Abstract 1,6‐Methano[10]annulene‐Cr(CO) 3 and several related complexes adopt an anomalous orientation of the Cr(CO) 3 unit with respect to the polyene, compared to all other hexatriene‐Cr(CO) 3 complexes. A theoretical analysis of this problem shows that these conformational preferences are closely related to the cycloheptatriene‐norcaradiene valence tautomerism. Several strategies for influencing the barrier to internal rotation in these complexes are presented. An analysis of the conformational preference, rotational barrier, and bending of the exocyclic methylene group in fulvene‐Cr(CO) 3 is also discussed. This is extended to the analogous benzyl‐Cr(CO) 3 and cyclobutadiene‐carbinyl‐Fe(CO) 3 cations. Finally, the orientations of these complexes are contrasted to those containing two more electrons.
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Albright et al. (1978) studied this question.
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