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Calculations and geometry optimizations have been carried out using the DFT formalism with the B3LYP exchange-correlation functional. All-electron valence double-ζ basis sets (D95V) were used to describe C, O, and H atoms. Full double-ζ (D95) bases were used, supplemented with one and two d-type polarization functions for N and S, respectively. The valence shell of Ni was described at the double-ζ level, and the Ne core was modeled with the Los Alamos core potential. The antiferromagnetic low-spin state of 3′ has been characterized using the broken-symmetry approach within the framework of the Heisenberg Hamiltonian, defined as Ĥ, 2J ABŜA·ŜB. We used the approximate projection proposed by Yamaguchi et al.16 More details can be found in ref 9
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