A second method, intended to overcome the limitations of the first method and achieve a better agreement with experimental chemical shifts, is one where we can implicitly account for the non-pointdipolar nature of the spin system (i.e. the spatial delocalization of 4f spin density) and the spin density at the nuclei of interest (i.e. including the contact contribution): here, we employ the van den Heuvel and Soncini method in the Hyperion program. Using the existing CASSCF-SO calculations from