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The current craze for research around the spin crossover phenomenon can be justified to some extent by the mechanical properties due to the decrease of volume associated with the transition of the metal ion from the HS state to the LS state. As demonstrated here, the molecular complex [Fe(PM‐pBrA)2(NCS)2] exhibits, on the contrary, an increase of the unit‐cell volume from HS to LS. This counter‐intuitive...
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