This work was divided in two parts dedicated to (i) the development of KC60 salts and the characterization of their physical properties; and (ii) the study and the analysis of the magnetic properties of Prussian Blue-like phases. Our goal was to bring experimental and theoretical answers to the contradictory results published on these two subjects. A particular effort was dedicated to the control of the conditions of KC60 synthesis which enabled us to control the nature of the fundamental state. This study in addition highlighted the important role of argon atoms insertion on the electronic properties of these compounds. With regard to the Prussian Blue-like phases, we showed that the magnetic order observed at low temperature is ferrimagnetic and this magnetic phase has an original magnetic anisotropy induced in these materials by the Mo(CN)7 4- unit.
