Metal-organic framework (MOF) thin films have recently attracted much attention as a new platform for surface/interface research, where unconventional structural and physical properties emerge. Among the many MOFs as candidates for fabrication of thin films, Hofmann-type MOFs {Fe(pz)[M(CN)]} [pz = pyrazine; M = Ni (), M = Pt ()] are attractive, because they undergo spin transitions with concomitant structural changes. Here, we demonstrate the first example of a strain-controlled spin transition in heterostructured MOF thin films. The spin transition temperature of can be controlled in the temperature range of 300-380 K by fabricating a nanometer-sized heterostructured thin film with a buffer layer, where the smaller lattice of causes epitaxial compressive strain to the layer. The fabricated heterostructured thin film exhibited a remarkable increase in spin transition temperature with a dynamic structural transformation, confirmed by variable-temperature (VT) X-ray diffraction and VT Raman spectroscopy. By verifying interfacial strain in a heterostructured thin film, we can rationally control the characteristics of MOFs-not only spin transition but also various physical properties such as gas storage, catalysis, sensing, proton conductivity, and electrical properties, among others.
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