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In this study, we demonstrate that a cyclic\u00ad(alkyl)\u00ad(amino)\u00adcarbene (CAAC)-derived carbon disulfide adduct functions as a radical ligand, supporting Pd\u00ad(II) and Ni\u00ad(II) complexes with multiconfigurational electronic structures. Single-crystal X-ray crystallography confirms that both 1\u2013Pd and 1\u2013Ni adopt a square planar geometry with structural parameters consistent with the presence of ligand-centered unpaired electrons. Computational studies indicate that both complexes favor an open-shell singlet ground state, with small energy gaps to the triplet and closed-shell singlet states, which could likely facilitate electronic state mixing. This work highlights the effectiveness of CAAC-derived radical ligands in stabilizing multiconfigurational electronic states in metal complexes, opening avenues for potential applications in catalysis and materials science.<\/jats:p>","DOI":"10.1021\/acsomega.5c04023","type":"journal-article","created":{"date-parts":[[2025,7,7]],"date-time":"2025-07-07T04:03:58Z","timestamp":1751861038000},"page":"29754-29759","source":"Crossref","is-referenced-by-count":4,"title":["Open-Shell Pd(II)\nand Ni(II) Complexes Supported by\nCyclic(alkyl)(amino)carbene-Derived Carbon Disulfide Radical Ligands"],"prefix":"10.1021","volume":"10","author":[{"given":"Gayeong","family":"Lim","sequence":"first","affiliation":[{"name":"Pusan National University , , ,","place":["Busan, Republic of Korea, 46241"]},{"name":"Pusan National University , , ,","place":["Busan, Republic of Korea, 46241"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongmin","family":"Kang","sequence":"additional","affiliation":[{"name":"Pusan National University , , ,","place":["Busan, Republic of Korea, 46241"]},{"name":"Pusan National University , , ,","place":["Busan, Republic of Korea, 46241"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jeongcheol","family":"Shin","sequence":"additional","affiliation":[{"name":"Duksung Women\u2019s University , , ,","place":["Seoul, Republic of Korea, 01369"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7378-2301","authenticated-orcid":true,"given":"Youngsuk","family":"Kim","sequence":"additional","affiliation":[{"name":"Pusan National University , , ,","place":["Busan, Republic of Korea, 46241"]},{"name":"Pusan National University , , ,","place":["Busan, Republic of Korea, 46241"]},{"name":"Pusan National University , , ,","place":["Busan, Republic\nof Korea, 46241"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2025,7,7]]},"reference":[{"issue":"1","key":"2026081812140659600_cit1a","doi-asserted-by":"publisher","first-page":"218","DOI":"10.1016\/j.ccr.2012.07.007","article-title":"Transition\nmetal complexes of donor\u2013acceptor\nbiradicals","volume":"257","author":"Kirk","year":"2013","journal-title":"Coord. 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