【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.更多还原

【Abstract】 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 C₅₁-C₅₉ 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 C₅₁-C₅₉ 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 C₅₄Rh have substitutional networked structures formed by replacing the two-fold coordinated carbon atom in C₅₅ 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.更多还原