Chemical susceptibility of fullerenes in view of Hartree–Fock approach
Chemical susceptibility of fullerenes in view of Hartree–Fock approach
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Hartree-Fock 方法的富勒烯化学敏感性
DOI：
10.1002/qua.21358
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发表时间：
2007
期刊：
影响因子：
--
通讯作者：
E. Sheka
中科院分区：
文献类型：
--
作者：
E. Sheka
构成从共价键中除去的富勒烯奇电子的一部分（Int J Quantum Chem，2004，100，375），有效的未成对电子由不受限制的Hartree-Fock SCF溶液的单线态不稳定性构成。该功能发生是一个特别重要的导致原子匹配的奇电子分子物种的化学敏感性通过原子上的相关电子密度的定量描述。UHF解能很好地提供有效未成对电子总数ND及其分密度NDA的正确测定。对一组双原子分子和乙烯的计算过程和所得结果的可靠性是合理的。NDA值和独立计算的自由价在X60（X = C，Si）和C70分子的原子上的分布的实际上完全相同使得可以将NDA图视为富勒烯的化学画像。NDA值是原子化学活性的定量指标，因此突出了对任何类型的加成反应最有利的目标。基于NDA的计算合成的富勒烯衍生物的基本理由说明C60的初始步骤。© 2007 Wiley Periodicals，Inc.国际量子化学杂志，2007年
Constituting a part of fullerenes odd electrons which are removed from the covalent bonding (Int J Quantum Chem, 2004, 100, 375), effectively unpaired electrons are posed by the singlet instability of the unrestricted Hartree–Fock SCF solution. The feature occurs to be of a particular importance leading to a quantitative description of atomically matched chemical susceptibility of the odd-electron molecular species via the relevant electron density on atoms. A correct determination of the total number of effectively unpaired electrons ND and its partial density NDA is well provided by the UHF solution. The calculation procedure and the obtained results reliability are justified for a set of diatomic molecules and ethylene. Practically full identity of the distribution of both NDA values and independently calculated free valence over atoms of X60 (X = C, Si) and C70 molecules makes it possible to consider the NDA maps as chemical portraits of the fullerenes. The NDA value is offered to be a quantitative pointer of the atom chemical activity thus highlighting targets, which are the most favorable for addition reactions of any type. Basic grounds for a NDA-based computational synthesis of the fullerene derivatives are illustrated for initial steps of C60 fluorination. © 2007 Wiley Periodicals, Inc. Int J Quantum Chem, 2007