The paramagnetic contributions to the experimental isotropic pNMR shifts of 1-Ce, 1-Pr, 1-Nd and 1-Sm were approximated by subtracting the shifts of the diamagnetic complex 1-La (see Table and Experimental Section for details and Supporting Information Tables ). To calculate the paramagnetic shifts, a variety of methods have been employed. Firstly, the common approach of assuming the nuclei are all in the long-range limit compared to the well-localized magnetic moment of the paramagnetic ion has been considered, and hence we employ the point-dipolar model for calculating pseudocontact shift. In the general case of low-symmetry structures, this takes the form: