Abstract
The transition of a fluid to a rigid glass on cooling is a common route of transformation from liquid to solid that embodies the most poorly understood features of both phases1,2,3. From the liquid perspective, the puzzle is to understand stress relaxation in the disordered state. From the perspective of solids, the challenge is to extend our description of structure and its mechanical consequences to materials without long-range order. Using computer simulations, we show that the localized low-frequency normal modes of a configuration in a supercooled liquid are causally correlated to the irreversible structural reorganization of the particles within this configuration. We also demonstrate that the spatial distribution of these soft local modes can persist in spite of significant particle reorganization. The consequence of these two results is that it is now feasible to construct a theory of relaxation length scales in glass-forming liquids without recourse to dynamics and to explicitly relate molecular properties to their collective relaxation.
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Acknowledgements
We would like to thank L. Berthier, G. Biroli, J. P. Bouchaud, A. Heuer, and C. O’Hern for discussions. H.P. and D.R.R. would like to thank P. Verrocchio for providing the equilibrated three-dimensional configurations and NSF for financial support. A.W.-C. and P.H. acknowledge the support of the Australian Research Council. H.P. was partially supported by the MRSEC program of the National Science Foundation under grant No DMR-0213574.
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P.H. and D.R.R. conceived this study and wrote the paper. A.W.-C. carried out the MD simulation, analysed the motions and devised the contour plots. H.P. carried out the normal-mode analysis and graphical representation of the eigenfunctions.
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Widmer-Cooper, A., Perry, H., Harrowell, P. et al. Irreversible reorganization in a supercooled liquid originates from localized soft modes. Nature Phys 4, 711–715 (2008). https://doi.org/10.1038/nphys1025
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DOI: https://doi.org/10.1038/nphys1025
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