Reuse & Permissions

It is not necessary to obtain permission to reuse this article or its components as it is available under the terms of the Creative Commons Attribution 4.0 International license. This license permits unrestricted use, distribution, and reproduction in any medium, provided attribution to the author(s) and the published article's title, journal citation, and DOI are maintained. Please note that some figures may have been included with permission from other third parties. It is your responsibility to obtain the proper permission from the rights holder directly for these figures.

Export citation

Export citation

Choose format for download:

Download Citation
  • Open Access

Motility-Induced Crystallization and Rotating Crystallites

Max Philipp Holl1,2,3,*,†, Alina Barbara Steinberg3,*,‡, Michael te Vrugt4,§, and Uwe Thiele3,5,║

  • 1Department of Chemistry and Materials Science, Aalto University, P.O. Box 16100, FI-00076 Aalto, Espoo 00076, Finland
  • 2Academy of Finland Center of Excellence in Life-Inspired Hybrid Materials (LIBER), Aalto University, P.O. Box 16100, FI-00076 Aalto, Espoo 00076, Finland
  • 3Institute of Theoretical Physics, University of Münster, Wilhelm-Klemm-Strasse 9, 48149 Münster, Germany
  • 4Institute of Physics, Johannes Gutenberg University Mainz, 55128 Mainz, Germany
  • 5Center for Nonlinear Science (CeNoS), University of Münster, Corrensstrasse 2, 48149 Münster, Germany

  • *These authors contributed equally to this work.
  • †Contact author: max.holl@aalto.fi
  • ‡Contact author: a_stei52@uni-muenster.de
  • §Contact author: tevrugtm@uni-mainz.de
  • ║Contact author: u.thiele@uni-muenster.de; www.uwethiele.de

Phys. Rev. Lett. 135, 158301 – Published 6 October, 2025

DOI: https://doi.org/10.1103/m3dy-53yc

Abstract

Active soft matter frequently shows motility-induced phase separation, where self-propelled particles condensate into clusters with an inner liquidlike structure. Such activity may also result in motility-induced crystallization into clusters with an inner crystalline structure. We derive a higher-order active phase-field-crystal model and employ it to study the interplay of passive (i.e., thermodynamic) and active (i.e., motility-induced) condensation or evaporation and crystallization or melting. Stability and morphological phase diagrams indicate the various occurring phase coexistences and transitions, e.g., the destruction of passive clusters in the case of a density-independent effective velocity and the possible creation of active clusters in the case of a density-dependent effective velocity. Finally, simple and complex rotating crystallites are discussed, including states of time-periodic chirality.

View figure in article

Physics Subject Headings (PhySH)

Article Text

Supplemental Material

References (90)

