Abstract
Polynuclear molecules with large-spin state and high anisotropy are discrete entities situated at the frontier between quantum and classical systems. These well defined complexes displaying uniform shape, magnetic moment and anisotropy can behave as single-molecule magnets. Following a bottom-up approach of nanomaterials, we present a rational synthetic route of such molecules based on hexacyanometalates [M(CN)6]3−cores. Thus, were built and fully characterised (mass spectroscopy, crystallographic structure, magnetic susceptibility, …) polynuclear species such as [M(CNM'L)6]9± or [M(CN)4(CNM'L)2]± (with M= CrIII, CoIII, FeIII; M′= NiII,CoII,CuII,…; L =polydentate ligand) showing large ground spin states.