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The local magnetic structure in the [FeIII(Tp)(CN)3]− building block was investigated by combining paramagnetic Nuclear Magnetic Resonance (pNMR) spectroscopy and polarized neutron diffraction (PND) with first‐principle calculations. The use of the pNMR and PND experimental techniques revealed the extension of spin‐density from the metal to the ligands, as well as the different spin mechanisms that...
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