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In this work, we investigate spin\u2013vibronic coherence along the Pt\u2013Pt stretching normal mode in a series of five structurally tuned, double-bridged Pt(II) dimers using nonadiabatic dynamics incorporating both spin\u2013orbit coupling and derivative nonadiabatic couplings. Across these systems, the variations in cyclometalating and bridging ligands modulate Pt\u2013Pt distances, excited-state electronic structure, and spin\u2013orbit coupling strengths that enable systematic probing of coherence mechanisms. We show that ligand-controlled spin\u2013orbit coupling dictates early time intersystem crossing behavior. Fourier analysis of time-dependent populations reveals that spin\u2013vibronic coherence arises when the Pt\u2013Pt stretching frequency becomes near-resonant with the spin\u2013orbit coupling between singlet and triplet states. If spin\u2013orbit coupling is too weak, vibrational motion dominates; if spin\u2013orbit coupling is too strong, intersystem crossing and vibration become decoupled. These results establish a clear mechanistic picture and provide molecular design guidelines for modulating spin\u2013vibronic coherence in photoluminescent and photocatalytic Pt(II) systems.<\/jats:p>","DOI":"10.1021\/acs.jpclett.6c01705","type":"journal-article","created":{"date-parts":[[2026,9,21]],"date-time":"2026-09-21T22:02:24Z","timestamp":1790028144000},"page":"11008-11016","source":"Crossref","is-referenced-by-count":0,"title":["Emergence of\nSpin\u2013Vibronic Coherence in the\nIntermediate Spin\u2013Orbit Coupling Regime Revealed by Mixed Quantum-Classical\nDynamics"],"prefix":"10.1021","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-2676-0271","authenticated-orcid":true,"given":"Maxwell","family":"Taub","sequence":"first","affiliation":[{"name":"University of Washington , , , ,","place":["Seattle, Washington, United States, 98195"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2276-4901","authenticated-orcid":true,"given":"Diandong","family":"Tang","sequence":"additional","affiliation":[{"name":"University of Washington , , , ,","place":["Seattle, Washington, United States, 98195"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5837-4740","authenticated-orcid":true,"given":"George C.","family":"Schatz","sequence":"additional","affiliation":[{"name":"Northwestern University , , , ,","place":["Evanston, Illinois, United States, 60208"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7546-8618","authenticated-orcid":true,"given":"Felix N.","family":"Castellano","sequence":"additional","affiliation":[{"name":"North Carolina State University , , , ,","place":["Raleigh, North Carolina, United States, 27695"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8450-6687","authenticated-orcid":true,"given":"Lin X.","family":"Chen","sequence":"additional","affiliation":[{"name":"Argonne National Laboratory , , , ,","place":["Lemont, Illinois, United States, 60439"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7341-6240","authenticated-orcid":true,"given":"Xiaosong","family":"Li","sequence":"additional","affiliation":[{"name":"University of Washington , , , ,","place":["Seattle, Washington, United States, 98195"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,21]]},"reference":[{"key":"2026100109084004700_cit1","doi-asserted-by":"publisher","first-page":"354","DOI":"10.1063\/1.1733665","article-title":"Vibronic\u2500Spin-Orbit\nPerturbations and the Assignment of the Lowest Triplet State of Benzene","volume":"38","author":"Albrecht","year":"1963","journal-title":"J. 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