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The initial state is confirmed with spectroelectrochemistry to have significant metal-to-ligand charge transfer (MLCT) character, unlike other Co complexes that generally have ligand-to-metal charge transfer or ligand-field transitions in this energy range. Ground-state recovery occurs in 8.65 ps in dichloromethane. Density functional theory calculations show that the MLCT state undergoes Jahn\u2013Teller distortion and converts to a five-coordinate triplet metal-centered state in which one Co\u2013N bond is broken. The results highlight a potential pitfall of heteroleptic bidentate ligands when designing strong-field ligands for transition-metal chromophores.<\/jats:p>","DOI":"10.1021\/acs.inorgchem.4c01959","type":"journal-article","created":{"date-parts":[[2024,7,18]],"date-time":"2024-07-18T11:01:08Z","timestamp":1721300468000},"page":"13825-13830","source":"Crossref","is-referenced-by-count":9,"title":["Picosecond Metal-to-Ligand Charge-Transfer Deactivation\nin Co(ppy)3 via Jahn\u2013Teller Distortion"],"prefix":"10.1021","volume":"63","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-8677-3167","authenticated-orcid":true,"given":"Claire","family":"Malme","sequence":"first","affiliation":[{"name":"University of Illinois at Urbana\u2212Champaign , , , ,","place":["Champaign, Illinois, United States, 61801"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Jenelle N.","family":"Weaver","sequence":"additional","affiliation":[{"name":"University of Illinois at Urbana\u2212Champaign , , , ,","place":["Champaign, Illinois, United States, 61801"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gregory S.","family":"Girolami","sequence":"additional","affiliation":[{"name":"University of Illinois at Urbana\u2212Champaign , , , ,","place":["Champaign, Illinois, United States, 61801"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7734-3130","authenticated-orcid":true,"given":"Josh","family":"Vura-Weis","sequence":"additional","affiliation":[{"name":"University of Illinois at Urbana\u2212Champaign , , , ,","place":["Champaign, Illinois, United States, 61801"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2024,7,18]]},"reference":[{"issue":"9","key":"2026091419063160500_cit1","doi-asserted-by":"publisher","first-page":"4903","DOI":"10.1021\/jacs.2c13432","article-title":"Photoactive Metal-to-Ligand Charge Transfer Excited\nStates in 3d6 Complexes with Cr0, MnI, FeII, and CoIII","volume":"145","author":"Sinha","year":"2023","journal-title":"J.\nAm. 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