Calculation of NMR Shielding in Paramagnetic Molecules: Roadmap and Magnetic Couplings

Abstract

We present a simple derivation of the nuclear shielding in paramagnetic molecules, extendable to strong spin-orbit coupling cases of relevance to lanthanides and actinides, as well as encompassing contributions from excited multiplets. While our general formulation does not need electron paramagnetic resonance parameters, using them a simple and practical expression is obtained for the special case of the zero-field-split ground-state manifold, including magnetic (Zeeman and hyperfine) couplings between the sublevels. The latter method is implemented computationally and applied in the context of first-principles calculations on example Ni(II) and Co(II) complexes.