Development of spintronic and quantum computing devices increases demand for efficient, energy saving method of spin manipulation at molecular scale. Polyoxovanadate molecular magnets being susceptible to both electric and magnetic fields may serve here as a good base material. In this paper, two isostructural anions $[{\mathrm{V}}_{12}{\mathrm{As}}_8{\mathrm{O}}_{40}$(${\mathrm{HCO}}_2{\left)\right]}^{n-}$ (with $n=3,5$) featuring two different mixed-valence states with itinerant and localized valence electrons are studied. The impact of the electric field on their magnetic properties is investigated by means of two complementary methods informed by magnetic measurements: effective Hamiltonian calculations and density functional theory. It is demonstrated that the magnetoelectric effect in theses molecules is induced mostly by relocation of itinerant electrons, is highly anisotropic, depends on the valence state and can be detected even at room temperature. These findings can pave the way to practical applications in which an electric field control over spin state is required.

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• Exchange interaction
• Magnetic susceptibility
• Magnetoelectric effect
• Molecular magnetism