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However, it remains challenging for the high\u2010precision laser\u2010assisted photoetching of colloidal quantum dots (QDs). Here, we report a laser\u2010assisted atom\u2010by\u2010atom photoetching process that post\u2010synthetically enables the state\u2010of\u2010the\u2010art colloidal CdSe QDs. By deciphering the surface chemistry and ultrafast excitonic dynamics, we provide an atomic\u2010level activation\u2013coordination coupling mechanism in such exciton\u2010involved photochemical reactions. In situ spectroscopies further reveal the reaction kinetics as a four\u2010step size\u2010focusing process that is highly dependent on the laser wavelength. As such, by modulating the laser wavelength, which dictates the excitonic absorption threshold of final QDs, we are capable of retrosynthetically programming their sizes across a wide quantum\u2010confined regime, thereby achieving an ultrabroad color gamut. These findings offer a guideline for the laser\u2010assisted retrosynthesis of high\u2010quality quantum\u2010confined materials.<\/jats:p>","DOI":"10.1002\/anie.202517547","type":"journal-article","created":{"date-parts":[[2025,12,22]],"date-time":"2025-12-22T05:41:30Z","timestamp":1766382090000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Laser\u2010Induced Size\u2010Focusing Synthesis of High\u2010Quality Colloidal Quantum Dots"],"prefix":"10.1002","volume":"65","author":[{"given":"Yu\u2010Zhuo","family":"Zhang","sequence":"first","affiliation":[{"name":"New Cornerstone Science Laboratory Department of Chemistry Institute of Biomimetic Materials and Chemistry Anhui Engineering Laboratory of Biomimetic Materials Division of Nanomaterials and Chemistry Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of China  Hefei 230026 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