In a first attempt to model the HYSCORE data of 1-Ce and 1-Nd, we used a simple point dipolar approach assuming the electron spin density to be located at the Ln 3+ ion, calculated (Supplementary Information Eqn 4) using the experimental g-values and the atomic coordinates from XRD (thus neglecting structural relaxation in solution). The calculated point dipolar hyperfine values for the Cp-ring hydrogen and carbon atoms (Tables and) were then used with EasySpin to calculate HYSCORE spectra. The calculated spectra show excellent agreement with the experimental data. (Figure ).