Modern valence-bond theory, in its spin-coupled (SC) form, is used to investigate the nature of the bonding in the tetramer of methyllithium. In keeping with previous studies, the system is found to be predominantly ionic, in the sense (CH3–)4(Li+)4, but it exhibits some delocalisation of the methyl electron density back onto the lithium framework. The SC description of this molecule turns out to be remarkably simple.
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