  1. S. Ramaswamy, The mechanics and statistics of active matter, Annu. Rev. Condens. Matter Phys. 1, 323 (2010).
  2. P. Romanczuk, M. Bär, W. Ebeling, B. Lindner, and L. Schimansky-Geier, Active Brownian particles from individual to collective stochastic dynamics, Eur. Phys. J. Spec. Top. 202, 1 (2012).
  3. M. C. Marchetti, J. F. Joanny, S. Ramaswamy, T. B. Liverpool, J. Prost, M. Rao, and R. A. Simha, Hydrodynamics of soft active matter, Rev. Mod. Phys. 85, 1143 (2013).
  4. M. E. Cates and J. Tailleur, Motility-induced phase separation, Annu. Rev. Condens. Matter Phys. 6, 219 (2015).
  5. D. Marenduzzo, An introduction to the statistical physics of active matter: Motility-induced phase separation and the “generic instability” of active gels, Eur. Phys. J. Spec. Top. 225, 2065 (2016).
  6. G. Gompper et al., The 2020 motile active matter roadmap, J. Phys. Condens. Matter 32, 193001 (2020).
  7. M. R. Shaebani, A. Wysocki, R. G. Winkler, G. Gompper, and H. Rieger, Computational models for active matter, Nat. Rev. Phys. 2, 181 (2020).
  8. I. Buttinoni, J. Bialké, F. Kümmel, H. Löwen, C. Bechinger, and T. Speck, Dynamical clustering and phase separation in suspensions of self-propelled colloidal particles, Phys. Rev. Lett. 110, 238301 (2013).
  9. C. Bechinger, R. Di Leonardo, H. Löwen, C. Reichhardt, G. Volpe, and G. Volpe, Active particles in complex and crowded environments, Rev. Mod. Phys. 88, 045006 (2016).
  10. A. A. Fragkopoulos, J. Vachier, J. Frey, F.-M. Le Menn, M. G. Mazza, M. Wilczek, D. Zwicker, and O. Bäumchen, Self-generated oxygen gradients control collective aggregation of photosynthetic microbes, J. R. Soc. Interface 18, 20210553 (2021).
  11. F. D. C. Farrell, M. C. Marchetti, D. Marenduzzo, and J. Tailleur, Pattern formation in self-propelled particles with density-dependent motility, Phys. Rev. Lett. 108, 248101 (2012).
  12. B. M. Mognetti, A. Saric, S. Angioletti-Uberti, A. Cacciuto, C. Valeriani, and D. Frenkel, Living clusters and crystals from low-density suspensions of active colloids, Phys. Rev. Lett. 111, 245702 (2013).
  13. A. Patch, D. Yllanes, and M. C. Marchetti, Kinetics of motility-induced phase separation and swim pressure, Phys. Rev. E 95, 012601 (2017).
  14. E. Crosato, M. Prokopenko, and R. E. Spinney, Irreversibility and emergent structure in active matter, Phys. Rev. E 100, 042613 (2019).
  15. L. Caprini, U. Marini Bettolo Marconi, and A. Puglisi, Spontaneous velocity alignment in motility-induced phase separation, Phys. Rev. Lett. 124, 078001 (2020).
  16. F. Turci and N. B. Wilding, Phase separation and multibody effects in three-dimensional active Brownian particles, Phys. Rev. Lett. 126, 038002 (2021).
  17. A. K. Omar, K. Klymko, T. GrandPre, and P. L. Geissler, Phase diagram of active Brownian spheres: Crystallization and the metastability of motility-induced phase separation, Phys. Rev. Lett. 126, 188002 (2021).
  18. R. Wittkowski, A. Tiribocchi, J. Stenhammar, R. J. Allen, D. Marenduzzo, and M. E. Cates, Scalar ϕ4 field theory for active-particle phase separation, Nat. Commun. 5, 4351 (2014).
  19. T. Speck, J. Bialké, A. M. Menzel, and H. Löwen, Effective Cahn-Hilliard equation for the phase separation of active Brownian particles, Phys. Rev. Lett. 111, 218304 (2014).
  20. T. Speck, A. M. Menzel, J. Bialké, and H. Löwen, Dynamical mean-field theory and weakly non-linear analysis for the phase separation of active Brownian particles, J. Chem. Phys. 142, 224109 (2015).
  21. L. Rapp, F. Bergmann, and W. Zimmermann, Systematic extension of the Cahn-Hilliard model for motility-induced phase separation, Eur. Phys. J. E 42, 57 (2019).
  22. J. Bickmann and R. Wittkowski, Predictive local field theory for interacting active Brownian spheres in two spatial dimensions, J. Phys. Condens. Matter 32, 214001 (2020).
  23. J. Bickmann and R. Wittkowski, Collective dynamics of active Brownian particles in three spatial dimensions: A predictive field theory, Phys. Rev. Res. 2, 033241 (2020).
  24. A. J. Bray, Theory of phase-ordering kinetics, Adv. Phys. 43, 357 (1994).
  25. I. Theurkauff, C. Cottin-Bizonne, J. Palacci, C. Ybert, and L. Bocquet, Dynamic clustering in active colloidal suspensions with chemical signaling, Phys. Rev. Lett. 108, 268303 (2012).
