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Here, we show that early collagen remodeling is first expressed as a loss of supramolecular chirality coherence, rather than a reduction in collagen density or network integrity. By correlating molecular-scale chiral order with mesoscale fibrillar organization across three independent adult skin sample donors (Samples 1\u20133, referred to as S1\u2013S3), we identify an abrupt collapse of chirality coherence despite preserved collagen mass and coverage. Only at some stages do fibrillar fragmentation and directional reorganization become apparent, accompanied by a reduction in nonlinear optical response. These findings establish supramolecular chirality coherence as an early-failing order parameter in collagen assemblies and reveal a previously unrecognized precursor to dermal remodeling. More broadly, this work provides a framework for detecting incipient failure in hierarchical chiral biomaterials before macroscopic degradation becomes evident.<\/jats:p>","DOI":"10.1021\/acsnano.6c06602","type":"journal-article","created":{"date-parts":[[2026,7,16]],"date-time":"2026-07-16T04:01:04Z","timestamp":1784174464000},"page":"20747-20760","source":"Crossref","is-referenced-by-count":0,"title":["Correlative Multimodal\nFramework Reveals Supramolecular\nChirality Loss Preceding Fibrillar Rarefaction in Dermal Collagen"],"prefix":"10.1021","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0009-0000-0971-2424","authenticated-orcid":true,"given":"Ali","family":"Haider","sequence":"first","affiliation":[{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8531"]},{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-7579-0935","authenticated-orcid":true,"given":"Yusuke","family":"Kochi","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8531"]},{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Andrew K.","family":"Schulz","sequence":"additional","affiliation":[{"name":"Max Planck Institute for Intelligent Systems , ,","place":["Stuttgart, Germany, 70569"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kuya","family":"Aoyama","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Hiroshima, Japan, 739-0046"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0984-4280","authenticated-orcid":true,"given":"Aiko","family":"Sada","sequence":"additional","affiliation":[{"name":"Kyushu University , , ,","place":["Fukuoka, Japan, 819-0395"]},{"name":"Kumamoto University , , ,","place":["Kumamoto, Japan, 860-0811"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hisako","family":"Sato","sequence":"additional","affiliation":[{"name":"Ehime University , , 2-5, Bunkyo-cho , ,","place":["Matsuyama, Japan, 790-8577"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1173-5163","authenticated-orcid":true,"given":"Elisabetta","family":"Matsumoto","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8531"]},{"name":"Georgia Institute of Technology , , , ,","place":["Atlanta, Georgia, United States, 30332"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4989-5688","authenticated-orcid":true,"given":"Malcolm","family":"Kadodwala","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8531"]},{"name":"University of Glasgow , , ,","place":["Glasgow, U.K., G12 8QQ"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8166-544X","authenticated-orcid":true,"given":"Koichi","family":"Matsuo","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8531"]},{"name":"Hiroshima University , , ,","place":["Hiroshima, Japan, 739-0046"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5542-3700","authenticated-orcid":true,"given":"Katsuya","family":"Inoue","sequence":"additional","affiliation":[{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8531"]},{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8526"]},{"name":"Hiroshima University , , ,","place":["Higashihiroshima, Japan, 739-8526"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,16]]},"reference":[{"issue":"1","key":"2026072810080100000_cit2","doi-asserted-by":"publisher","first-page":"139","DOI":"10.1016\/j.jmbbm.2011.08.016","article-title":"Characterization of the anisotropic mechanical properties\nof excised human skin","volume":"5","author":"Annaidh","year":"2012","journal-title":"J. 