000863686 001__ 863686 000863686 005__ 20210130002256.0 000863686 0247_ $$2doi$$a10.1021/acs.cgd.9b00298 000863686 0247_ $$2ISSN$$a1528-7483 000863686 0247_ $$2ISSN$$a1528-7505 000863686 0247_ $$2altmetric$$aaltmetric:63336179 000863686 0247_ $$2WOS$$aWOS:000480499600036 000863686 037__ $$aFZJ-2019-03692 000863686 082__ $$a540 000863686 1001_ $$0P:(DE-HGF)0$$aRok, Magdalena$$b0$$eCorresponding author 000863686 245__ $$aScreening ferroelastic transitions in switchable cyano-bridged perovskites: [CH3C(NH2)2]2[KM(CN)6], M = Cr3+, Fe3+, Co3+. Crystal structure characterisation, dielectric properties, 1H NMR and quasielastic neutron scattering studies. 000863686 260__ $$aWashington, DC$$bACS Publ.$$c2019 000863686 3367_ $$2DRIVER$$aarticle 000863686 3367_ $$2DataCite$$aOutput Types/Journal article 000863686 3367_ $$0PUB:(DE-HGF)16$$2PUB:(DE-HGF)$$aJournal Article$$bjournal$$mjournal$$s1568029731_22203 000863686 3367_ $$2BibTeX$$aARTICLE 000863686 3367_ $$2ORCID$$aJOURNAL_ARTICLE 000863686 3367_ $$00$$2EndNote$$aJournal Article 000863686 520__ $$aHere we report the dynamics of organic cations as guest molecules in the novel perovskite host framework. The novel switchable crystals from the coordination family [CH3C(NH2)2]2[KB″(CN)6] were constructed by employing acetamidinium cations (ACE = [CH3C(NH2)2]) as A-site and B″: Cr3+, Fe3+, Co3+ in the inorganic cage. The molecular motion of ACE+ as well as the effect of the trivalent metallic cation type on two-step transitions were studied using a combination of experimental methods: (i) X-ray diffraction experiments, (ii) thermal analysis, (iii) dielectric and electric studies, (iv) optical observations, (v) 1H NMR spectroscopy, and (vi) quasielastic neutron scattering (QENS). On the basis of the X-ray analysis, transitions occur from a frozen-order phase (III, monoclinic, C2/m) to an in-plane rotational disorder state (II, trigonal, R3̅m) and to a melt-like disorder one (I, cubic, Fm3̅m). A markedly temperature-dependent dielectric constant indicates the tunable and switchable properties of all complexes. The QENS, as well as 1H NMR spectroscopy, were applied to measure the dynamics of the organic cations residing in the inorganic framework. The ferroelastic nature of the phases III and II were proven based on the polarized light microscopy photographs. 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