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Excitation in all cases results in prompt C\u2013Cl bond fission, on timescales shorter than the parent rotational period. Most of the excess energy is partitioned into product kinetic energy, ET, but the deduced Cl\/Cl* branching ratios and favored CH3 product vibrational motions are excitation wavelength\/excited state dependent. So, too, are the fragment recoil anisotropies which, even within one CH3(v) + Cl\/Cl* product channel, are found to be sensitive functions of ET. The trends observed at longer \u03bb reflect the wavelength dependent partial cross sections for excitation to the 3Q1, 3Q0, and 1Q1 components of the A band continuum, but full interpretation of the present data demands a much more detailed, quantum state resolved picture of the non-adiabatic population transfer probabilities between these dissociative parent states and, at higher excitation energies, the Jahn\u2013Teller induced distortions within the photoexcited Rydberg states and their non-adiabatic couplings with the continuum states. Additional CH3+ and Cl+ signals evident in the images at lower ET are attributed to, respectively, two pump photon induced dissociative ionizations and one probe photon induced photodissociation of CH2Cl products formed via a competing primary C\u2013H bond fission process.<\/jats:p>","DOI":"10.1063\/5.0282223","type":"journal-article","created":{"date-parts":[[2025,10,1]],"date-time":"2025-10-01T11:33:56Z","timestamp":1759318436000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":3,"title":["Velocity map imaging studies of the ultraviolet photodissociation of methyl chloride"],"prefix":"10.1063","volume":"163","author":[{"ORCID":"https:\/\/orcid.org\/0009-0002-6802-3340","authenticated-orcid":false,"given":"Yucheng","family":"Wu","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 1 , 457 Zhongshan Road, Dalian 116023,","place":["China"]},{"name":"University of Chinese Academy of Sciences 2 , Beijing 100049,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9376-3629","authenticated-orcid":false,"given":"Zijie","family":"Luo","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 1 , 457 Zhongshan Road, Dalian 116023,","place":["China"]},{"name":"Marine Engineering College, Dalian Maritime University 3 , Liaoning 116026,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0008-4293-8204","authenticated-orcid":false,"given":"Shuaikang","family":"Yang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 1 , 457 Zhongshan Road, Dalian 116023,","place":["China"]},{"name":"Department of Chemical Physics, School of Chemistry and Materials Science, University of Science and Technology of China 4 , Jinzhai Road 96, Hefei, Anhui 230026,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Stephanie J.","family":"McGoldrick","sequence":"additional","affiliation":[{"name":"School of Chemistry, University of New South Wales 5 , Sydney, NSW 2052,","place":["Australia"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-7797-0234","authenticated-orcid":false,"given":"Jay L.","family":"Mendham","sequence":"additional","affiliation":[{"name":"School of Chemistry, University of New South Wales 5 , Sydney, NSW 2052,","place":["Australia"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0006-9266-9191","authenticated-orcid":false,"given":"Zhenxing","family":"Li","sequence":"additional","affiliation":[{"name":"Institute of Advanced Light Source Facilities 6 , Shenzhen, Guangdong 518100,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shunyang","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 1 , 457 Zhongshan Road, Dalian 116023,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yongxin","family":"Dong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 1 , 457 Zhongshan Road, Dalian 116023,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dongxu","family":"Dai","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics and Dalian Coherent Light Source, Dalian Institute of Chemical Physics, Chinese Academy of Sciences 1 , 457 Zhongshan Road, Dalian 116023,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8954-0825","authenticated-orcid":false,"given":"Christopher S.","family":"Hansen","sequence":"additional","affiliation":[{"name":"School of Chemistry, University of New South Wales 5 , Sydney, NSW 2052,","place":["Australia"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5762-7048","authenticated-orcid":false,"given":"Michael N. 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