Synthesis. We started with the Ni derivative, 1-Ni, utilizing a two-step one-pot reaction (Scheme 1). The reaction of Ni(COD)2 (COD=1,5-cyclooctadiene) in pentane with an excess allylchloride affords {Ni(h 3 -allyl)Cl}2 in situ. Further reaction with Li(DIA)(thf) yields the desired product in 91% yield as an orange-red microcrystalline solid after sublimation (10 -3 mbar, 45 °C) -see experimental section for more details. The 1 H NMR spectrum of 1-Ni in C6D6 (Figure ) shows a triplet of triplets at 4.84 ppm for the central proton of the allyl, a heptet at 3.12 ppm for the central proton on the amidinate iso-propyl group, doublets at 2.88 ppm and 1.66 ppm and for the terminal protons on the allyl ligand that are syn and anti to the central C-H bond, respectively, a singlet at 1.39 ppm for the CH3 group bound to the quaternary carbon, and two doublets at 1.04 ppm and 0.84 ppm for the diastereotopic terminal protons on the iso-propyl group. The observed signals are consistent with 1-Ni being diamagnetic and adopting a pseudo-square planar geometry.