CAJ | 학술논문

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.
용유전산법(GA)화밀도범함이론(DFT)상결합적방법,대실험중소관찰도적기수고탄단족(C51～C59)급상관적함Rh부륵희단족적결구진행료계산. 수선이용유전산법대기수고탄단족C51～C59적결구진행수색,조출기최저능량결구,연후재차기출상이용B3LYP/3-21G방법대상응적기수고탄단족결구진행재우화. 이용유전산법득도료비이보도적능량경저적기수고탄단족C51～C59적기태결구. 계산소득적기수고탄단족구유준롱상류부륵희결구,기최저능량이구체도함유일개량배위적탄원자. 재금속부륵희C54Rh적결구중,Rh원자취대C55상량배위적탄원자이형성취대형류부륵희결구. 대기수고탄단족급함Rh부륵희단족적결합능화결구삼수진행료계산,환토론료기수고탄단족이구체적결구수능량적변화.
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.