Abstract
The dynamical behaviour of liquids is frequently characterized by the fragility, which can be defined from the temperature dependence of the shear viscosity, η (ref. 1). For a strong liquid, the activation energy for η changes little with cooling towards the glass transition temperature, Tg. The change is much greater in fragile liquids, with the activation energy becoming very large near Tg. While fragility is widely recognized as an important concept—believed, for example, to play an important role in glass formation2—the microscopic origin of fragility is poorly understood. Here, we present new experimental evidence showing that fragility reflects the strength of the repulsive part of the interatomic potential, which can be determined from the steepness of the pair distribution function near the hard-sphere cutoff. On the basis of an analysis of scattering data from ten different metallic alloy liquids, we show that stronger liquids have steeper repulsive potentials.
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Acknowledgements
We thank D. Robinson for his assistance with the high-energy X-ray diffraction studies at the APS and A. Agrawal, A. Gangopadhyay, K. Samwer and L. Yang for useful discussions. K.F.K. and C.E.P. gratefully acknowledge support by NASA under Grant No. NNX16AB52G and the National Science Foundation under Grant No. DMR 15-06553. M.S. gratefully acknowledges support by the Foundation for the Science and Technological Innovation Talent of Harbin (No. 2010RFQXG028). The synchrotron measurements were made on the Sector 6 beamline at the Advanced Photon Source. Use of the Advanced Photon Source is supported by the US Department of Energy, Basic Energy Science, Office of Science, under contract no. DE-AC02-06CH11357. Any opinions, findings and conclusions or recommendations expressed in this article are those of the author(s) and do not necessarily reflect the views of the National Science Foundation or of NASA.
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K.F.K. conceived of the study. K.F.K. and C.E.P. obtained the experimental data, and M.S. carried out the MD simulations. K.F.K. and C.E.P. analysed all experimental and MD data, and all authors contributed to writing and editing the document.
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Pueblo, C., Sun, M. & Kelton, K. Strength of the repulsive part of the interatomic potential determines fragility in metallic liquids. Nature Mater 16, 792–796 (2017). https://doi.org/10.1038/nmat4935
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DOI: https://doi.org/10.1038/nmat4935
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