N-heterocyclic carbenes are an important class of molecules that have wide applications in chemical catalysis. Several widely employed organometallic catalytic complexes have a carbene bound to a transition metal. The description of carbene and transition metal chemistry using theoretical/computational methods is difficult due to the complicated electronic structure of these molecules due to the multiconfigurational nature of transition metals and carbenes. Multiconfiguration pair-density functional theory (MC-PDFT) is a low-cost and accurate method that has been shown to produce accurate results for small- and medium-sized chemical systems exhibiting strong multiconfiguration correlation energy. The central goal of this work is to develop the computational parameters needed for MC-PDFT to obtain highly accurate bond dissociation energies for a series of NHC first-row transition metal compounds. Key computational parameters include determining the choice of the on-top pair density functional and the identification of an appropriate set of active space orbitals that reasonably describe the bond-breaking process. The accuracy of the computed results is evaluated by comparison to high-level computations.

Accurate determination of bond dissociation energies of N-heterocyclic transition metal compounds using MC-PDFT

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