Irreversible reorganization in a supercooled liquid originates from localized soft modes

被引:394
作者
Widmer-Cooper, Asaph [1 ]
Perry, Heidi [2 ]
Harrowell, Peter [1 ]
Reichman, David R. [2 ]
机构
[1] Univ Sydney, Sch Chem, Sydney, NSW 2006, Australia
[2] Columbia Univ, Dept Chem, New York, NY 10027 USA
基金
美国国家科学基金会;
关键词
D O I
10.1038/nphys1025
中图分类号
O4 [物理学];
学科分类号
0702 ;
摘要
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 phases(1-3). 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.
引用
收藏
页码:711 / 715
页数:5
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