  26. J. Palacci, S. Sacanna, A. P. Steinberg, D. J. Pine, and P. M. Chaikin, Living crystals of light-activated colloidal surfers, Science 339, 936 (2013).
  27. A. P. Petroff, X.-L. Wu, and A. Libchaber, Fast-moving bacteria self-organize into active two-dimensional crystals of rotating cells, Phys. Rev. Lett. 114, 158102 (2015).
  28. A. Zöttl and H. Stark, Emergent behavior in active colloids, J. Phys. Condens. Matter 28, 253001 (2016).
  29. A. P. Petroff and A. Libchaber, Nucleation of rotating crystals by Thiovulum majus bacteria, New J. Phys. 20, 015007 (2018).
  30. F. Ginot, I. Theurkauff, F. Detcheverry, C. Ybert, and C. Cottin-Bizonne, Aggregation-fragmentation and individual dynamics of active clusters, Nat. Commun. 9, 696 (2018).
  31. R. J. Hawkins and T. B. Liverpool, Stress reorganization and response in active solids, Phys. Rev. Lett. 113, 028102 (2014).
  32. C. Hernández-López, P. Baconnier, C. Coulais, O. Dauchot, and G. Düring, Model of active solids: Rigid body motion and shape-changing mechanisms, Phys. Rev. Lett. 132, 238303 (2024).
  33. E. Ferrante, A. E. Turgut, M. Dorigo, and C. Huepe, Elasticity-based mechanism for the collective motion of self-propelled particles with springlike interactions: A model system for natural and artificial swarms, Phys. Rev. Lett. 111, 268302 (2013).
  34. A. Maitra and S. Ramaswamy, Oriented active solids, Phys. Rev. Lett. 123, 238001 (2019).
  35. A. M. Menzel and H. Löwen, Traveling and resting crystals in active systems, Phys. Rev. Lett. 110, 055702 (2013).
  36. A. M. Menzel, T. Ohta, and H. Löwen, Active crystals and their stability, Phys. Rev. E 89, 022301 (2014).
  37. A. I. Chervanyov, H. Gomez, and U. Thiele, Effect of the orientational relaxation on the collective motion of patterns formed by self-propelled particles, Europhys. Lett. 115, 68001 (2016).
  38. F. Alaimo, S. Praetorius, and A. Voigt, A microscopic field theoretical approach for active systems, New J. Phys. 18, 083008 (2016).
  39. L. Ophaus, S. V. Gurevich, and U. Thiele, Resting and traveling localized states in an active phase-field-crystal model, Phys. Rev. E 98, 022608 (2018).
  40. S. Praetorius, A. Voigt, R. Wittkowski, and H. Löwen, Active crystals on a sphere, Phys. Rev. E 97, 052615 (2018).
  41. L. Ophaus, J. Kirchner, S. V. Gurevich, and U. Thiele, Phase-field-crystal description of active crystallites: Elastic and inelastic collisions, Chaos 30, 123149 (2020).
  42. L. Ophaus, E. Knobloch, S. V. Gurevich, and U. Thiele, Two-dimensional localized states in an active phase-field-crystal model, Phys. Rev. E 103, 032601 (2021).
  43. M. P. Holl, A. J. Archer, S. V. Gurevich, E. Knobloch, L. Ophaus, and U. Thiele, Localized states in passive and active phase-field-crystal models, IMA J. Appl. Math. 86, 896 (2021).
  44. K. R. Elder, M. Katakowski, M. Haataja, and M. Grant, Modeling elasticity in crystal growth, Phys. Rev. Lett. 88, 245701 (2002).
  45. H. Emmerich, H. Löwen, R. Wittkowski, T. Gruhn, G. I. Tóth, G. Tegze, and L. Gránásy, Phase-field-crystal models for condensed matter dynamics on atomic length and diffusive time scales: An overview, Adv. Phys. 61, 665 (2012).
  46. U. Thiele, A. J. Archer, M. J. Robbins, H. Gomez, and E. Knobloch, Localized states in the conserved Swift-Hohenberg equation with cubic nonlinearity, Phys. Rev. E 87, 042915 (2013).
  47. A. J. Archer, D. J. Ratliff, A. M. Rucklidge, and P. Subramanian, Deriving phase field crystal theory from dynamical density functional theory: Consequences of the approximations, Phys. Rev. E 100, 022140 (2019).
  48. M. te Vrugt, H. Löwen, and R. Wittkowski, Classical dynamical density functional theory: From fundamentals to applications, Adv. Phys. 69, 121 (2020).
  49. P. Subramanian, A. J. Archer, E. Knobloch, and A. M. Rucklidge, Spatially localized quasicrystalline structures, New J. Phys. 20, 122002 (2018).
  50. Z.-L. Wang, Z. Liu, Z.-F. Huang, and W. Duan, Minimal phase-field crystal modeling of vapor-liquid-solid coexistence and transitions, Phys. Rev. Mater. 4, 103802 (2020).
