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Recently, muons have been applied to produce short\u2010lived paramagnetic species from the heavier unsaturated organic molecules including the p\u2010block elements. This article overviews recent muon spin rotation\/resonance (\u03bcSR) studies on the phosphorus analogs of alkenes, anthracenes, and cyclobutane\u20101,3\u2010diyls together with the fundamentals of \u03bcSR. The acyclic phosphaalkene of P=C and phosphasilenes of P=Si can accept muonium (Mu=[<jats:italic>\u03bc<\/jats:italic><jats:sup>+<\/jats:sup><jats:italic>e<\/jats:italic><jats:sup>\u2212<\/jats:sup>]) at the heavier double bonds, and the corresponding radicals have been characterized. The phosphorus atom in 9\u2010phosphaanthracene, whose P=C double bond is stabilized by the <jats:italic>peri<\/jats:italic>\u2010substituted CF<jats:sub>3<\/jats:sub> groups, predominantly captures muonium to provide the corresponding paramagnetic fused heterocyclic system. The <jats:italic>peri\u2010<\/jats:italic>trifluoromethyl groups are functional to promote the unprecedented light isotope effect of muon providing the planar three\u2010cyclic molecular structure to consume the increased zero\u2010point energy. The formally open\u2010shell singlet 1,3\u2010diphosphacyclobutane\u20102,4\u2010diyl unit can accept muonium at the (ylidic) phosphorus or the skeletal radicalic carbon, and the corresponding paramagnetic phosphorus heterocycles can be characterized by \u03bcSR. The findings on these muoniation processes to the unsaturated phosphorus\u2010containing compounds will contribute not only to development of novel paramagnetic functional species but also to progress on muon science.<\/jats:p>","DOI":"10.1002\/chem.202200843","type":"journal-article","created":{"date-parts":[[2022,6,15]],"date-time":"2022-06-15T01:54:15Z","timestamp":1655258055000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Muon Spin Rotation\/Resonance (\u03bcSR) for Studying Radical Reactivity of Unsaturated Organophosphorus Compounds"],"prefix":"10.1002","volume":"28","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-5737-8499","authenticated-orcid":false,"given":"Shigekazu","family":"Ito","sequence":"first","affiliation":[{"name":"Department of Applied Chemistry School of Materials and Chemical Technology Tokyo Institute of Technology  2-12-1-H113 Ookayama, Meguro-ku Tokyo 152-8552 Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2022,7,25]]},"reference":[{"key":"e_1_2_10_1_1","volume-title":"Muon Spectroscopy \u2013 An Introduction","author":"Blundell S. 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