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- Title
Early-stage bifurcation of crystallization in a sphere.
- Authors
Mbah, Chrameh Fru; Wang, Junwei; Englisch, Silvan; Bommineni, Praveen; Varela-Rosales, Nydia Roxana; Spiecker, Erdmann; Vogel, Nicolas; Engel, Michael
- Abstract
Bifurcations in kinetic pathways decide the evolution of a system. An example is crystallization, in which the thermodynamically stable polymorph may not form due to kinetic hindrance. Here, we use confined self-assembly to investigate the interplay of thermodynamics and kinetics in the crystallization pathways of finite clusters. We report the observation of decahedral clusters from colloidal particles in emulsion droplets and show that these decahedral clusters can be thermodynamically stable, just like icosahedral clusters. Our hard sphere simulations reveal how the development of the early nucleus shape passes through a bifurcation that decides the cluster symmetry. A geometric argument explains why decahedral clusters are kinetically hindered and why icosahedral clusters can be dominant even if they are not in the thermodynamic ground state. Thermodynamics predicts equilibrium crystal structures and kinetics discover the pathway to form them. The authors investigate the interplay of thermodynamics and kinetics in the formation of colloidal clusters and reveal a bifurcation at an early stage of the crystallization process.
- Subjects
CRYSTALLIZATION; CRYSTALLIZATION kinetics; SPHERES; THERMODYNAMIC equilibrium; COLLOIDAL crystals; CRYSTAL structure
- Publication
Nature Communications, 2023, Vol 14, Issue 1, p1
- ISSN
2041-1723
- Publication type
Article
- DOI
10.1038/s41467-023-41001-6