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Although phosphorescent transition\u2010metal complexes exhibit significant potential as aggregation\u2010induced emission luminogens (AIEgens), their exploration and utilization have remained limited, partly due to the insufficient understanding of the underlying mechanisms. Here, we report a new series of platinum(II) complexes, <jats:italic>trans<\/jats:italic>\u2010bis(2\u2010iminomethylpyrrolato)platinum derivatives (<jats:bold>1a<\/jats:bold>\u2013<jats:bold>d<\/jats:bold>), which feature vaulted polymethylene chains of varying lengths (n\u00a0=\u00a09\u201312) that bridge over the metal atom. Notably, racemic complexes <jats:bold>1b<\/jats:bold> and <jats:bold>1d<\/jats:bold> (with chain lengths of 10 and 12) exhibit strong yellow emission in the crystalline state (quantum yields of 24% and 33%, respectively), despite showing no emission in solution. X\u2010ray diffraction analysis revealed face\u2010to\u2010face dimer packing in these emissive crystals, suggesting that dimer formation contributes to their enhanced emission. In contrast, complexes with odd\u2010numbered chain lengths (<jats:bold>1a<\/jats:bold> and <jats:bold>1c<\/jats:bold>) showed no such emission enhancement. Density functional theory (DFT) calculations revealed that the minimum energy crossing point (MECP) between the excited triplet and ground state lies at significantly higher energy in the dimeric structure than in the monomer, suggesting suppression of nonradiative decay in the crystalline state. This work provides a design strategy for inducing solid\u2010state phosphorescence by controlling the 3D molecular structure to facilitate favorable molecular stacking while suppressing nonradiative decay pathways.<\/jats:p>","DOI":"10.1002\/chem.202501670","type":"journal-article","created":{"date-parts":[[2025,7,31]],"date-time":"2025-07-31T10:50:14Z","timestamp":1753959014000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Aggregation\u2010Induced Phosphorescence of a <i>Trans<\/i>\u2010Bis(iminomethylpyrolato)Platinum Complex Bearing a Polymethylene Vaulted Structure: Chain Length\u2013Dependent Solid\u2010State Emissions"],"prefix":"10.1002","volume":"31","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2093-5175","authenticated-orcid":false,"given":"Soichiro","family":"Kawamorita","sequence":"first","affiliation":[{"name":"Department of Chemistry Graduate School of Engineering Science The University of Osaka  Machikaneyama Toyonaka Osaka 560\u20138531 Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Shufang","family":"Huang","sequence":"additional","affiliation":[{"name":"Department of Chemistry Graduate School of Engineering Science The University of Osaka  Machikaneyama Toyonaka Osaka 560\u20138531 Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Atsushi","family":"Yoshida","sequence":"additional","affiliation":[{"name":"Department of Chemistry Graduate School of Engineering Science The University of Osaka  Machikaneyama Toyonaka Osaka 560\u20138531 Japan"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6294-9084","authenticated-orcid":false,"given":"Shuichi","family":"Suzuki","sequence":"additional","affiliation":[{"name":"Department of Chemistry Graduate School of Engineering Science The University of Osaka  Machikaneyama Toyonaka Osaka 560\u20138531 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