Urquhart Stephen G, Gillies Rob
Department of Chemistry, 110 Science Place, Saskatoon, Saskatchewan S7N 5C9, Canada.
J Phys Chem A. 2005 Mar 17;109(10):2151-9. doi: 10.1021/jp045370e.
We have acquired high-resolution carbon 1s near-edge X-ray absorption fine structure (NEXAFS) spectra of methane, ethane, propane, isobutane, and neopentane. These experimental measurements are complemented by high-quality ab initio calculations, performed with the improved virtual orbital approximation. The degree and character of Rydberg-valence mixing in the preedge of the NEXAFS spectra of these species is explored. Significant Rydberg-valence mixing only occurs when there are excited states of valence sigma(C-H) character that have the appropriate symmetry to interact with excited states of Rydberg character. Our results show that this mixing is only present when there are C-H bonds to the core excited carbon atom.
我们已经获得了甲烷、乙烷、丙烷、异丁烷和新戊烷的高分辨率碳1s近边X射线吸收精细结构(NEXAFS)光谱。这些实验测量结果得到了采用改进的虚拟轨道近似进行的高质量从头算计算的补充。研究了这些物质的NEXAFS光谱预边中里德堡-价态混合的程度和特征。只有当存在具有适当对称性以与里德堡特征的激发态相互作用的价σ(C-H)特征的激发态时,才会发生显著的里德堡-价态混合。我们的结果表明,只有当与核心激发碳原子存在C-H键时,这种混合才会出现。