%0 Journal Article %T Role of molecular damage in crack initiation mechanisms of tough elastomers %+ Sciences et Ingénierie de la Matière Molle (UMR 7615) (SIMM) %+ Laboratoire Charles Coulomb (L2C) %+ Axe Matière Molle & Verres (MMV) %+ Cornell University [Ithaca] (CU) %A Ju, Jianzhu %A Sanoja, Gabriel %A Cipelletti, Luca %A Ciccotti, Matteo %A Zhu, Bangguo %A Narita, Tetsuharu %A Yuen Hui, Chung %A Creton, Costantino %Z This work was financially supported by The European Union’s Horizon 2020 Programme for Research and Innovation under Marie Skłodowska-Curie grant agreement no. 765811 (DoDyNet) ERC Grant agreement AdG no. 695351 (CHEMECH) ANR MultiNet (grant no. ANR-20-CE06-0028-01) NSF under Grant No. CMMI-1903308. %< avec comité de lecture %@ 0027-8424 %J Proceedings of the National Academy of Sciences of the United States of America %I National Academy of Sciences %V 121 %N 45 %P e2410515121 %8 2024-10-30 %D 2024 %R 10.1073/pnas.2410515121 %K elastomers | mechanochemistry | digital image correlation | damage | fracture %Z Physics [physics] %Z Engineering Sciences [physics]Journal articles %X 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. %G English %2 https://hal.science/hal-04800400v1/document %2 https://hal.science/hal-04800400v1/file/2024%20Ju%20PNAS.pdf %L hal-04800400 %U https://hal.science/hal-04800400 %~ ESPCI %~ CNRS %~ L2C %~ SIMM %~ INC-CNRS %~ PSL %~ UNIV-MONTPELLIER %~ SORBONNE-UNIVERSITE %~ SORBONNE-UNIV %~ SU-SCIENCES %~ ESPCI-PSL %~ SU-TI %~ ALLIANCE-SU %~ UM-2015-2021 %~ UM-EPE %~ CHIMIE-SU %~ SUPRA_PHYS_CHIMIE