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Here we report on the dark\u2010field microscopic (DFM) imaging approach to in situ monitor the guest\u2010induced deformation evolution of individual COF\u2010300 crystals in real time. We observe not only transient and nonequilibrium intermediate deformation states but also local surface curvature\u2010driven diverse adsorption behaviours of single COF\u2010300 particles for dichloromethane (DCM), undergoing one, two, and multiple expansion\u2010contraction deformations as well as contraction\u2010to\u2010expansion transition. The surface curvature\u2010dominated deformations are ascribed to the significant differences in the adsorption capacity for DCM at the curved tip and flat side regions, in which DCM can be adsorbed preferentially by curved tip regions of COF\u2010300.<\/jats:p>","DOI":"10.1002\/anie.202214569","type":"journal-article","created":{"date-parts":[[2022,12,7]],"date-time":"2022-12-07T20:35:41Z","timestamp":1670445341000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":11,"title":["Surface Curvature Dominated Guest\u2010Induced Nonequilibrium Deformations of Single Covalent Organic Framework\u2010300 Particles"],"prefix":"10.1002","volume":"62","author":[{"given":"Guihua","family":"Zhang","sequence":"first","affiliation":[{"name":"National Collaborative Innovation Center for Nuclear Waste and Environmental Safety School of National Defence Science &amp; Technology Southwest University of Science and Technology  Mianyang 621010 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xinyi","family":"Zou","sequence":"additional","affiliation":[{"name":"National Collaborative Innovation Center for Nuclear Waste and Environmental Safety School of National Defence Science &amp; Technology Southwest University of Science and Technology  Mianyang 621010 P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qianxi","family":"Wang","sequence":"additional","affiliation":[{"name":"National Collaborative Innovation Center for Nuclear Waste and Environmental Safety School of National Defence Science &amp; Technology Southwest University of Science and Technology  Mianyang 621010 P. R. 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