双二十面体Agn(n=19, 23, 24, 25)团簇低能稳态构型的TS搜索

doi:10.6023/A13050470

化学学报 ›› 2013, Vol. 71 ›› Issue (10): 1429-1434.DOI: 10.6023/A13050470 上一篇下一篇

研究论文

双二十面体Ag_n(n=19, 23, 24, 25)团簇低能稳态构型的TS搜索

蒋元祺, 彭平, 文大东, 韩绍昌

湖南大学材料科学与工程学院长沙 410082

投稿日期:2013-05-02 发布日期:2013-06-27
通讯作者: 彭平,E-mail:ppeng@hnu.edu.cn E-mail:ppeng@hnu.edu.cn
基金资助:
项目受国家自然科学基金(No. 51071065)和高等学校博士学科点专项科研基金(No. 20100161110001)资助.

A TS Search for Stable Configurations of Double Icosahedral Ag_n (n=19, 23, 24, 25) Clusters Linked by Sharing Atoms

Jiang Yuanqi, Peng Ping, Wen Dadong, Han Shaochang

School of Materials Science and Engineering, Hunan University, Changsha 410082

Received:2013-05-02 Published:2013-06-27
Supported by:
Project supported by the National Natural Science Foundation of China (Grant No. 51071065) and the Research Fund for the Doctoral Program of Higher Education of China (Grant No. 20100161110001).

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摘要/Abstract

采用基于NEB的MEP的LST/QST方法, 发展了一种不依赖团簇初始结构而得到其低能稳态构型的过渡态搜索方法, 预测和分析了孤立与铰链双二十面体Ag_n (n=13, 19, 23, 24, 25)的低能稳态构型. 证实Ag₁₃-I_h的低能稳态构型是一个含有五角双锥碎片的Ag₁₃-C₂扁平层状结构, 而Ag₁₉-D_5h的低能稳态构型则是在13原子二十面体上添加6原子组成Ag₁₉-C₁球形结构. 并且揭示Ag₂₃-D_3h, Ag₂₄-D_2h, Ag₂₅-D_5d与Ag_n (n=17～22)团簇一样, 其低能稳态构型也含有一个13原子的变形二十面体核心.

关键词: Ag_n团簇, 稳态构型, 过渡态搜索, DMol³

A DMol³ molecular orbital package based on DFT theory is adopted to calculate the energetics and electronic structures of icosahedral Ag₁₃ and double icosahedral Ag_n (n=19, 23, 24, 25) clusters. Ab initio MD simulation for Ag₁₃cluster at 300 K is also carried out in the micro-canonical ensemble (NVE). During optimization and total energy calculation, electronic exchange-correlation energy functions represented in reciprocal space with the PBE type under GGA approximation are used. A double-numerical basis set together with d-polarization functions (DNP) is chosen to describe the electronic wave functions of Ag atoms. And only core electrons described by the DFT Semi-core Pseudopots (DSPP) are calculated. All atomic positions in Ag_n (n=13, 19, 23, 24, 25) clusters are relaxed by geometry optimization under RMS force of 0.002 Ha/Å and RMS displacement of 0.005 Å. The calculation of total energy and electronic structure is followed by the geometry optimization with self-consistent field (SCF) tolerance of 1×10^-5 Ha. Further, using linear synchronous transit (LST) and quadratic synchronous transit (QST) methods based on the minimum energy path (MEP) with the aid of the climbing image nudged elastic band (NEB) method, a new transition state (TS) search technique for stable configurations of clusters is developed, in which the stable configuration is independent on selected initial configurations. As this technique being applied to search the stable configurations of Ag_n (n=7, 13, 19, 23, 25) clusters, it is confirmed the low energy stable configuration of the isolated icosahedron Ag₁₃-I_h is indeed a plate-shape layered structure Ag₁₃-C₂including a pentagonal bipyramid segment. The ground state of the double icosahedra linked with intercross sharing atoms Ag₁₉-D_5h is also demonstrated to be a spherical geometry Ag₁₉-C₁ consisting of 6 atoms around a deformed Ag₁₃icosahedron. And similarly to Ag_n (n=17～22) clusters, all stable configurations of Ag₂₃-D_3h, Ag₂₄-D_2h, Ag₂₅-D_5d clusters have a deformed Ag₁₃icosahedral nucleus as reported in literatures.

Key words: Ag_n cluster, stable configuration, TS search, DMol³

引用此文

蒋元祺, 彭平, 文大东, 韩绍昌. 双二十面体Ag_n(n=19, 23, 24, 25)团簇低能稳态构型的TS搜索[J]. 化学学报, 2013, 71(10): 1429-1434.

Jiang Yuanqi, Peng Ping, Wen Dadong, Han Shaochang. A TS Search for Stable Configurations of Double Icosahedral Ag_n (n=19, 23, 24, 25) Clusters Linked by Sharing Atoms[J]. Acta Chimica Sinica, 2013, 71(10): 1429-1434.

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双二十面体Ag_n(n=19, 23, 24, 25)团簇低能稳态构型的TS搜索

A TS Search for Stable Configurations of Double Icosahedral Ag_n (n=19, 23, 24, 25) Clusters Linked by Sharing Atoms

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双二十面体Agn(n=19, 23, 24, 25)团簇低能稳态构型的TS搜索

A TS Search for Stable Configurations of Double Icosahedral Agn (n=19, 23, 24, 25) Clusters Linked by Sharing Atoms

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双二十面体Ag_n(n=19, 23, 24, 25)团簇低能稳态构型的TS搜索

A TS Search for Stable Configurations of Double Icosahedral Ag_n (n=19, 23, 24, 25) Clusters Linked by Sharing Atoms