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The singlet wave function is quite complicated having 62% contribution of the closed shell configuration and 11% from double excitations in the active space, 2% contribution from the configuration with four open shells and still 2% contribution from the quadruple excitation within the active space. Thus, the first-order interacting space of this calculation included up to hextuple excitations relative to the closed shell configuration, which shows that a multireference treatment is hardly avoidable in predicting the ground-state properties of such complicated spin-coupled molecules from correlated ab initio methods. The only state with a simple configurational structure is the quintet state. The population analysis of the correlated density shows indeed 1.8 unpaired electrons on the nickel center and two unpaired electrons delocalized over the ligands, which is in support of the DFT results.
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