In Chapter 1, a series of "constrained geometry" organoactinide complexes, (CGC)An(NMe)2 (CGC = Me2Si(h5-Me4C5)(tBuN); An = Th, 1; U, 2), prepared via efficient in situ, two-step protodeamination routes in good yields and high purity, is presented. Both 1 and 2 are quantitatively converted to the neutrally charged, solvent-free dihalides (1-Cl2,...