de Sousa David Wilian Oliveira, Nascimento Marco Antonio Chaer
Instituto de Química, Universidade Federal do Rio de Janeiro Cidade Universitária , CT Bloco A Sala 412, Rio de Janeiro, RJ 21941-909, Brazil.
J Chem Theory Comput. 2016 May 10;12(5):2234-41. doi: 10.1021/acs.jctc.6b00055. Epub 2016 Apr 13.
The chemical structure of the ground state of C2 has been the subject of intense debate after the suggestion that the molecule could exhibit a "fourth" covalent bond. In this paper, we investigate this problem explicitly avoiding all the points of conflict from the previous papers to show that there is no quadruple bond in C2. The generalized product function energy partitioning (GPF-EP) method has been applied to calculate the interference energy (IE) that accounts for the formation of covalent bonds for each bond of the molecule. The IE analysis shows that for the standard σ and π bonds interference exhibits the expected behavior, while for the "fourth" bond interference is a destabilizing factor. To make sure this could not be attributed to a new kind of bond, we performed an equivalent analysis for the (3)Σ(-) excited state of C3 molecule in which similar "bonding" occurs between the two ending carbon atoms. We also show that the difference in force constants of C2 and acetylene can be rationalized in terms of the amount of charge density in the internuclear region by looking at the changes in the overlaps between orbitals along the bond axis.
在有人提出C₂分子可能存在“第四个”共价键之后,C₂基态的化学结构一直是激烈争论的主题。在本文中,我们明确研究了这个问题,避开了以往论文中所有存在争议的点,以表明C₂中不存在四重键。广义乘积函数能量划分(GPF-EP)方法已被用于计算干涉能(IE),该干涉能解释了分子中每个键的共价键形成情况。IE分析表明,对于标准的σ键和π键,干涉表现出预期的行为,而对于“第四个”键,干涉是一个使分子不稳定的因素。为确保这不能归因于一种新型键,我们对C₃分子的(3)Σ⁻激发态进行了等效分析,在该激发态中,两个末端碳原子之间发生了类似的“键合”。我们还表明,通过观察沿键轴轨道重叠的变化,C₂和乙炔力常数的差异可以根据核间区域的电荷密度量来解释。