N_4O_n(n=3～5)团簇结构与分解机理的理论研究

Theoretical research on the structures and decomposition mechanism of N_4O_n(n=3～5) clusters

采用密度泛函理论在B3LYP/6-31G*水平上对N4On(n=3～4)团簇异构体的结构进行优化,得到了5种N4O3、5种N4O4,在能量方面探讨了其作为高能密度材料的可能性。采用3种密度泛函理论(DFT)方法 B3LYP、BB1K、MPWB1K和6-31G*基组,找到了5个N4On(n=3～5)团簇(N4O3中的A3、A4,N4O4中的B3、B4,N4O5中的Z8)分解反应的过渡态,并探讨了它们的分解反应机理;B3LYP方法的能垒明显比另两种方法低很多;BB1K和MPWB1K方法能垒很接近,结果比B3LYP方法可靠,是计算过渡态的较好方法。

We optimized possible geometrical structures of N4On（n=3～4） clusters at the B3LYP/6-31G＊ level and obtained five isomers of N4O3 and N4O4.We also addressed the possibility of N4On（n=3～4） clusters,high energy density materials.We further discovered five transitional states of the dissociation reaction of N4O3（A3,A4）,N4O4（B3,B4） and N4O5（Z8） clusters with functoinals B3LYP,BB1K and MPWB1K and the basis set 6-31G＊ and analyzed their composition mechanism.Energy barrier of functional B3LYP is much lower than that of the other two functionals.Energy barriers of functionals BB1K and MPWB1K are similar to each other and are more reliable than that of functional B3LYP.Therefore,functionals BB1K and MPWB1K are two better methods to calculate the transitional state.