奇数类富勒烯团簇结构的遗传算法和密度泛函理论研究(英文)  

Structures of Odd-Numbered Pseudo-Fullerene Clusters: Genetic Algorithm and Density Functional Studies

作　　者：李郁芬[1] 庄军[1] 孔庆宇[2] 沈义峰[3] 徐炯[1] 赵利[4] 孙志华[1] 蔡瑞芳[5] 

机构地区：[1]复旦大学光科学与工程系,上海200433 [2]复旦大学激光化学研究所,上海200433 [3]复旦大学物理系,上海200433 [4]复旦大学先进光子材料与器件国家重点实验室,上海200433 [5]复旦大学化学系,上海200433

出　　处：《复旦学报（自然科学版）》2003年第6期833-842,共10页Journal of Fudan University：Natural Science

基　　金：ProjectssupportedbytheNationalNaturalScienceFoundationofChina(No .10 0 0 4 0 0 2 ;2 9890 2 16 ;and2 0 2 710 30 )andtheTechnologyDevelopmentFoundationofShanghai(No .0 2QA14 0 0 7)

摘　　要：用遗传算法(GA)和密度泛函理论(DFT)相结合的方法,对实验中所观察到的奇数高碳团簇(C51～C59)及相关的含Rh富勒烯团簇的结构进行了计算.首先利用遗传算法对奇数高碳团簇C51～C59的结构进行搜索,找出其最低能量结构,然后在此基础上利用B3LYP/3 21G方法对相应的奇数高碳团簇结构进行再优化.利用遗传算法得到了比已报道的能量更低的奇数高碳团簇C51～C59的基态结构.计算所得的奇数高碳团簇具有准笼状类富勒烯结构,其最低能量异构体都含有一个两配位的碳原子.在金属富勒烯C54Rh的结构中,Rh原子取代C55上两配位的碳原子而形成取代型类富勒烯结构.对奇数高碳团簇及含Rh富勒烯团簇的结合能和结构参数进行了计算,还讨论了奇数高碳团簇异构体的结构随能量的变化.Using a combination of genetic algorithm(GA) and density functional theory (DFT) approach, the structures of the odd-numbered all-carbon and rhodium-containing high carbon clusters observed in mass spectrometric experiments were studied. The structures of the lower energy isomers of the odd-numbered clusters C_(51)-C_(59) found by GA global searching were re-optimized with DFT at the B3LYP/3-21G level. In GA calculation all the minimal energy isomers of the odd-numbered all-carbon clusters C_(51)-C_(59) have energies lower than those previously reported. The lowest energy isomers of the odd-numbered clusters are cage-like pseudo-fullerenes containing a single two-fold coordinated carbon atom in addition to trivalent carbon atoms. The Rh-containing odd-numbered high carbon clusters C_(54)Rh have substitutional networked structures formed by replacing the two-fold coordinated carbon atom in C_(55) by the Rh atom. The binding energies and the structural parameters are reported. To the isomers of the odd-numbered carbon clusters, the structure change with the energy is discussed.

关 键 词：团簇 富勒烯 金属富勒烯 奇数高碳团簇 几何结构 遗传算法 密度泛函理论 

分 类 号：O613.71[理学—无机化学]