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Natl. Acad. Sci. U.S.A."],"published-print":{"date-parts":[[2024,11,5]]},"abstract":"<jats:p>Tough soft materials such as multiple network elastomers (MNE) or filled elastomers are typically stretchable and include significant energy dissipation mechanisms that prevent or delay crack growth. Yet most studies and fracture models focus on steady-state propagation and damage is assumed to be decoupled from the local stress and strain fields near the crack tip. We report an in situ spatial-temporally resolved 3D measurement of molecular damage in mechanophore-labeled MNE just before a crack propagates. This technique, complemented by digital image correlation, allows us to compare the spatial distribution of both damage and deformation in single network (SN) elastomers and in MNE. Compared to SN, MNE have a wide-spread damage in front of the crack and, surprisingly, delocalize strain concentration. A continuum model, where damage distribution is fully coupled to the crack tip fields, is proposed to explain these results. Additional measurements of time-dependent molecular damage during fixed grips relaxation in the presence of a crack reveal that the less localized damage distribution delays fracture initiation. The observations and exploratory modeling reveal the dynamic fracture mechanism of MNE, providing guidance for rational design of high-performance tough elastomers.<\/jats:p>","DOI":"10.1073\/pnas.2410515121","type":"journal-article","created":{"date-parts":[[2024,10,30]],"date-time":"2024-10-30T14:02:39Z","timestamp":1730296959000},"update-policy":"https:\/\/doi.org\/10.1073\/pnas.cm10313","source":"Crossref","is-referenced-by-count":27,"title":["Role of molecular damage in crack initiation mechanisms of tough elastomers"],"prefix":"10.1073","volume":"121","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2933-3787","authenticated-orcid":false,"given":"Jianzhu","family":"Ju","sequence":"first","affiliation":[{"name":"Sciences et Ing\u00e9nierie de la Mati\u00e8re Molle, CNRS UMR 7615, \u00c9cole sup\u00e9rieure de physique et de chimie industrielles de la Ville de Paris, Sorbonne Universit\u00e9, Paris Sciences et Lettres Universit\u00e9, Paris 75005, France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5477-2346","authenticated-orcid":false,"given":"Gabriel E.","family":"Sanoja","sequence":"additional","affiliation":[{"name":"Sciences et Ing\u00e9nierie de la Mati\u00e8re Molle, CNRS UMR 7615, \u00c9cole sup\u00e9rieure de physique et de chimie industrielles de la Ville de Paris, Sorbonne Universit\u00e9, Paris Sciences et Lettres Universit\u00e9, Paris 75005, France"},{"name":"McKetta Department of Chemical Engineering, The University of Texas at Austin, Austin, TX 78723"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2956-7580","authenticated-orcid":false,"given":"Luca","family":"Cipelletti","sequence":"additional","affiliation":[{"name":"Laboratoire Charles Coulomb (L2C), University of Montpellier, CNRS, Montpellier 34095, France"},{"name":"Institut Universitaire de France, Paris 75005, France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Matteo","family":"Ciccotti","sequence":"additional","affiliation":[{"name":"Sciences et Ing\u00e9nierie de la Mati\u00e8re Molle, CNRS UMR 7615, \u00c9cole sup\u00e9rieure de physique et de chimie industrielles de la Ville de Paris, Sorbonne Universit\u00e9, Paris Sciences et Lettres Universit\u00e9, Paris 75005, France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0549-8114","authenticated-orcid":false,"given":"Bangguo","family":"Zhu","sequence":"additional","affiliation":[{"name":"Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, NY 14853"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tetsuharu","family":"Narita","sequence":"additional","affiliation":[{"name":"Sciences et Ing\u00e9nierie de la Mati\u00e8re Molle, CNRS UMR 7615, \u00c9cole sup\u00e9rieure de physique et de chimie industrielles de la Ville de Paris, Sorbonne Universit\u00e9, Paris Sciences et Lettres Universit\u00e9, Paris 75005, France"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chung","family":"Yuen Hui","sequence":"additional","affiliation":[{"name":"Sibley School of Mechanical and Aerospace Engineering, Cornell University, Ithaca, NY 14853"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0177-9680","authenticated-orcid":false,"given":"Costantino","family":"Creton","sequence":"additional","affiliation":[{"name":"Sciences et Ing\u00e9nierie de la Mati\u00e8re Molle, CNRS UMR 7615, \u00c9cole sup\u00e9rieure de physique et de chimie industrielles de la Ville de Paris, Sorbonne Universit\u00e9, Paris Sciences et Lettres Universit\u00e9, Paris 75005, France"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"341","published-online":{"date-parts":[[2024,10,30]]},"reference":[{"key":"e_1_3_4_1_2","doi-asserted-by":"publisher","DOI":"10.1039\/b924290b"},{"key":"e_1_3_4_2_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.1248494"},{"key":"e_1_3_4_3_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2116127119"},{"key":"e_1_3_4_4_2","doi-asserted-by":"publisher","DOI":"10.1126\/sciadv.abg9410"},{"key":"e_1_3_4_5_2","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.1807750115"},{"key":"e_1_3_4_6_2","doi-asserted-by":"publisher","DOI":"10.1021\/acs.macromol.1c01214"},{"key":"e_1_3_4_7_2","doi-asserted-by":"publisher","DOI":"10.1038\/nature11409"},{"key":"e_1_3_4_8_2","article-title":"Designing toughness and strength for soft materials","author":"Zhao X.","year":"2017","unstructured":"X. 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