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Long-Lived Non-Equilibrium Interstitial-Solid-Solutions in Binary Mixtures

Rios de Anda, Ioatzin, Turci, Francesco, Sear, Richard and Royall, Patrick (2017) Long-Lived Non-Equilibrium Interstitial-Solid-Solutions in Binary Mixtures Journal of Chemical Physics, 147.

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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 find 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 at equilibrium when the size ratios are 0.3 [Filion et al., Phys. Rev. Lett. 107, 168302 (2011)] and 0.4 [Filion, PhD Thesis, Utrecht University (2011)]. However, unlike these previous studies, 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.

Item Type: Article
Divisions : Faculty of Engineering and Physical Sciences > Physics
Authors :
Rios de Anda, Ioatzin
Turci, Francesco
Royall, Patrick
Date : 28 September 2017
DOI : 10.1063/1.4985917
Copyright Disclaimer : Copyright 2017 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in The Journal of Chemical Physics 147, 124504 (2017); doi: 10.1063/1.4985917
Depositing User : Clive Harris
Date Deposited : 15 Sep 2017 12:23
Last Modified : 16 Jan 2019 18:56

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