One-dimensional solid-state MAS NMR spectra of 1 H, C and Si are shown in Figure . Each of these spectra exhibits poorly resolved patterns, due to hyperfine interactions with the unpaired electron, which induce large shifts and shift anisotropies and extremely large inhomogeneous line-broadenings. We see shift anisotropies that are very large for all three nuclei, of the order of hundreds of ppm, in contrast to the Lu analogue, where the 1 H and 13 C diamagnetic chemical shift anisotropies (CSAs) were too small to be measured and for Si were of the order of tens of ppm. In particular, for the Lu analogue, Si CSAs were used to characterize the metal-ligand interaction. That approach is not at first sight obviously applicable to the paramagnetic Yb complex, since the interpretation of the shift anisotropy is more complex. C MAS spectra of at 14.286 kHz MAS and (c) Si MAS spectra at 30 kHz MAS, showing two distinct Si signals. The spinning sidebands are marked with asterisks ( * ). 2D aMAT spectrum: (d) 1 H at 30 kHz, (e) C at 20 kHz and (f) Si at 20 kHz. The indirect dimension projections were deconvolved using asymmetric Gaussian functions to extract the isotropic shifts and quantify shift dispersion. (g)-(i) extracted slices with isotropic shift corresponding to the maxima of the deconvolved projections and labelled with Roman numerals. Each slice was subsequently fitted considering a simple CSA model using the Haeberlen convention 43 (δ iso = 1 3 ( δxx + δyy + δzz ), ∆δ = δzz -δ iso and η = ( δyyδxx )/∆δ, where δ xx , δ xx and are the components of the CSA tensor in the principal axes frame). See SI chapter 1.6 for more details.