  51. J. Bialké, H. Löwen, and T. Speck, Microscopic theory for the phase separation of self-propelled repulsive disks, Europhys. Lett. 103, 30008 (2013).
  52. See Supplemental Material at http://link.aps.org/supplemental/10.1103/m3dy-53yc for details on the underlying energy functional, governing equations and parameters, a microscopic derivation of the model, a linear stability analysis of uniform states, a discussion of the quantitative relation to classical MIPS and active Cahn-Hilliard models, details on the used numerical methods, and an analysis of the bifurcation behavior for one-dimensional states. It also includes Refs. [53–72].
  53. J. P. Boyd, Chebyshev and Fourier Spectral Methods (Dover Publ., Mineola, NY, 2. (rev.) edition, 2001).
  54. S. Engelnkemper, S. V. Gurevich, H. Uecker, D. Wetzel, and U. Thiele, Continuation for thin film hydrodynamics and related scalar problems, in Computational Modeling of Bifurcations and Instabilities in Fluid Mechanics, edited by A. Gelfgat, Computational Methods in Applied Sciences Vol. 50 (Springer, Cham, 2019), pp. 459–501, 10.1007/978-3-319-91494-7_13.
  55. H. Uecker, D. Wetzel, and J. D. M. Rademacher, pde2path—a matlab package for continuation and bifurcation in 2D elliptic systems, Numer. Math. Theory Methods Appl. 7, 58 (2014).
  56. D. Greve and U. Thiele, An amplitude equation for the conserved-Hopf bifurcation—derivation, analysis, and assessment, Chaos 34, 123134 (2024).
  57. G. S. Redner, M. F. Hagan, and A. Baskaran, Structure and dynamics of a phase-separating active colloidal fluid, Phys. Rev. Lett. 110, 055701 (2013).
  58. M. te Vrugt and R. Wittkowski, Relations between angular and Cartesian orientational expansions, AIP Adv. 10, 035106 (2020).
  59. M. te Vrugt, J. Bickmann, and R. Wittkowski, How to derive a predictive field theory for active Brownian particles: A step-by-step tutorial, J. Phys. Condens. Matter 35, 313001 (2023).
  60. M. te Vrugt, M. P. Holl, A. Koch, R. Wittkowski, and U. Thiele, Derivation and analysis of a phase field crystal model for a mixture of active and passive particles, Modelling Simul. Mater. Sci. Eng. 30, 084001 (2022).
  61. S. Hermann, P. Krinninger, D. de las Heras, and M. Schmidt, Phase coexistence of active Brownian particles, Phys. Rev. E 100, 052604 (2019).
  62. Z.-F. Huang, M. te Vrugt, R. Wittkowski, and H. Löwen, Active pattern formation emergent from single-species nonreciprocity, arXiv:2404.10093.
  63. Z.-F. Huang, M. te Vrugt, R. Wittkowski, and H. Löwen, Anomalous grain dynamics and grain locomotion of odd crystals, arXiv:2505.03957 [Proc. Natl. Acad. Sci. U.S.A. (to be published)].
  64. R. Wittkowski, J. Stenhammar, and M. E. Cates, Nonequilibrium dynamics of mixtures of active and passive colloidal particles, New J. Phys. 19, 105003 (2017).
  65. S. Bröker, M. te Vrugt, J. Jeggle, J. Stenhammar, and R. Wittkowski, Pair-distribution function of active Brownian spheres in three spatial dimensions: Simulation results and analytical representation, Soft Matter 20, 224 (2024).
  66. S. Bröker, M. te Vrugt, and R. Wittkowski, Collective dynamics and pair-distribution function of active Brownian ellipsoids in two spatial dimensions, Commun. Phys. 7, 238 (2024).
  67. J. Jeggle, J. Stenhammar, and R. Wittkowski, Pair-distribution function of active Brownian spheres in two spatial dimensions: Simulation results and analytic representation, J. Chem. Phys. 152, 194903 (2020).
  68. U. Marini Bettolo Marconi and P. Tarazona, Dynamic density functional theory of fluids, J. Chem. Phys. 110, 8032 (1999).
  69. A. J. Archer and R. Evans, Dynamical density functional theory and its application to spinodal decomposition, J. Chem. Phys. 121, 4246 (2004).
  70. A. J. M. Yang, P. D. Fleming, and J. H. Gibbs, Molecular theory of surface tension, J. Chem. Phys. 64, 3732 (1976).
  71. J. Toner and Y. Tu, Long-range order in a two-dimensional dynamical XY model: How birds fly together, Phys. Rev. Lett. 75, 4326 (1995).
  72. M. P. Holl, A. J. Archer, and U. Thiele, Efficient calculation of phase coexistence and phase diagrams: Application to a binary phase-field crystal model, J. Phys. Condens. Matter 33, 115401 (2021).
  73. The constant α allows one to easily switch between common parametrizations.

