Four heterometallic formate frameworks templated by various alkylamine cations with the general formula [cat][GaMn(HCOO)] {cat is MA (CHNH) for 1, DMA [(CH)NH] for 2, EtA (CHCHNH) for 3, and DEtA [(CHCH)NH] for 4} have been prepared and characterized by X-ray diffraction, differential scanning calorimetry, and dielectric studies. All of the complexes have niccolite-like structures, which possess the same [GaMn(HCOO)] anionic framework with binodal (4·6)(4·6) topology; only the counterions in the cavity are different. Complex 4 undergoes a reversible ferroelastic phase transition around 220 K accompanied by a thermally switchable dielectric constant transition triggered by the freezing of the order-disorder DEtA cations.
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