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SCO can be understood as the interplay of anharmonically coupled vibrational modes that collectively drive the system across curve\u2010crossings. However, these modes are difficult to identify due to challenges in simulating open\u2010shell systems. Here, we combine ultrafast broadband transient absorption spectroscopy in single crystals with multireference excited\u2010state dynamical simulations to reveal the SCO mechanism in an Fe(III) complex. We identify the key doorway modes that direct the system across the curve\u2010crossing region to form the high\u2010spin state. The pronounced anharmonicity and reactive forces at SCO curve crossings provide a strong driving force for these displaced modes, leading to phase\u2010delayed, coherent non\u2010impulsive vibrational energy transfer. This study leads to unprecedented direct visualization of the SCO dynamics, revealing how the transition kernel and low\u2010dimensional pathways emerge from the strongly anharmonic crossing regions of the potential energy surfaces. A detailed understanding of these SCO processes is crucial for the development of advanced materials with applications ranging from high\u2010speed memory storage to light\u2010harvesting devices.<\/jats:p>","DOI":"10.1002\/anie.1079807","type":"journal-article","created":{"date-parts":[[2026,4,1]],"date-time":"2026-04-01T13:32:11Z","timestamp":1775050331000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":4,"title":["Elucidating the Transition Kernel and Anharmonic Coupling in the Spin\u2010crossover Process of a [Fe\n                    <sup>III<\/sup>\n                    (qsal)\n                    <sub>2<\/sub>\n                    ] CH\n                    <sub>3<\/sub>\n                    OSO\n                    <sub>3<\/sub>\n                    Complex"],"prefix":"10.1002","volume":"65","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-7239-1547","authenticated-orcid":false,"given":"Soumyajit","family":"Mitra","sequence":"first","affiliation":[{"name":"Departments of Chemistry and Physics University of Toronto  Toronto Canada"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0003-2012-1221","authenticated-orcid":false,"given":"Dilara","family":"Farkhutdinova","sequence":"additional","affiliation":[{"name":"Institute of Theoretical Chemistry Faculty of Chemistry University of Vienna  Vienna Austria"},{"name":"Vienna Doctoral School in Chemistry (DoSChem) University of Vienna  Vienna Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5327-8880","authenticated-orcid":false,"given":"Sebastian","family":"Mai","sequence":"additional","affiliation":[{"name":"Institute of Theoretical Chemistry Faculty of Chemistry University of Vienna  Vienna Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-6750-5563","authenticated-orcid":false,"given":"Stuart A.","family":"Hayes","sequence":"additional","affiliation":[{"name":"Departments of Chemistry and Physics University of Toronto  Toronto Canada"},{"name":"European XFEL  Schenefeld Germany"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yifeng","family":"Jiang","sequence":"additional","affiliation":[{"name":"European XFEL  Schenefeld Germany"},{"name":"State Key Laboratory of Precision Spectroscopy East China Normal University  Shanghai China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7018-654X","authenticated-orcid":false,"given":"Tadahiko","family":"Ishikawa","sequence":"additional","affiliation":[{"name":"Department of Chemistry Institute of Science Tokyo  Tokyo Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1776-4416","authenticated-orcid":false,"given":"Kazuyuki","family":"Takahashi","sequence":"additional","affiliation":[{"name":"Department of Chemistry Kobe University  Kobe Japan"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5112-794X","authenticated-orcid":false,"given":"Leticia","family":"Gonz\u00e1lez","sequence":"additional","affiliation":[{"name":"Institute of Theoretical Chemistry Faculty of Chemistry University of Vienna  Vienna Austria"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-0884-0541","authenticated-orcid":false,"given":"R. 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