- Access by Xinjiang University
Control of phase transition patterning in the wake of reaction fronts
Phys. Rev. E 114, 044218 – Published 22 October, 2026
DOI: https://doi.org/10.1103/5v7k-w2k3
Abstract
When two initially separated reactants A and B are put in contact, a chemical front can develop if a bimolecular reaction interplays with diffusion. In the case of a precipitation reaction, a phase transition may occur in the wake of this reaction front provided that the concentration of C is larger than a critical threshold. We analyze the scalings of resulting phase transition patterns in both one-dimensional (1D) and two-dimensional (2D) rectilinear and radial geometries by numerical simulation of the Cahn-Hilliard equation with a reactive source term, solution of reaction-diffusion-advection equations for the concentrations of A and B. We find that the temporal and spatial scalings of the precipitate patterns depend on the properties of the fronts and can be controlled by the injection flow rate . In particular, we show that the Matalon-Packter law classically used to characterize Liesegang patterns in one-dimensional rectilinear reaction-diffusion systems can be generalized to 1D radial geometry with injection. We discuss the further generalization of pattern selection between stripes and spotted patterns in 2D systems.
Physics Subject Headings (PhySH)
Article Text
References (38)
- M. C. Cross and P. C. Hohenberg, Pattern formation outside of equilibrium, Rev. Mod. Phys. 65, 851 (1993).
- G. Schuszter, F. Brau, and A. De Wit, Calcium carbonate mineralization in a confined geometry, Environ. Sci. Technol. Lett. 3, 156 (2016).
- P. Damacet and K. A. Mirica, Periodic patterning of matter in non-equilibrium Liesegang-type structures, Angew. Chem. Int. Ed. 64, e202425292 (2025).
- F. Haudin, J. H. E. Cartwright, F. Brau, and A. De Wit, Spiral precipitation patterns in confined chemical gardens, Proc. Natl. Acad. Sci. USA 111, 17363 (2014).
- M. Itatani, Q. Fang, K. Unoura, and H. Nabika, Programmable design of self-organized patterns through a precipitation reaction, J. Phys. Chem. B 124, 8402 (2020).
- Q. Wang and E. Nakouzi, Reaction-diffusion coupling facilitates the sequential precipitation of metal ions from battery feedstock solutions, Environ. Sci. Technol. Lett. 10, 1188 (2023).
- B. Bohner, G. Schuszter, O. Berkesi, D. Horváth, and A. Tóth, Self-organization of calcium oxalate by flow-driven precipitation, Chem. Commun. 50, 4289 (2014).
- I. Ziemecka, S. Gokalp, S. Stroobants, F. Brau, D. Maes, and A. De Wit, Polymorph selection of ROY by flow-driven crystallization, Crystals 9, 351 (2019).
- B. A. Grzybowski and C. J. Campbell, Fabrication using programmed reactions, Mater. Today 10, 38 (2007).
- P. Knoll, E. Nakouzi, and O. Steinbock, Mesoscopic reaction-diffusion fronts control biomorph growth, J. Phys. Chem. 121, 26133 (2017).
- B. Bohner, G. Schuszter, D. Horváth, and A. Tóth, Morphology control by flow-driven self-organizing precipitation, Chem. Phys. Lett. 631–632, 114 (2015).
- G. Schuszter and A. De Wit, Comparison of flow-controlled calcium and barium carbonate precipitation patterns, J. Chem. Phys. 145, 224201 (2016).
- G. Facchini, M. A. Budroni, G. Schuszter, F. Brau, and A. De Wit, Phyllotactic structures in radially growing spatial symmetry breaking systems, Phys. Rev. Lett. 135, 018001 (2025).
- E. Balog, P. Papp, A. Tóth, D. Horváth, and G. Schuszter, The impact of reaction rate on the formation of flow-driven confined precipitate patterns, Phys. Chem. Chem. Phys. 22, 13390 (2020).
- Y. Nagatsu, Y. Ishii, Y. Tada, and A. De Wit, Hydrodynamic fingering instability induced by a precipitation reaction, Phys. Rev. Lett. 113, 024502 (2014).
- E. Balog, K. Bittmann, K. Schwarzenberger, K. Eckert, A. De Wit, and G. Schuszter, Influence of microscopic precipitate structures on macroscopic pattern formation in reactive flows in a confined geometry, Phys. Chem. Chem. Phys. 21, 2910 (2019).
- L. Gálfi and Z. Rácz, Properties of the reaction front in an type reaction-diffusion process, Phys. Rev. A 38, 3151 (1988).
