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Despite significant advances in main group\u2010based diradicaloids in contemporary chemistry, main group THs containing an anthrylene cores have remained elusive, primarily due to the lack of straightforward synthetic strategies and the inherent high reactivity of these species. In this study, we utilize an anthracene\u2010based phosphine synthon to demonstrate, for the first time, a facile and high\u2010yielding synthetic strategy for robust P\u2010functionalized overcrowded ethylenes (OCEs) within the TH family. These OCEs feature a non\u2010symmetric environment, incorporating (thio) xanthyl and phosphaalkene termini. We systematically probe the electronic structures of these derivatives to illustrate the impact of the isolobal phosphaalkene motif on the quinoidal\/diradicaloid character. Notably, the compounds exhibit dynamic redox behavior, leading to orthogonally twisted conformational changes upon oxidation, with a kinetically locked redox\u2010couple.<\/jats:p>","DOI":"10.1002\/anie.202406076","type":"journal-article","created":{"date-parts":[[2024,8,19]],"date-time":"2024-08-19T12:55:11Z","timestamp":1724072111000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":14,"title":["Introducing Phosphorus into the Overcrowded Thiele's hydrocarbon Family: Unveiling Contorted Main Group Diradicaloids with Dynamic Redox Behavior"],"prefix":"10.1002","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9460-1784","authenticated-orcid":false,"given":"Rajesh","family":"Deka","sequence":"first","affiliation":[{"name":"Department of Chemistry\u2013\u00c5ngstr\u00f6m laboratories (Synthetic Molecular Chemistry) Uppsala University  BOX 523 75120 Uppsala 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