We have modified synthetic protocols for the preparation of solvated Ln(III) tris-(bistrimethylsilyl)phosphide complexes to expand the [Ln{P(SiMe3)2}3(THF)2] series to Ln = La, Ce, Pr, Nd, Sm, Tm. The unexpected observation of resonances in the both the solution and solid-state complexes. We find diminishing agreement with experiment for calculated C, Si and 31 P pNMR chemical shifts as the distances between Ln(III) ions and ligands decrease across the 1-Ln series; this highlights the current limitations of these methods for nuclei where contact shift contributions dominate.