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However, directly tracking the nanoscale carrier dynamics of a single photocatalyst crystal under the reaction conditions is essential but remains challenging. Here, we employed in situ transient reflection microscopy to spatiotemporally resolve the evolution of photogenerated carriers in facet-engineered bismuth vanadate (BiVO4) photocatalyst. It is revealed that photogenerated holes undergo three sequential steps: initial ultrafast charge separation (\u223c5\u00a0ps), hole trapping (\u223c1.5\u00a0ns) and trap states-mediated interfacial transfer to pre-adsorbed H2O on the surface (\u223c19\u00a0ps). Crucially, trap states associated with oxygen lattice sites act as nanoscale relay sites that enable rapid hole injection into pre-adsorbed H2O, whereas direct valence-band hole injection is negligible. These findings provide a comprehensive mechanistic picture of photogenerated carrier dynamics across the entire photocatalytic process, directly linking nanostructure to interfacial chemistry and revealing trap states as critical mediators of efficient interfacial charge transfer.<\/jats:p>","DOI":"10.1093\/nsr\/nwag379","type":"journal-article","created":{"date-parts":[[2026,6,17]],"date-time":"2026-06-17T11:16:40Z","timestamp":1781695000000},"source":"Crossref","is-referenced-by-count":0,"title":["Unraveling the evolution of photogenerated holes from charge separation to interfacial transfer in photocatalysis"],"prefix":"10.1093","volume":"13","author":[{"given":"Fengke","family":"Sun","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 ,","place":["China"]},{"name":"University of Chinese Academy of Sciences , Beijing 100049 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yue","family":"Zhao","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xianchang","family":"Yan","sequence":"additional","affiliation":[{"name":"ZJU-Hangzhou Global Scientific and Technological Innovation Center, Zhejiang University , Hangzhou 311200 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Panwang","family":"Zhou","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Can","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rengui","family":"Li","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), Dalian Institute of Chemical Physics, Chinese Academy of Sciences , Dalian 116023 ,","place":["China"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shengye","family":"Jin","sequence":"additional","affiliation":[{"name":"State Key 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