Legrand et al. (Reports, 16 July 2010, p. 299) reported the experimental observation of square-planar and rectangular-bent geometries of 1,3-dimethylcyclobutadiene (Me(2)CBD) confined within a crystalline matrix. However, we found no evidence for the Me(2)CBD formation. We argue that the experimental x-ray density data are better attributed to the bicyclic β-lactone intermediate where carbon dioxide is covalently bound to cyclobutadiene.
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Alabugin et al. (2010) studied this question.
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