  74. M. E. Cates and J. Tailleur, When are active Brownian particles and run-and-tumble particles equivalent? Consequences for motility-induced phase separation, Europhys. Lett. 101, 20010 (2013).
  75. T. Frohoff-Hülsmann and U. Thiele, Nonreciprocal Cahn-Hilliard model emerges as a universal amplitude equation, Phys. Rev. Lett. 131, 107201 (2023).
  76. U. Thiele, T. Frohoff-Hülsmann, S. Engelnkemper, E. Knobloch, and A. J. Archer, First order phase transitions and the thermodynamic limit, New J. Phys. 21, 123021 (2019).
  77. H. Xu, Y. Huang, R. Zhang, and Y. Wu, Autonomous waves and global motion modes in living active solids, Nat. Phys. 19, 46 (2023).
  78. T. H. Tan, A. Mietke, J. Li, Y. Chen, H. Higinbotham, P. J. Foster, S. Gokhale, J. Dunkel, and N. Fakhri, Odd dynamics of living chiral crystals, Nature (London) 607, 287 (2022).
  79. J. Yan, S. C. Bae, and S. Granick, Rotating crystals of magnetic Janus colloids, Soft Matter 11, 147 (2015).
  80. M. N. van der Linden, L. C. Alexander, D. G. A. L. Aarts, and O. Dauchot, Interrupted motility induced phase separation in aligning active colloids, Phys. Rev. Lett. 123, 098001 (2019).
  81. N. H. P. Nguyen, D. Klotsa, M. Engel, and S. C. Glotzer, Emergent collective phenomena in a mixture of hard shapes through active rotation, Phys. Rev. Lett. 112, 075701 (2014).
  82. Z. T. Liu, Y. Shi, Y. Zhao, H. Chaté, X.-q. Shi, and T. H. Zhang, Activity waves and freestanding vortices in populations of subcritical Quincke rollers, Proc. Natl. Acad. Sci. U.S.A. 118, e2104724118 (2021).
  83. B. V. Hokmabad, A. Nishide, P. Ramesh, C. Krüger, and C. C. Maass, Spontaneously rotating clusters of active droplets, Soft Matter 18, 2731 (2022).
  84. A. S. Moskalenko, A. W. Liehr, and H. G. Purwins, Rotational bifurcation of localized dissipative structures, Europhys. Lett. 63, 361 (2003).
  85. J. Burke and E. Knobloch, Localized states in the generalized Swift-Hohenberg equation, Phys. Rev. E 73, 056211 (2006).
  86. E. Knobloch, Localized structures and front propagation in systems with a conservation law, IMA J. Appl. Math. 81, 457 (2016).
  87. At mean densities higher than ϕ¯=−0.45, one finds a larger Rmin≈18.8 due to the softening of the interface between uniform background and pattern. The interface is quite sharp at low T but widens at larger T.

  88. That their simulations do not show traveling crystallites may be due to their choice of boundary conditions.

  89. Z. F. Huang, A. M. Menzel, and H. Löwen, Dynamical crystallites of active chiral particles, Phys. Rev. Lett. 125, 218002 (2020).
  90. M. P. Holl, A. B. Steinberg, M. te Vrugt, and U. Thiele, Data supplement for “Motility-induced crystallization and rotating crystallites”, Zenodo, 2025, 10.5281/zenodo.17104279.

Outline

Information

Sign In to Your Journals Account

Filter

Filter

Article Lookup

Enter a citation