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Opt."},{"issue":"106","key":"2026072810080100000_cit25","doi-asserted-by":"publisher","first-page":"87180","DOI":"10.1039\/C5RA14423J","article-title":"A new collagen\nsolution with high concentration and collagen native structure perfectly\npreserved","volume":"5","author":"Qi","year":"2015","journal-title":"RSC Adv."},{"issue":"1","key":"2026072810080100000_cit26","doi-asserted-by":"publisher","first-page":"39","DOI":"10.1039\/B316168B","article-title":"Synchrotron radiation\ncircular dichroism spectroscopy\nof proteins and applications in structural and functional genomics","volume":"35","author":"Miles","year":"2006","journal-title":"Chem. Soc. Rev."},{"key":"2026072810080100000_cit27","doi-asserted-by":"publisher","first-page":"1023","DOI":"10.1016\/j.elspec.2005.01.102","article-title":"Vacuum-ultraviolet\ncircular dichroism spectrophotometer using synchrotron\nradiation","volume":"144","author":"Matsuo","year":"2005","journal-title":"J. Electron Spectrosc. Relat. Phenom."},{"issue":"12","key":"2026072810080100000_cit28","doi-asserted-by":"publisher","first-page":"1765","DOI":"10.1002\/pro.2558","article-title":"Distinct circular\ndichroism spectroscopic signatures of polyproline II and unordered\nsecondary structures: applications in secondary structure analyses","volume":"23","author":"Lopes","year":"2014","journal-title":"Protein Sci."},{"issue":"12","key":"2026072810080100000_cit29","doi-asserted-by":"publisher","first-page":"2100","DOI":"10.1016\/j.jmb.2013.03.018","article-title":"Polyproline-II helix in proteins:\nstructure and function","volume":"425","author":"Adzhubei","year":"2013","journal-title":"J. Mol. Biol."},{"issue":"1","key":"2026072810080100000_cit30","doi-asserted-by":"publisher","first-page":"19","DOI":"10.1186\/s42825-020-00033-0","article-title":"Factors affecting thermal stability\nof collagen from the aspects of extraction, processing and modification","volume":"2","author":"Zhang","year":"2020","journal-title":"J. Leather Sci. Eng."},{"issue":"1","key":"2026072810080100000_cit31","doi-asserted-by":"publisher","first-page":"74","DOI":"10.1110\/ps.051779806","article-title":"Stereoelectronic\neffects on polyproline conformation","volume":"15","author":"Horng","year":"2006","journal-title":"Protein\nSci."},{"issue":"3","key":"2026072810080100000_cit32","doi-asserted-by":"publisher","first-page":"405","DOI":"10.1093\/jb\/mvh048","article-title":"Secondary-structure analysis of proteins\nby vacuum-ultraviolet circular dichroism spectroscopy","volume":"135","author":"Matsuo","year":"2004","journal-title":"J. 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Rev."},{"issue":"3","key":"2026072810080100000_cit40","doi-asserted-by":"publisher","first-page":"155","DOI":"10.1002\/bip.21719","article-title":"Structural\nproperties of DNA oligomers containing (GACX)n\nand (GAXC)n tandem repeats","volume":"97","author":"Dasgupta","year":"2012","journal-title":"Biopolymers."},{"key":"2026072810080100000_cit41","first-page":"37","article-title":"Circular\ndichroism and conformation of unordered peptides","volume":"2","author":"Woody","year":"1992","journal-title":"Adv. Biophys. 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Biol."},{"key":"2026072810080100000_cit51","doi-asserted-by":"publisher","first-page":"266","DOI":"10.1016\/j.actbio.2024.07.026","article-title":"Second\nharmonic generation microscopy,\nbiaxial mechanical tests and fiber dispersion models in human skin\nbiomechanics","volume":"185","author":"Alberini","year":"2024","journal-title":"Acta Biomater."},{"issue":"8","key":"2026072810080100000_cit52","doi-asserted-by":"publisher","first-page":"899","DOI":"10.1111\/exd.13560","article-title":"Texture analysis of second-harmonic-generation\nimages for quantitative\nanalysis of reticular dermal collagen fibre in vivo in human facial\ncheek skin","volume":"28","author":"Ogura","year":"2019","journal-title":"Exp. 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