Crystal growth rates in supercooled atomic liquid mixtures

Abstract

Crystallization is a fundamental process in materials science, providing the primary route for the realization of a wide range of new materials. Crystallization rates are also considered to be useful probes of glass-forming ability1,2,3. At the microscopic level, crystallization is described by the classical crystal nucleation and growth theories4,5, yet in general solid formation is a far more complex process. In particular, the observation of apparently different crystal growth regimes in many binary liquid mixtures greatly challenges our understanding of crystallization1,6,7,8,9,10,11,12. Here, we study by experiments, theory and computer simulations the crystallization of supercooled mixtures of argon and krypton, showing that crystal growth rates in these systems can be reconciled with existing crystal growth models only by explicitly accounting for the non-ideality of the mixtures. Our results highlight the importance of thermodynamic aspects in describing the crystal growth kinetics, providing a substantial step towards a more sophisticated theory of crystal growth.

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Fig. 1: Schematic of the experiment and diffraction profiles.
Fig. 2: Experimental data and comparison with theoretical calculations and simulation results.
Fig. 3: Temperature dependence of simulated and theoretical crystal growth rates.

Data availability

The datasets generated and/or analysed during the current study are available from the corresponding author on reasonable request.

Code availability

The codes used during the current study are available from the corresponding author on reasonable request.

Change history

  • 03 March 2020

    In the version of this Article originally published, the Δ in ΔSm and ΔG in the paragraph after equation (1) should have been roman; the x in (1 − x) before equation (12) should have been italic; and ‘measurement’, ‘thermodynamic’ and ‘vibrational’ in refs. 35, 36 and 39, respectively, should have been capitalized. These have now been updated.

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Acknowledgements

We acknowledge financial support from the Bundesministerium für Bildung und Forschung (grant no. 05K13RF5). We acknowledge the CINECA award nos. LISA-PUMAS (2016), IscraC-GLEMD (2017) and IscraB-MEMETICO (2018) for the availability of high-performance computing resources and support. We acknowledge DESY (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III and we thank S. Roth for the unlimited support during the experiments at the beamline P03.

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A.S. and F.M. contributed equally to this work. R.E.G. conceived the experiment. A.S. designed and assembled the experimental setup. A.S., F.M., A.K., B.B., A.R., C.G., J.M., N.P., M.R., F.T., J.M.F., T.A.E. and R.E.G. performed the experiments. A.S. and R.E.G. analysed the experimental data. R.E.G. performed the theoretical crystal growth rate calculations. F.M. and D.E.G. conceived and carried out the molecular dynamics simulations. F.M., D.E.G. and R.E.G. wrote the paper, with contributions from all authors

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Correspondence to Robert E. Grisenti.

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Supplementary Figs. 1–6 and Tables 1 and 2.

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Schottelius, A., Mambretti, F., Kalinin, A. et al. Crystal growth rates in supercooled atomic liquid mixtures. Nat. Mater. 19, 512–516 (2020). https://doi.org/10.1038/s41563-020-0613-z

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