Ni(II) is . A square-planar complex can keep its strongly antibonding in-plane orbital empty and has a paired, configuration. A tetrahedral arrangement has two unpaired electrons, .
The important change here is the substituent on the imine nitrogen: Me, Et, then tert-butyl. The phenolic ortho-tert-butyl substituent is common to all three ligands. The small N-Me groups permit coplanar NO coordination in . N-tert-butyl crowds that arrangement and favors twisting the two chelate planes toward a distorted tetrahedron in . N-Et gives a closer energetic competition, so accesses both structures. The observed equilibrium reflects ligand-field stabilization, pairing, steric strain and temperature-dependent entropy; it is not a change in nickel oxidation state.