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Here, we report a polyoxometalate (POM)\u2010scaffolded strategy that integrates structural preorganization with dynamic charge regulation in perylene diimide (PDI) dimers. Rigid, redox\u2010active lacunary POM clusters preorganize two PDIs into a tightly stacked, parallel\u2010displaced, rotationally aligned arrangement favorable for excimer formation. This preorganization enables ultrafast excimer formation, prolongs excited\u2010state lifetimes, and promotes efficient singlet oxygen generation. Beyond structural preorganization, the POM scaffolds actively regulate excited\u2010state charge dynamics by acting as intramolecular charge buffers, suppressing radical\u2010induced photodegradation under aerobic conditions. The combination of geometric control and dynamic charge regulation affords durable photosensitization, establishing inorganic molecular clusters as multifunctional scaffolds for excited\u2010state engineering.<\/jats:p>","DOI":"10.1002\/smll.76213","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T08:34:57Z","timestamp":1791794097000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Polyoxometalate\u2010Scaffolded Perylene Diimide Dimers: Preorganization and Dynamic Charge Regulation for Enhanced and Durable Photosensitization"],"prefix":"10.1002","author":[{"given":"Masahiro","family":"Yamaguchi","sequence":"first","affiliation":[{"name":"Department of Applied Chemistry School of Engineering The University of Tokyo  Bunkyo\u2010ku Tokyo 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