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A comprehensive study of the magnetocaloric effect (MCE) in the Mn2‐[Nb(CN)8] molecular magnet with a two‐step magnetic sponge behavior is reported. The structural transformations provoked by dehydration bring about an increase in the magnetic ordering temperature (Tc) from 43 K through to 68 K and up to 98 K. All three phases are soft isotropic ferrimagnets. The change in magnetic entropy in the...
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