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Here, we theoretically show that two ultraviolet pulses enable mode-selective photodissociation in HOD, which has distinct O\u2013H and O\u2013D bonds. The first pulse initiates dissociation and, through resonant Raman scattering, creates vibrational coherence in the ground electronic state. The second pulse, applied after a controlled delay, interacts with this coherence to determine which bond breaks. By adjusting the inter-pulse delay, we tune the H + OD-to-D + OH branching ratio from above 2.0 (single-pulse) to about 1.3. Modifying the chirps of both pulses further reduces the ratio to nearly 1.0. These results show that vibrational coherence from resonant Raman scattering can be used to control chemical reactions on femtosecond timescales, and this method may be applicable to other molecular systems.<\/jats:p>","DOI":"10.1063\/5.0349395","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T17:54:21Z","timestamp":1786989261000},"update-policy":"https:\/\/doi.org\/10.1063\/aip-crossmark-policy-page","source":"Crossref","is-referenced-by-count":0,"title":["Raman-induced vibrational coherence control of bond-selective HOD photodissociation with two UV pulses"],"prefix":"10.1063","volume":"165","author":[{"ORCID":"https:\/\/orcid.org\/0009-0008-8329-3182","authenticated-orcid":false,"given":"Wen-Quan","family":"Jing","sequence":"first","affiliation":[{"name":"Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics, Central South University 1 , Changsha 410083,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5665-0879","authenticated-orcid":false,"given":"Zhao-Peng","family":"Sun","sequence":"additional","affiliation":[{"name":"School of Physics and Optoelectric Engineering, Institute of Theoretical Physics, Ludong University 2 , Yantai 264025,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3168-9819","authenticated-orcid":false,"given":"Jian-Qiao","family":"Meng","sequence":"additional","affiliation":[{"name":"Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics, Central South University 1 , Changsha 410083,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3105-3872","authenticated-orcid":false,"given":"Song-Feng","family":"Zhao","sequence":"additional","affiliation":[{"name":"Key Laboratory of Atomic and Molecular Physics and Functional Materials of Gansu Province, College of Physics and Electronic Engineering, Northwest Normal University 3 , Lanzhou 730070,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9096-5129","authenticated-orcid":false,"given":"Chuan-Cun","family":"Shu","sequence":"additional","affiliation":[{"name":"Hunan Key Laboratory of Super-Microstructure and Ultrafast Process, School of Physics, Central South University 1 , Changsha 410083,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"317","published-online":{"date-parts":[[2026,8,17]]},"reference":[{"key":"2026081713541643200_c1","doi-asserted-by":"publisher","first-page":"1115","DOI":"10.1063\/1.447805","article-title":"Intramolecular vibrational relaxation and spectra of CH and CD overtones in benzene and perdeuterobenzene","volume":"81","year":"1984","journal-title":"J.\u00a0Chem. 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