General. All manipulations were conducted under argon with the strict exclusion of oxygen and water by using Schlenk line and glove box techniques. [LnI3(THF)x] and KP(SiMe3)2 were synthesized according to literature procedures, and 1-Nd was prepared by modification of literature procedures. Diethyl ether and toluene were purged with nitrogen and passed through columns containing alumina catalyst and molecular sieves, and hexane was dried by refluxing over potassium; these solvents were degassed, refilled with argon and stored over a potassium mirror before use. For NMR spectroscopy, C6D6 was dried by refluxing over K, and (1-Ln) frames by ω rotation. Cell parameters were refined from the observed positions of all strong reflections in each data set. A Gaussian grid face-indexed was used to correct for X-ray absorption. The structures were solved using SHELXT; the datasets were refined by fullmatrix least-squares on all unique F 2 values, with anisotropic displacement parameters for all non-hydrogen atoms, and with constrained riding hydrogen geometries; Uiso(H) was set at 1.2