Furukawa Akira, Tanaka Hajime
Institute of Industrial Science, University of Tokyo, Meguro-ku, Tokyo 153-8505, Japan.
Phys Rev E Stat Nonlin Soft Matter Phys. 2011 Dec;84(6 Pt 1):061503. doi: 10.1103/PhysRevE.84.061503. Epub 2011 Dec 14.
Dynamic heterogeneity is now considered to be an intrinsic kinetic feature of a supercooled liquid. Here, we access the nonlocal complex modulus of a glass-forming liquid using molecular dynamics simulations. We find that the shear-stress relaxation exhibits a marked wave number dependence in a supercooled state. This dependence provides direct evidence that slow mechanical relaxation takes place heterogeneously in space. Its characteristic length ξ increases with decreasing temperature and becomes mesoscopic. The response involves particle rearrangements over ξ and takes a time comparable to the structural relaxation time τ(α). Our finding suggests that the heterogeneous structural relaxation is of fundamental importance in anomalous viscous transport and viscoelasticity in supercooled liquids.
动态非均匀性现在被认为是过冷液体的一种内在动力学特征。在这里,我们使用分子动力学模拟来研究玻璃形成液体的非局部复模量。我们发现,在过冷状态下,剪切应力弛豫表现出明显的波数依赖性。这种依赖性提供了直接证据,表明缓慢的力学弛豫在空间中是不均匀发生的。其特征长度ξ随温度降低而增加,并变为介观尺度。这种响应涉及到在ξ尺度上的粒子重排,并且所需时间与结构弛豫时间τ(α)相当。我们的发现表明,非均匀结构弛豫在过冷液体的反常粘性输运和粘弹性中具有至关重要的意义。