Salt-concentration-dependent nucleation rates in low-metastability colloidal charged sphere melts containing small amounts of doublets

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2021
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Schwarz, Jürgen
Palberg, Thomas
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We determined bulk crystal nucleation rates in aqueous suspensions of charged spheres at low metastability. Experiments were performed in dependence on electrolyte concentration and for two different particle number densities. The time-dependent nucleation rate shows a pronounced initial peak, while postsolidification crystal size distributions are skewed towards larger crystallite sizes. At each concentration, the nucleation rate density initially drops exponentially with increasing salt concentration. The full data set, however, shows an unexpected scaling of the nucleation rate densities with metastability times the number density of particles. Parameterization of our results in terms of classical nucleation theory reveals unusually low interfacial free energies of the nucleus surfaces and nucleation barriers well below the thermal energy. We tentatively attribute our observations to the presence of doublets introduced by the employed conditioning technique. We discuss the conditions under which such small seeds may induce nucleation.

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ISO 690SCHWARZ, Jürgen, Paul LEIDERER, Thomas PALBERG, 2021. Salt-concentration-dependent nucleation rates in low-metastability colloidal charged sphere melts containing small amounts of doublets. In: Physical Review E. American Physical Society (APS). 2021, 104(6), 064607. ISSN 2470-0045. eISSN 2470-0053. Available under: doi: 10.1103/PhysRevE.104.064607
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@article{Schwarz2021Saltc-56076,
  year={2021},
  doi={10.1103/PhysRevE.104.064607},
  title={Salt-concentration-dependent nucleation rates in low-metastability colloidal charged sphere melts containing small amounts of doublets},
  number={6},
  volume={104},
  issn={2470-0045},
  journal={Physical Review E},
  author={Schwarz, Jürgen and Leiderer, Paul and Palberg, Thomas},
  note={Article Number: 064607}
}
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    <dcterms:abstract xml:lang="eng">We determined bulk crystal nucleation rates in aqueous suspensions of charged spheres at low metastability. Experiments were performed in dependence on electrolyte concentration and for two different particle number densities. The time-dependent nucleation rate shows a pronounced initial peak, while postsolidification crystal size distributions are skewed towards larger crystallite sizes. At each concentration, the nucleation rate density initially drops exponentially with increasing salt concentration. The full data set, however, shows an unexpected scaling of the nucleation rate densities with metastability times the number density of particles. Parameterization of our results in terms of classical nucleation theory reveals unusually low interfacial free energies of the nucleus surfaces and nucleation barriers well below the thermal energy. We tentatively attribute our observations to the presence of doublets introduced by the employed conditioning technique. We discuss the conditions under which such small seeds may induce nucleation.</dcterms:abstract>
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