the most stable structures were confirmed. It is shown that the structural growth pattern of YSi n À (n ¼ 6-20) is from Y-linked two subcluster structure to a Yencapsulated structure in Si cages, while that of YSi n (n ¼ 6-20) is from substitutional to linked structures, and as the number of Si atoms increases, it evolves toward the encapsulated structure.Superatom YSi 20 À with a high-symmetry endohedral I h structure has an ideal thermodynamic stability and chemical reactivity, making it the most suitable building block for novel optical, optoelectronic photosensitive or catalytic nanomaterials.

Global optimization of chemical cluster structures: Methods, applications, and challenges

“…Yang et al used ABCluster to study metal‐doped silicon clusters ( q = 0, − 1, n ≤ 20, M = Sc, Y, Ti, Zr, and some lanthanides) [91, 116, 208–220]. The computed photoelectron spectroscopies using GMs agree well with experimental ones.…”

Structural stability and evolution of terbium‐doped silicon clusters and influence of 4f → 5d electronic transition mechanism on magnetism and appearance of photoelectron spectroscopy for TbSin0/− (n = 6‐18) clusters

“…For example, the ground state structures of M@Si 16 (M = transition metal atom including RE metal atom) tend to be fullerene‐like configuration when radii of M are larger than 2.09 Å, but to be Frank‐Kasper (FK) motif when radii of M atom are less than or equal to 2.09 Å. That is, M@Si 16 for M = Y, La‐Lu, Zr, and Hf is fullerene‐like configuration, and that for M = Sc, Ti, and Ta is FK geometry …”

“…Most studies have focused on the formation of terbium silicides and have demonstrated that nanoclusters and/or nanowires may play an important role in this physical and chemical process. Correspondingly, nanoclusters have become one of the core issues in the field of nanotechnology owing to their extraordinary structures and properties . On the other hand, the miniaturization of subnano devices could make the cluster assembly change electronic properties by changing shape, size, and composition, but it needs a comprehensive understanding of the interaction between RE atoms and silicon clusters.…”

“…Correspondingly, nanoclusters have become one of the core issues in the field of nanotechnology owing to their extraordinary structures and properties. [7][8][9][10][11] On the other hand, the miniaturization of subnano devices could make the cluster assembly change electronic properties by changing shape, size, and composition, but it needs a comprehensive understanding of the interaction between RE atoms and silicon clusters. Thus, it is of great significance to figure out the relationship between the structural evolution and properties of terbium silicide nanoclusters during the transition from molecular to condensed phase.…”

The Artificial Bee Colony Algorithm for Global Optimization of Nanosized Clusters

“…One example is that ABCluster was used to search the GMs of lanthanide (Ln) doped silicon cluster anions as large as LnSi 20 − , and the calculated photoelectron spectroscopy from these GMs agree well with the experimental ones. [21][22][23][24][25][26][27][28][29][30] Another example is that several authors searched the GMs of clusters consisting of atmosphere related molecules like water, ammonia, nitric acid, hydroxymethanesulfonic acid, sulfuric anhydride, and pentoxide−iodic acid. [31][32][33][34][35][36][37][38][39][40][41][42][43] Using GMs of different sizes, atmospheric cluster dynamics equations can be solved 44 and a lot of atmospheric chemical phenomena were successfully explained.…”