Silva M X, Silva F T, Galvão B R L, Braga J P, Belchior J C
Departamento de Química-ICEx, Universidade Federal de Minas Gerais, Av. Antônio Carlos 6627, Pampulha, 31.270-901, Belo Horizonte, MG, Brazil.
Departamento de Química Fundamental-CCEN, Universidade Federal de Pernambuco, Av. Jornalista Anibal Fernandes, Cidade Universitária, 50.740-560, Recife, Pernambuco, Brazil.
J Mol Model. 2018 Jul 7;24(8):196. doi: 10.1007/s00894-018-3724-6.
The DFT potential energy hypersurfaces of closed-shell nitrogen clusters up to ten atoms are explored via a genetic algorithm (GA). An atom-atom distance threshold parameter, controlled by the user, and an "operator manager" were added to the standard evolutionary procedure. Both B3LYP and PBE exchange-correlation functionals with 6-31G basis set were explored using the GA. Further evaluation of the structures generated were performed through reoptimization and vibrational analysis within MP2 and CCSD(T) levels employing larger correlation consistent basis set. The binding energies of all stable structures found are calculated and compared, as well as their energies relative to the dissociation into N, [Formula: see text] and [Formula: see text] molecules. With the present approach, we confirmed some previously reported polynitrogen structures and predicted the stability of new ones. We can also conclude that the energy surface profile clearly depends on the calculation method employed.
通过遗传算法（GA）探索了多达十个原子的闭壳层氮簇的密度泛函理论（DFT）势能超曲面。在标准进化过程中添加了一个由用户控制的原子 - 原子距离阈值参数和一个“算子管理器”。使用GA探索了具有6 - 31G基组的B3LYP和PBE交换相关泛函。通过在MP2和CCSD(T)水平上使用更大的相关一致基组进行重新优化和振动分析，对生成的结构进行了进一步评估。计算并比较了所有发现的稳定结构的结合能，以及它们相对于分解为N、[公式：见原文]和[公式：见原文]分子的能量。采用本方法，我们证实了一些先前报道的多氮结构，并预测了新结构的稳定性。我们还可以得出结论，能量表面轮廓明显取决于所采用的计算方法。
