Formation of .eta.1-iminoacyl compounds by insertion of isonitriles into pentamethylcyclopentadienyl-tetramethylfulvene compounds of titanium and zirconium. Intramolecular C-H activation of a pentamethylcyclopentadienyl group to give a tridentate ligand with two bridged cyclopentadienyl rings and a titanium-vinyl bond in the bridge. Molecular structure of [cyclic][.eta.5:.eta.1:.eta.5-C5Me4CH2C(NHXyl):CN(Xyl)CH2C5Me4]TiCl and [cyclic]Cp*[.eta.5:.eta.1-C5Me4CH2C(:NXyl)C(:NXyl)]ZrCl (Xyl=2,6-Me2C6H3)

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