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The latter employ local high\u2010spin metal centers; however, iron\u2013dinitrogen coordination chemistry remains dominated by low\u2010valent states, contrasting the enzyme systems. Here, we report a high\u2010spin mixed\u2010valent <jats:italic>cis<\/jats:italic>\u2010(<jats:italic>\u03bc<\/jats:italic>\u20101,2\u2010dinitrogen)diiron(I\/II) complex [(FeBr)<jats:sub>2<\/jats:sub>(<jats:italic>\u03bc<\/jats:italic>\u2010N<jats:sub>2<\/jats:sub>)<jats:bold>L<jats:sup>bis<\/jats:sup><\/jats:bold>]<jats:sup>\u2212<\/jats:sup> (<jats:bold>2<\/jats:bold>), where [<jats:bold>L<jats:sup>bis<\/jats:sup><\/jats:bold>]<jats:sup>\u2212<\/jats:sup> is a bis(\u03b2\u2010diketiminate) cyclophane. Field\u2010applied M\u00f6ssbauer spectra, dc and ac magnetic susceptibility measurements, and computational methods support a delocalized <jats:italic>S<\/jats:italic>=<jats:sup>7<\/jats:sup>\/<jats:sub>2<\/jats:sub> Fe<jats:sub>2<\/jats:sub>N<jats:sub>2<\/jats:sub> unit with <jats:italic>D<\/jats:italic>=\u22125.23\u2005cm<jats:sup>\u22121<\/jats:sup> and consequent slow magnetic relaxation.<\/jats:p>","DOI":"10.1002\/anie.202202329","type":"journal-article","created":{"date-parts":[[2022,3,18]],"date-time":"2022-03-18T13:26:40Z","timestamp":1647610000000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":18,"title":["Dinitrogen Coordination to a High\u2010Spin Diiron(I\/II) Species"],"prefix":"10.1002","volume":"61","author":[{"given":"Juan F.","family":"Torres","sequence":"first","affiliation":[{"name":"Center for Catalysis and Florida Center for Heterocyclic Chemistry Department of Chemistry University of Florida  Gainesville FL 32611 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Collin H.","family":"Oi","sequence":"additional","affiliation":[{"name":"Center for Catalysis and Florida Center for Heterocyclic Chemistry Department of Chemistry University of Florida  Gainesville FL 32611 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ian P.","family":"Moseley","sequence":"additional","affiliation":[{"name":"Department of Chemistry Colorado State University  Fort Collins CO 80523 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Nabila","family":"El\u2010Sakkout","sequence":"additional","affiliation":[{"name":"Univ. Grenoble Alpes CNRS CEA IRIG Laboratoire de Chimie et Biologie des M\u00e9taux  17 rue des Martyrs 38000 Grenoble France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Brian J.","family":"Knight","sequence":"additional","affiliation":[{"name":"Center for Catalysis and Florida Center for Heterocyclic Chemistry Department of Chemistry University of Florida  Gainesville FL 32611 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jason","family":"Shearer","sequence":"additional","affiliation":[{"name":"Department of Chemistry Trinity University  San Antonio TX 78212 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ricardo","family":"Garc\u00eda\u2010Serres","sequence":"additional","affiliation":[{"name":"Univ. Grenoble Alpes CNRS CEA IRIG Laboratoire de Chimie et Biologie des M\u00e9taux  17 rue des Martyrs 38000 Grenoble France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Joseph M.","family":"Zadrozny","sequence":"additional","affiliation":[{"name":"Department of Chemistry Colorado State University  Fort Collins CO 80523 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1568-958X","authenticated-orcid":false,"given":"Leslie J.","family":"Murray","sequence":"additional","affiliation":[{"name":"Center for Catalysis and Florida Center for Heterocyclic Chemistry Department of Chemistry University of Florida  Gainesville FL 32611 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2022,3,31]]},"reference":[{"key":"e_1_2_3_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.0c00042"},{"key":"e_1_2_3_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.200800480"},{"key":"e_1_2_3_2_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.200800480"},{"key":"e_1_2_3_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.9b00556"},{"key":"e_1_2_3_4_1","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.1315852110"},{"key":"e_1_2_3_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/C9SC03610E"},{"key":"e_1_2_3_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c07914"},{"key":"e_1_2_3_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.biochem.8b00509"},{"key":"e_1_2_3_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c01861"},{"key":"e_1_2_3_9_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c01488"},{"key":"e_1_2_3_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201409676"},{"key":"e_1_2_3_10_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201409676"},{"key":"e_1_2_3_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.8b02021"},{"key":"e_1_2_3_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/ejic.201901335"},{"key":"e_1_2_3_13_1","doi-asserted-by":"publisher","DOI":"10.1039\/c3cc43395a"},{"key":"e_1_2_3_14_1","doi-asserted-by":"publisher","DOI":"10.1039\/B617136B"},{"key":"e_1_2_3_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja507442b"},{"key":"e_1_2_3_16_1","doi-asserted-by":"publisher","DOI":"10.1021\/ic101646p"},{"key":"e_1_2_3_17_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8CC07294A"},{"key":"e_1_2_3_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja036687f"},{"key":"e_1_2_3_19_1","doi-asserted-by":"publisher","DOI":"10.1039\/jr9590002003"},{"key":"e_1_2_3_20_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1CS00001B"},{"key":"e_1_2_3_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/andp.19123441404"},{"key":"e_1_2_3_22_1","doi-asserted-by":"publisher","DOI":"10.1039\/c001397h"},{"key":"e_1_2_3_23_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.585"},{"key":"e_1_2_3_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja808783u"},{"key":"e_1_2_3_25_1","unstructured":"Deposition Numbers2121401 (for1) 2121402 (forBr3) 2121403 (for2-crypt) and 2121404 (for H2Lbis)contain the supplementary crystallographic data for this paper. 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