The first alkyl-amido tantalum(V) compounds having the composition Ta(NMe 2 ) 4 R (where R = Et, i Pr, t Bu, CH 2 SiMe 3 ) were reported by Chisholm et al. in 1982. 1 These monoalkyl derivatives were prepared from TaCl(NMe 2 ) 4 and the appropriate organolithium reagent. The molecular structure of the t Bu derivative revealed a square-pyramidal tantalum compound, and the alkyl group was situated at the apical site. More recently, Xue and co-workers have prepared the related silyl-substituted Ta-(NMe 2 ) 4 R derivatives (where R = SiMe 3 , Si t BuPh2), and the molecular structure of Ta(NMe 2 ) 4 (Si t BuPh2) was found to exhibit a trigonal-bipyramidal geometry with the silyl substituent residing at an equatorial site. 2 To our knowledge, Ta(NMe 2 ) 4 -( t Bu) and Ta(NMe 2 ) 4 (Si t BuPh2), whose structures are shown below, represent the only structurally characterized derivatives for this genre of compounds.Industrial demands for new, single-source tantalum compounds remain high. In particular, new tantalum compounds