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Herein, we report a model van der Waals solid based on copper\u2013iodide clusters, where two vertically oriented and alternately arranged [Cu\n                    <jats:sub>2<\/jats:sub>\n                    I\n                    <jats:sub>4<\/jats:sub>\n                    ]\n                    <jats:sup>2\u2212<\/jats:sup>\n                    clusters are assembled via protection and interaction afforded by peripheral long\u2010alkyl\u2010chain cetyltrimethylammonium bromide ligands. This unique architecture affords a cooperative distortion response and exceptional buffering capacity, enabling precise control and direct probing of atomic\u2010scale structural distortions under pressure. We demonstrate that hydrostatic pressure induces controlled atomic distortions and an isostructural phase transition, which collectively enhance exciton localization. This leads to a dramatic amplification of self\u2010trapped emission, boosting the photoluminescence quantum yield from 32.25% to near\u2010unity (99.82%). Our work establishes atomic\u2010distortion engineering as a general principle for achieving ultimate control over light emission in hybrid semiconductors.\n                  <\/jats:p>","DOI":"10.1002\/anie.202522640","type":"journal-article","created":{"date-parts":[[2025,12,10]],"date-time":"2025-12-10T07:02:36Z","timestamp":1765350156000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Atomic\u2010Scale Structural Distortion Drives Exciton Localization for Near\u2010Unity Photoluminescence in Copper\u2013Iodide Clusters"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9281-3484","authenticated-orcid":false,"given":"Haifeng","family":"Zhu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Integrated Optoelectronics College of Electronic Science and Engineering Jilin University  2699 Qianjin Street Changchun 130012 P.R. 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