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Four nickel(II) salpn (salicylidenepropylene iminate) complexes are investigated concerning their capability to perform CISSS (coordination‐induced spin‐state switching). To this end, pyridine titration experiments are performed with the nickel salpn complexes [Ni(salpn)], [Ni(salpntBuCF3)], [Ni(salpnCF3)] and [Ni(salpnSbenz)]. The electronic‐structural changes are monitored by UV/Vis spectroscopy...