Evolution of the electronic structure and properties of neutral and charged arsenic clusters
Evolution of the electronic structure and properties of neutral and charged arsenic clusters
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DOI：
10.1007/s10853-007-1928-8
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发表时间：
2007-11-01
影响因子：
4.5
通讯作者：
Guo, Ling
中科院分区：
文献类型：
--
作者：
Guo, Ling
用B3LYP的密度泛函方法研究了As-n （n = 2-15）中性、阳离子和阴离子的几何和电子性质。在6-311 + G(d)的基础上对中性离子和带电离子进行了Berny结构优化和频率分析。然后用这些团簇的总能量来研究它们的结合能、相对稳定性和电子性质随尺寸的变化。当团簇包含四个原子时，发现几何形状经历了从二维到三维的结构变化。几何变化伴随着最近邻距离和配位数的相应变化。在整个尺寸范围内，电离势和电子亲和都有随团簇中As数量增加而减小的趋势。星团的稳定性在几个幻数的作用下表现出很强的奇偶交替。中性As (n)团簇为偶数，在n = 2和4处有局部最大值，而阳离子和阴离子团簇优先为奇数，其中As-3（+）、As-5（+）和As-5（-）是最稳定的离子。
Geometrical and electronic properties of As-n (n = 2-15) neutrals, cations and anions have been investigated using the density functional method of B3LYP. Berny structural optimization and frequency analyses are performed with the basis of 6-311 + G(d) for both neutrals and charged ions. The total energies of these clusters are then used to study the evolution of their binding energy, relative stability, and electronic properties as a function of size. The geometries are found to undergo a structural change from two dimensional to three-dimensional when the cluster contains four atoms. The geometrical changes are companied by corresponding changes in the nearest-neighbor distances and coordination numbers. In the whole size range, both ionization potential and electron affinity have the tendency of decrease when the number of As units in the cluster increases. The stability of clusters exhibits strong even-odd alternations with several magic numbers. The neutral As (n) clusters are found to be even-numbered with local maxima at n = 2 and 4, while the cationic and anionic clusters are preferentially odd-numbered with As-3(+), As-5(+) and As-5(-) being the most stable ions according to the calculated results of the both energy gain and electronic properties.