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Single-molecule magnets based on lanthanides have accounted for many important advances, including systems with very large energy barriers to reversal of the magnetization, and a di-terbium complex that displays magnetic hysteresis up to 14\u2009K and shows strong coercivity. Ligand design is crucial for the development of new single-molecule magnets: organometallic chemistry presents possibilities for using unconventional ligands, particularly those with soft donor groups. Here we report dysprosium single-molecule magnets with neutral and anionic phosphorus donor ligands, and show that their properties change dramatically when varying the ligand from phosphine to phosphide to phosphinidene. A phosphide-ligated, trimetallic dysprosium single-molecule magnet relaxes via the second-excited Kramers' doublet, and, when doped into a diamagnetic matrix at the single-ion level, produces a large energy barrier of 256\u2009cm<jats:sup>\u22121<\/jats:sup> and magnetic hysteresis up to 4.4\u2009K.<\/jats:p>","DOI":"10.1038\/ncomms8492","type":"journal-article","created":{"date-parts":[[2015,7,1]],"date-time":"2015-07-01T12:24:03Z","timestamp":1435753443000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":144,"title":["Influencing the properties of dysprosium single-molecule magnets with phosphorus donor ligands"],"prefix":"10.1038","volume":"6","author":[{"given":"Thomas","family":"Pugh","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Floriana","family":"Tuna","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5015-4225","authenticated-orcid":false,"given":"Liviu","family":"Ungur","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"David","family":"Collison","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Eric J.L.","family":"McInnes","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Liviu F.","family":"Chibotaru","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Richard A.","family":"Layfield","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2015,7,1]]},"reference":[{"key":"BFncomms8492_CR1","doi-asserted-by":"publisher","first-page":"8694","DOI":"10.1021\/ja029629n","volume":"125","author":"N Ishikawa","year":"2003","unstructured":"Ishikawa, N., Sugita, M., Ishikawa, T., Koshihara, S. & Kaizu, Y. 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