Figure : (a) 1 H-13 C correlation spectrum achieved by using the TEDOR experiment 45 at 30 kHz MAS, yielding two distinct correlations of the resonances (III/I) and (IV/II), shown in Fig. , which were subsequently used to model the paramagnetic shifts in the following section. The spinning sidebands are marked with asterisks ( * ). (b) 1 H NMR shift distributions considering solely the contributions arising from the presence of the unpaired electron and neglecting long-range PCS effects stemming from parametric centres in neighboring unit cells (δ p ). The shifts were calculated considering the Moon and Patchkovski, Vaara et al. and van den Heuvel and Soncini 26,27 formalism using the g tensor obtained using multireference perturbation theory (SO-CASPT2) on the DFT optimized geometry (see sections 1.8 and 5.3 of the SI for details) and the experimental 1 H hyperfine tensor. A distribution of relative orientations of the g and A tensors were considered using Zaremba, Conroy, Wolfsberg orientational averaging scheme with 1154 orientations. The relative orientation of the z axes of the g and A tensors was kept fixed at 45 • , in order to match with the EPR results.