To get a fuller appreciation of the effect of the magnetic anisotropy of 1-Ln, P and H MAS NMR spectra were recorded of the pure solids (Figure and Supporting Information Figures ). Unlike for the analogous Si MAS NMR of [Ln{Si(SiMe3)3}3(THF)2], the 31 P resonances from the metal-bound nuclear spins can be observed for all 1-Ln; this is owing to the much greater NMR receptivity of 31 P compared to Si (~180 times greater). For diamagnetic 1-La it is evident that on top of the spinning side band pattern that can be used to determine the CSA parameters (Table ), there are some underlying features (see Figure for the calculated fit). The J-coupling of the 31 P spins to 139 La (abundance = 99.95%;