Long-lived non-equilibrium interstitial solid solutions in binary mixtures

Ioatzin Rios De Anda, Francesco Turci, Richard P Sear, C P Royall

Research output: Contribution to journalArticle (Academic Journal)peer-review

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We perform particle resolved experimental studies on the heterogeneous crystallisation process of two component mixtures of hard spheres. The components have a size ratio of 0.39. We compared these with molecular dynamics simulations of homogenous nucleation. We found for both experiments and simulations that the final assemblies are interstitial solid solutions, where the large particles form crystalline close-packed lattices, whereas the small particles occupy random interstitial sites. This interstitial solution resembles that found when the small particles are 0.3 and 0.4 of the larger particle’s diameter [Filion et al., Phys. Rev. Lett. 107, 168302 (2011)]. However, unlike these size ratios, for our system simulations showed that the small particles are trapped in the octahedral holes of the ordered structure formed by the large particles, leading to long-lived non-equilibrium structures in the time scales studied and not the equilibrium interstitial solutions found earlier. Interestingly, the percentage of small particles in the crystal formed by the large ones rapidly reaches a maximum of ∼14% for most of the packing fractions tested, unlike previous predictions where the occupancy of the interstitial sites increases with the system concentration. Finally, no further hopping of the small particles was observed.
Original languageEnglish
Article number124504
Number of pages10
JournalJournal of Chemical Physics
Issue number12
Early online date28 Sep 2017
Publication statusPublished - 28 Sep 2017


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