Mind the gap: A complete, cooperative spin transition for a mononuclear MnIII complex is reported with an 8 K hysteresis window. Raman spectra collected at a single temperature in warming and cooling modes confirm the electronic bistability within the hysteresis loop. The source of the cooperativity is a disconnection in the hydrogen-bonded 1D chains that connect adjacent cations owing to an order–disorder transition in the PF6− counterion.
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