THE GEOMETRIC AND ELECTRONIC-STRUCTURES OF AR-N(+) (N=3-27)
THE GEOMETRIC AND ELECTRONIC-STRUCTURES OF AR-N(+) (N=3-27)
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DOI：
10.1063/1.464130
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发表时间：
1993-02-15
影响因子：
4.4
通讯作者：
IWATA, S
中科院分区：
文献类型：
--
作者：
IKEGAMI, T;KONDOW, T;IWATA, S
用双原子分子哈密顿量的解析梯度法确定了Ar(N)+最稳定的结构，n=3-27。对振子强度分布进行了估算。发现电荷集中在中心的三个原子上，这三个原子形成了三聚离子核。第一个溶剂化壳层围绕离子核心演化，在n=25时完成。计算表明，光吸收带位于可见光区，该吸收带起源于Ar3+离子核的2SIGMA(U)+-->；2SIGMA(G)+跃迁，并随着团簇尺寸的增大而红移，再现了实验结果。红移可以用溶剂化离子核模型来解释，在该模型中，离子核的激发态与周围的溶剂原子发生强烈的相互作用。
The most stable structures of Ar(n)+, n = 3-27, are determined with the analytical gradient method for the diatomics-in-molecules Hamiltonian. The oscillator strength distribution is evaluated. The charge is found to be localized on the central three atoms, which form the trimeric ion core. The first solvation shell evolves around the ion core and is completed at n=25. The calculation shows that the photoabsorption band is in the visible region, which originates from the 2SIGMA(u)+ --> 2SIGMA(g)+ transition of the Ar3+ ion core, and is red-shifted with the increase of the cluster size, reproducing the experimental results. The red-shift is explained in terms of the solvated ion core model, in which the excited state of the ion core interacts strongly with the surrounding solvent atoms.