Specifically, solid-state NMR with fast MAS and broadband adiabatic irradiation sequences can now be used to obtain data on microcrystalline powders, where the complex dynamics are simplified and only the relevant internal ligand motions are retained. Nonetheless, obtaining high-quality magnetic resonance data on these systems represents only part of the challenge, since the resulting spectra are often very difficult to interpret using standard assignment methods. In this respect, recent progress in wave-function based/DFT methods for the computation of NMR parameters of paramagnetic complexes has also been impressive. For NMR, there have been significant advances both in the development of the formalism of the paramagnetic shifts and the computational implementation. However, applying the developed methods to lanthanides has been a much more difficult matter.