Guest-Adaptable Spin Crossover Properties in a Dinuclear Species Underpinned by Supramolecular Interactions

Molecular crystals with guest-adaptable crystalline structures and properties are comparatively rare owing to their inherent reduced structural stability and malleability to support molecular variation. To overcome this intrinsic challenge, here we introduce structural stabilizing supramolecular interactions into a dinuclear material and henceforth demonstrate a dynamic structural and spin crossover property interchange between solvated (A·3MeOH) and desolvated (A·O) products (A = [FeII2(o-NTrz)5(NCS)4]; 4-(o-nitrobenzyl)imino-1,2,4-triazole). Relatively uncommon for molecular species, the guest molecules in A·3MeOH are evolved (A·O) via a single-crystal to single-crystal transformation with affiliated phase transition resulting in a reversible transformation from one- to two-step spin crossover (SCO) transition character. We additionally present the water-saturated product (A·3H2O), which distinctly shows an abrupt one-step SCO character with a 22 K wide thermal hysteresis loop. Detailed structure–proper...