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The NDI units are \u201cdirectionally flexible\u201d in concert with the pivoting motion of the ferrocene unit with a small rotational barrier. The NDI units rotate around the ferrocene unit faster than the NMR time scale in solution at room temperature. UV\u2013vis absorption, synchrotron X-ray diffraction, and atomic force microscope studies reveal that NDI\u2013Fc\u2013NDI forms a fibrous supramolecular assembly in solution (methylcyclohexane and highly concentrated chloroform) and film states, wherein the NDI units are in the slipped-stack conformation. The NDI\u2013Fc\u2013NDI supramolecular assembly in the film state exhibits multiple phase transitions associated with conformational changes at different temperatures, which are confirmed by differential scanning calorimetry, polarized optical microscopy, and temperature-dependent X-ray diffraction. Such thermal transitions of NDI\u2013Fc\u2013NDI films also induce changes in the optical and electronic properties as revealed by UV\u2013vis absorption and photoelectron yield spectroscopies, respectively. The thermal behaviors of NDI\u2013Fc\u2013NDI, realized by the unique molecular design, are considerably different from the reference compounds such as an NDI dimer connected with a flexible 1,4-butylene linker. These results provide us with a plausible strategy to propagate the molecular dynamics of the \u03c0-system into macroscopic properties in film states; the key factors are (i) the supramolecular alignment of molecular switching units and (ii) the directional motion of the switching units perpendicular to the supramolecular axis.<\/jats:p>","DOI":"10.1021\/jacs.6b05824","type":"journal-article","created":{"date-parts":[[2016,8,26]],"date-time":"2016-08-26T16:28:42Z","timestamp":1472228922000},"page":"11245-11253","source":"Crossref","is-referenced-by-count":32,"title":["Supramolecular\nAssemblies of Ferrocene-Hinged Naphthalene\u00addiimides:\nMultiple Conformational Changes in Film States"],"prefix":"10.1021","volume":"138","author":[{"given":"Atsuro","family":"Takai","sequence":"first","affiliation":[{"name":"National Institute for Materials Science (NIMS) , , 1-2-1 Sengen , Tsukuba , Ibaraki 305-0047 ,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takashi","family":"Kajitani","sequence":"additional","affiliation":[{"name":"Tokyo Institute of Technology , , 4259 Nagatsuta , Midori-ku , Yokohama 226-8503 ,","place":["Japan"]},{"name":"RIKEN SPring-8 Center, 1-1-1 Kouto, Sayo, Hyogo679-5148, Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takanori","family":"Fukushima","sequence":"additional","affiliation":[{"name":"Tokyo Institute of Technology , , 4259 Nagatsuta , Midori-ku , Yokohama 226-8503 ,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Keiki","family":"Kishikawa","sequence":"additional","affiliation":[{"name":"Chiba University , , 1-33 Yayoi-cho , Inage-ku , Chiba 263-8522 ,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Takeshi","family":"Yasuda","sequence":"additional","affiliation":[{"name":"National Institute for Materials Science (NIMS) , , 1-2-1 Sengen , Tsukuba , Ibaraki 305-0047 ,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Masayuki","family":"Takeuchi","sequence":"additional","affiliation":[{"name":"National Institute for Materials Science (NIMS) , , 1-2-1 Sengen , Tsukuba , Ibaraki 305-0047 ,","place":["Japan"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2016,8,26]]},"reference":[{"key":"2026081802293928800_cit1a","volume-title":"Molecular Devices and\nMachines","author":"Balzani","year":"2003"},{"key":"2026081802293928800_cit1b","first-page":"295","volume-title":"Functional Organic\nMaterials: Syntheses, Strategies and Applications","author":"Saha","year":"2007"},{"key":"2026081802293928800_cit1c","volume-title":"From Non-Covalent\nAssemblies to Molecular Machines","author":"Sauvage","year":"2011"},{"key":"2026081802293928800_cit1d","doi-asserted-by":"crossref","DOI":"10.1002\/9781118680469","volume-title":"Intelligent Stimuli-Responsive\nMaterials: From Well-Defined Nanostructures to Applications","author":"Li","year":"2013"},{"key":"2026081802293928800_cit1e","doi-asserted-by":"crossref","DOI":"10.1007\/978-3-319-08678-1","volume-title":"Molecular Machines and Motors:\nRecent Advances and Perspectives Preface","author":"Credi","year":"2014"},{"key":"2026081802293928800_cit1f","doi-asserted-by":"publisher","first-page":"1281","DOI":"10.1021\/cr0300993","volume":"105","author":"Kottas","year":"2005","journal-title":"Chem. 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