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Herein, we demonstrate SCSC transformation driven by the intrinsic NIR photothermal effect of a rationally designed croconium derivative CR\u2010DPA\u2010OMe, which features strong NIR absorption and a high photothermal conversion efficiency of 60%. Solvated CR\u2010DPA\u2010OMe single crystals encapsulating CHCl\n                    <jats:sub>3<\/jats:sub>\n                    molecules exhibit exceptional ambient stability with crystallinity preserved for over two years. Benefiting from the robust dimeric packing of croconium motifs and the conformationally flexible methoxy\u2010substituted diphenylamine moieties, the resulting crystals successfully reconcile long\u2010range lattice order with structural flexibility, thus enabling efficient SCSC transformation upon NIR photothermal stimulation. Combined density functional theory (DFT) calculations and in situ single\u2010crystal x\u2010ray diffraction analysis confirm that the transformation is driven by the synergistic interplay of photoinduced molecular conformational reorganization and photothermally\u2010converted\u00a0heat, affording markedly faster transformation than conventional oven heating. Furthermore, tailored NIR irradiation enables spatiotemporally programmable guest release, demonstrating a remote manipulation inaccessible via macroscopic conductive heating. These findings highlight the substantial promise of NIR photothermal modulation as an emerging stimuli\u2010responsive strategy for precise structural engineering in molecular crystals, opening new avenues toward tailored functional material applications.\n                  <\/jats:p>","DOI":"10.1002\/anie.3462526","type":"journal-article","created":{"date-parts":[[2026,10,15]],"date-time":"2026-10-15T04:35:26Z","timestamp":1792038926000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Intrinsic Near\u2010Infrared Photothermal Effect Induces Single\u2010Crystal\u2010to\u2010Single\u2010Crystal Transformation in Organic Molecular Crystals"],"prefix":"10.1002","author":[{"given":"Liming","family":"Yang","sequence":"first","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Binjie","family":"Chen","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Rushuai","family":"Deng","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiangwei","family":"Kong","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yunze","family":"Huang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Mingxing","family":"Chen","sequence":"additional","affiliation":[{"name":"Analytical Instrumentation Center of Peking University Peking University  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1678-2823","authenticated-orcid":false,"given":"Xinggui","family":"Gu","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering College of Materials Science and Engineering Beijing University of Chemical Technology  Beijing P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,10,14]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566\u2010022\u201000957\u20105"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.2c00818"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41565\u2010025\u201001882\u20108"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41586\u2010025\u201008833\u20102"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563\u2010025\u201002411\u20107"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c12874"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c12153"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.adr0936"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202516540"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.4c01331"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202411880"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202204141"},{"key":"e_1_2_8_14_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.0c09732"},{"key":"e_1_2_8_15_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202500151"},{"key":"e_1_2_8_16_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2023.01.013"},{"key":"e_1_2_8_17_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202418570"},{"key":"e_1_2_8_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c01145"},{"key":"e_1_2_8_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.9345668"},{"key":"e_1_2_8_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.5c21191"},{"key":"e_1_2_8_21_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201069516\u20108"},{"key":"e_1_2_8_22_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202212290"},{"key":"e_1_2_8_23_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202511365"},{"key":"e_1_2_8_24_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41566\u2010026\u201001912\u20104"},{"key":"e_1_2_8_25_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202416160"},{"key":"e_1_2_8_26_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202215372"},{"key":"e_1_2_8_27_1","doi-asserted-by":"publisher","DOI":"10.1002\/agt2.680"},{"key":"e_1_2_8_28_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202402726"},{"key":"e_1_2_8_29_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202508821"},{"key":"e_1_2_8_30_1","doi-asserted-by":"publisher","DOI":"10.1039\/d5cs00843c"},{"key":"e_1_2_8_31_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202508314"},{"key":"e_1_2_8_32_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010022\u201031481\u20103"},{"key":"e_1_2_8_33_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010023\u201037086\u20108"},{"key":"e_1_2_8_34_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202512603"},{"key":"e_1_2_8_35_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c03588"},{"key":"e_1_2_8_36_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.5856537"},{"key":"e_1_2_8_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/adfm.202305916"},{"key":"e_1_2_8_38_1","doi-asserted-by":"publisher","DOI":"10.1007\/s40820\u2010025\u201001996\u20107"},{"key":"e_1_2_8_39_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010023\u201039162\u20105"},{"key":"e_1_2_8_40_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.ccr.2022.214865"},{"key":"e_1_2_8_41_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202409041"},{"key":"e_1_2_8_42_1","doi-asserted-by":"publisher","DOI":"10.1002\/agt2.91"},{"key":"e_1_2_8_43_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja038741y"},{"key":"e_1_2_8_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202303057"},{"key":"e_1_2_8_45_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467\u2010026\u201073177\u2010y"},{"key":"e_1_2_8_46_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.9215288"},{"key":"e_1_2_8_47_1","unstructured":"Deposition 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These data are provided free of charge by the joint Cambridge Crystallographic Data Centre and Fachinformationszentrum Karlsruhe Access Structures service."},{"key":"e_1_2_8_48_1","unstructured":"Gaussian 16 Revision C.01 M. J.Frisch G. W.Trucks H. B.Schlegel et\u00a0al. 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