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Our results reveal that, while extraction of hot holes becomes efficient for interband excitation, harvesting of multiple hot holes from the excited Au nanospheres becomes prevalent only beyond a threshold light intensity. We show that the alkene oxidation proceeded via a sequence of two consecutive elementary steps; namely, a binding step and a cyclic oxometallate transition state as the rate\u2010determining step. This demonstration of plasmon\u2010excitation\u2010mediated harvesting of multiple hot holes without the use of an extra hole transport media opens exciting possibilities, notably for difficult catalytic transformations involving multielectron oxidation processes.<\/jats:p>","DOI":"10.1002\/anie.202215933","type":"journal-article","created":{"date-parts":[[2022,12,16]],"date-time":"2022-12-16T08:38:38Z","timestamp":1671179918000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":28,"title":["Simultaneous Harvesting of Multiple Hot Holes via Visible\u2010Light Excitation of Plasmonic Gold Nanospheres for Selective Oxidative Bond Scission of Olefins to Carbonyls"],"prefix":"10.1002","volume":"62","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8693-2591","authenticated-orcid":false,"given":"Swathi","family":"Swaminathan","sequence":"first","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Kanpur  Kanpur 208016 Uttar Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5689-8863","authenticated-orcid":false,"given":"Jitendra K.","family":"Bera","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Kanpur  Kanpur 208016 Uttar Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5272-4591","authenticated-orcid":false,"given":"Manabendra","family":"Chandra","sequence":"additional","affiliation":[{"name":"Department of Chemistry Indian Institute of Technology Kanpur  Kanpur 208016 Uttar Pradesh India"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,1,12]]},"reference":[{"key":"e_1_2_7_1_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja310501y"},{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201301096"},{"key":"e_1_2_7_2_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.201301096"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.5b00950"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1021\/nl303940z"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja411017b"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/nl302796f"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/nnano.2013.18"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.1032"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1038\/nmat3454"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1231631"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202101639"},{"key":"e_1_2_7_11_2","doi-asserted-by":"publisher","DOI":"10.1002\/ange.202101639"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.6b01373"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.8b03617"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.0c03040"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpclett.7b00563"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.8b00241"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.8b04950"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1007\/s12274-020-3031-2"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1021\/jp405430m"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsnano.5b06199"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201200994"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1038\/srep18276"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpcc.9b08923"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1039\/C9EE04192C"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.nanolett.7b05410"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-018-0054-3"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr040679f"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1021\/cr040682z"},{"key":"e_1_2_7_29_1","first-page":"355","volume-title":"Ozonation in Organic Chemistry V2: Nonolefinic Compounds","author":"Bailey P. 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