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Spin crossover frameworks and molecular crystals display fascinatingcollective behaviours. This includes multi-step transitions with hysteresis anda wide variety of long-range ordered patterns of high-spin and low-spin metalcentres. From both practical and fundamental perspectives it is important tounderstand the mechanisms behind these collective behaviours. We study a simplemodel of elastic interactions and identify thirty six different spin-stateordered phases. We observe spin-state transitions with between one and eightsteps. These include both sharp transitions and crossovers, and both completeand incomplete spin crossover. We demonstrate structure-property relationshipsthat explain these differences. These arise because through-bond interactionsare antiferroelastic (favour metal centres with different spin-states);whereas, through-space interactions are typically ferroelastic (favour the samespin-state). In general, rigid materials with longer range elastic interactionslead to transitions with more steps and more diverse spin-state ordering, whichexplains why both are prominent in frameworks.

Structure-property relationships and the mechanisms of multistep transitions in spin crossover materials and frameworks