摘要
在UBP86/LANL2DZ和UBP86/def2-TZVP水平下详细研究了AumNin(m+n≤6)团簇的几何结构和电子性质.详细地分析了团簇的结构特征,平均结合能,垂直电离势,垂直电子亲和能,电荷转移以及成键特征.所有混合团簇中,镍原子趋于聚集到一起,形成最多Ni—Ni键,金原子分布在镍原子聚集体周围以形成最多Au—Ni键.Ni原子较少团簇的电子性质与纯金团簇类似,呈现一定奇偶振荡.混合团簇中存在镍到金原子间的电荷转移.Ni原子较少团簇中,自旋电子主要定域在Ni原子上,Ni原子较多团簇中,Au原子明显受到自旋极化.混合团簇的分波态密度表明,AuNi混合团簇对小分子的反应活性要高于纯金团簇.
The structural and electronic properties of small AumNin （m ＋n≤6） clusters have been studied at the UBP86/LANL2DZ and UBP86/def2-TZVP levels, respectively. Structural features, binding energies, vertical ionization potentials, vertical electron affinity, charge transfers, and binding characters were evaluated for each Au-Ni binary cluster. In all of the Au-Ni binary clusters, the nickel atoms are brought together, yielding the most Ni-Ni bonds, and the gold atoms are located around a Ni core with the most Au- Ni bonds. The vertical ionization potentials, vertical electron affinity, and Fermi level of the Au-rich clusters are similar to the pure gold clusters, demonstrating an odd-even oscillation. A very large electronic charge transfer from Ni to Au was found in the binary clusters. The spin density is located on Ni atoms in the Au-rich clusters, while the gold atoms are spin-polarized in the Ni-rich clusters. The partial density of state of the Au-Ni binary clusters makes it clear that the reactivity of the Au-Ni binary clusters toward the small molecule is higher than that of the pure gold clusters.
出处
《化学学报》
SCIE
CAS
CSCD
北大核心
2009年第14期1539-1546,共8页
Acta Chimica Sinica
基金
四川省自然科学基金(No.2008JY0119)
四川教育厅(No.07ZA158)资助项目
关键词
金镍混合团簇
垂直电离能
垂直电子亲和能
态密度(DOS)
密度泛函理论
gold-nickel cluster
vertical ionization potential
vertical electron affinity
density of state（DOS）
density functional theory
