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It is well-established that rotationally inelastic collisions of heteronuclear diatoms might exhibit double rainbows, due to different intermolecular interactions at the two ends of the diatom. This is in sharp contrast to single rainbows for homonuclear diatoms. Here, we present experimental observations of double rainbow structures in the collisional charge-transfer reaction between spin\u2013orbit selected Ar+(2P3\/2) ions and a representative homonuclear diatom (N2), using an advanced imaging-based ion\u2013molecule crossed-beam method. Trajectory surface hopping calculations involving multiple electronic states reproduced the experimental observations qualitatively and revealed that collinear approaches of the two colliders show higher charge-transfer efficiencies than side-on approaches due to angle-dependent nonadiabatic interactions. The closest encounters before and after charge transfer experience vastly different anisotropies of the short-range intermolecular repulsion in the two charge-transfer states, thus manifesting as the twin rainbow structures. This mechanism differs fundamentally from those observed in the adiabatic scattering.<\/jats:p>","DOI":"10.1021\/jacs.6c05560","type":"journal-article","created":{"date-parts":[[2026,6,2]],"date-time":"2026-06-02T06:25:59Z","timestamp":1780381559000},"page":"24317-24325","source":"Crossref","is-referenced-by-count":0,"title":["Double Rotational Rainbows\nin Collisions of Homonuclear\nDiatoms Stemming from Steric Charge Transfer"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0009-0009-9907-8687","authenticated-orcid":true,"given":"Hanyao","family":"Wang","sequence":"first","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dandan","family":"Lu","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of New Mexico , , , ,","place":["Albuquerque, New Mexico, United States, 87131"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5826-5149","authenticated-orcid":true,"given":"Min","family":"Cheng","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Guodong","family":"Zhang","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9901-053X","authenticated-orcid":true,"given":"Hua","family":"Guo","sequence":"additional","affiliation":[{"name":"University of New Mexico , , , ,","place":["Albuquerque, New Mexico, United States, 87131"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6168-7630","authenticated-orcid":true,"given":"Hong","family":"Gao","sequence":"additional","affiliation":[{"name":"Chinese Academy of Sciences , , ,","place":["Beijing, China, 100190"]},{"name":"University of Chinese Academy of Sciences , ,","place":["Beijing, China, 100049"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,6,2]]},"reference":[{"key":"2026073023155836200_cit1","doi-asserted-by":"publisher","first-page":"109","DOI":"10.1146\/annurev.pc.46.100195.000545","article-title":"Gas-phase reactions and energy transfer at very low\ntemperatures","volume":"46","author":"Sims","year":"1995","journal-title":"Annu. 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Chem.\nLett."},{"issue":"1","key":"2026073023155836200_cit36","doi-asserted-by":"publisher","first-page":"149","DOI":"10.1016\/0301-0104(87)80227-6","article-title":"A crossed-beam study\nof the reactive and unreactive scattering of Ar+(2P3\/2) and Ar+(2P1\/2)\nby N2 at low energies","volume":"113","author":"Birkinshaw","year":"1987","journal-title":"Chem. Phys."},{"issue":"25","key":"2026073023155836200_cit37","doi-asserted-by":"publisher","first-page":"2990","DOI":"10.1039\/B603109A","article-title":"Velocity map imaging of ion\u2013molecule reactive\nscattering: The Ar+ + N2 charge transfer reaction","volume":"8","author":"Mikosch","year":"2006","journal-title":"Phys. Chem. Chem. 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Chem."}],"container-title":["Journal of the American\nChemical Society"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/jacs.6c05560","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/23\/24317\/66272012\/jacs.6c05560.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/jacsat\/article-pdf\/148\/23\/24317\/66272012\/jacs.6c05560.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,7,31]],"date-time":"2026-07-31T03:16:07Z","timestamp":1785467767000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/jacsat\/article\/148\/23\/24317\/5233499\/Double-Rotational-Rainbows-in-Collisions-of"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,6,2]]},"references-count":52,"journal-issue":{"issue":"23","published-online":{"date-parts":[[2026,6,2]]},"published-print":{"date-parts":[[2026,6,17]]}},"URL":"https:\/\/doi.org\/10.1021\/jacs.6c05560","relation":{},"ISSN":["0002-7863","1520-5126"],"issn-type":[{"value":"0002-7863","type":"print"},{"value":"1520-5126","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,6,2]]}}}