- F. Brau, G. Schuszter, and A. De Wit, Flow control of fronts by radial injection, Phys. Rev. Lett. 118, 134101 (2017).
- Y. Stergiou, D. M. Escala, P. Papp, D. Horváth, M. J. B. Hauser, F. Brau, A. De Wit, A. Tóth, K. Eckert, and K. Schwarzenberger, Unraveling dispersion and buoyancy dynamics around radial reaction fronts: Microgravity experiments and numerical simulations, npj Microgravity 10, 53 (2024).
- Y. Stergiou, M. J. B. Hauser, A. Comolli, F. Brau, A. De Wit, G. Schuszter, P. Papp, D. Horváth, C. Roux, V. Pimienta, K. Eckert, and K. Schwarzenberger, Effects of gravity modulation on the dynamics of a radial reaction front, Chem. Eng. Sci. 257, 117703 (2022).
- R. Matalon and A. Packter, The Liesegang phenomenon. I. Sol protection and diffusion, J. Colloid Sci. 10, 46 (1955).
- S. K. Smoukov, A. Bitner, C. J. Campbell, K. Kandere-Grzybowska, and B. A. Grzybowski, Nano- and microscopic surface wrinkles of linearly increasing heights prepared by periodic precipitation, J. Am. Chem. Soc. 127, 17803 (2005).
- A. Sahu, B. B. Kanrar, and D. Panda, Evolution of micron-spaced patterns within precipitating patterns of in situ synthesized silver nanoparticles in a nanodot-embedded PVA/PVP film, Langmuir 37, 4460 (2021).
- H. Nabika, M. Itatani, and I. Lagzi, Pattern formation in precipitation reactions: The Liesegang phenomenon, Langmuir 36, 481 (2020).
- T. Antal, M. Droz, J. Magnin, and Z. Rácz, Formation of Liesegang patterns: A spinodal decomposition scenario, Phys. Rev. Lett. 83, 2880 (1999).
- I. Lagzi, A. Volford, and A. Büki, Effect of geometry on the time law of Liesegang patterning, Chem. Phys. Lett. 396, 97 (2004).
- M. Dayeh, M. Ammar, and M. Al-Ghoul, Transition from rings to spots in a precipitation reaction-diffusion system, RSC Adv. 4, 60034 (2014).
- F. Izsák and I. Lagzi, A new universal law for the Liesegang pattern formation, J. Chem. Phys. 122, 184707 (2005).
- P. Papp, B. Bohner, A. Tóth, and D. Horváth, Fine tuning of pattern selection in the cadmium-hydroxyde system, J. Chem. Phys. 152, 094906 (2020).
- H. Wu, A review on the Cahn-Hilliard equation: Classical results and recent advances in dynamic boundary conditions, Electron. Res. Arch. 30, 2788 (2022).
- F. Brau and A. De Wit, Influence of rectilinear vs radial advection on the yield of reaction fronts: A comparison, J. Chem. Phys. 152, 054716 (2020).
- W. van Saarloos, Front propagation into unstable states, Phys. Rep. 386, 29 (2003).
- S. M. Tuur, A. M. Nelson, D. W. Gibson, R. C. Neafie, F. B. Johnson, F. K. Mostofi, and D. H. Connor, Liesegang rings in tissue. How to distinguish Liesegang rings from the giant kidney worm, dioctophyma renale, Am. J. Surg. Pathol. 11, 598 (1987).
- T. S. Babicheva, A. A. Konduktorova, S. L. Shmakov, and A. B. Shipovskaya, Formation of Liesegang structures under the conditions of the spatiotemporal reaction of polymer-analogous transformation (salt-base) of chitosan, J. Phys. Chem. B 124, 9255 (2020).
- R. M. Walliser, F. Boudoire, E. Orosz, R. Tóth, A. Braun, E. C. Constable, Z. Rácz, and I. Lagzi, Growth of nanoparticles and microparticles by controlled reaction-diffusion processes, Langmuir 31, 1828 (2015).
- C. Campbell, E. Baker, M. Fialkowski, and B. Grzybowski, Arrays of microlenses of complex shapes prepared by reaction-diffusion in thin films of ionically doped gels, Appl. Phys. Lett. 85, 1871 (2004).
- U. Thiele, T. Frohoff-Hülsmann, S. Engelnkemper, E. Knobloch, and A. Archer, First order phase transitions and the thermodynamic limit, New J. Phys. 21, 123021 (2019).
- Z. Koza, The long-time behavior of initially separated A + 0 reaction-diffusion systems with arbitrary diffusion constants, J. Stat. Phys. 85, 179 (1996).