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Herein, multicolor emission is governed by tailoring the geometries of \u03c0\u2013\u03c0 dimers. Using perylene (PE) as a planar \u03c0\u2010fluorophore, we strategically design a compound, 3\u2010(4\u2010(1,2,2\u2010triphenylvinyl)phenyl)perylene (pTPE\u2010PE), which integrates a tetraphenyl ethylene (TPE) substituent with multiple rotatable phenyl rings to modulate the PE\u2010based \u03c0\u2013\u03c0 dimer formation. On the one hand, pTPE\u2010PE crystallization produces four polymorphs exhibiting green, yellow, orange, and red emission color, which are static presentations of the dimer model. This static multicolor emission is directly linked to \u03c0\u2013\u03c0 interactions within the dimers: a smaller interplanar distance and a larger overlap ratio between \u03c0\u2013\u03c0 PE units result in more strengthened interactions and more red\u2010shifted emission. On the other hand, the observed multicolor transitions under pressure (yellow\u00a0\u2192\u00a0orange\u00a0\u2192\u00a0red) via dimer compression and thermal stimuli (sky\u2010blue\u00a0\u2192\u00a0green\u00a0\u2192\u00a0orange) through dimer (dis)assembly provide dynamic presentation of the dimer model. Consequently, polymorphism\/piezochromism\/thermochromism not only provides\u00a0direct experimental evidence for exciton modulation from the perspective of the simplest supramolecular dimer model, but also offers insights for designing intelligent optical materials.<\/jats:p>","DOI":"10.1002\/anie.8118945","type":"journal-article","created":{"date-parts":[[2026,6,18]],"date-time":"2026-06-18T17:49:25Z","timestamp":1781804965000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Geometric Evolution of Perylene\u2010Based Intermolecular \u03c0\u2013\u03c0 Dimers Toward Static and Dynamic Multicolor Emission"],"prefix":"10.1002","volume":"65","author":[{"given":"Zhou\u2010An","family":"Xia","sequence":"first","affiliation":[{"name":"State Key Laboratory of Supramolecular Structure and Materials College of Chemistry Jilin University  Changchun 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