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The on-off switching of spin-crossover (SCO) and single-molecule magnetism (SMM) remains highly attractive, especially if it involves dynamic crystal-to-crystal transformation. Herein we report the first molecule, a mononuclear cobalt(ii) complex, that exhibits on-off switching between SCO and SMM reversibly during crystal-to-crystal transformation. Subtle structural transformation triggered by a simple dehydration-rehydration process induces significant geometrical changes of the CoII center and modification of the supramolecular interactions and switches its colour and magnetic properties (dark red/SCO-on/SMM-off ↔ orange/SCO-off/SMM-on). This work suggests that modification of the weak supramolecular interactions could be very effective in achieving switchable materials involving both SCO and SMM properties.
Shao et al. (Mon,) studied this question.