We note that in none of the cases are the pNMR shifts of the coordinated SiM atoms correctly predicted for paramagnetic 1-Ln, and that the choice of structural model has a significant effect on the calculated values (see Supporting Information Tables ). This indicates substantial influence of the contact spin density based on structural models that we cannot capture with these simplified static models and minimal CASSCF-SO calculations. For paramagnetic 1-Ln, only one non-metal-bound Si resonance is observed, again likely a result of dynamic averaging.