Furukawa Akira
Institute of Industrial Science, University of Tokyo, Tokyo 153-8505, Japan.
Phys Rev E Stat Nonlin Soft Matter Phys. 2013 Jun;87(6):062321. doi: 10.1103/PhysRevE.87.062321. Epub 2013 Jun 28.
Although it is now well established that in glassy liquids, slow structural relaxation accompanies a correlated structural rearrangement, the role of such a correlation in the transport anomaly, and thus in the slow dynamics, remains unclear. In this paper, we argue from a hydrodynamic viewpoint that a correlated structure (cluster) with a characteristic size ξ sustains the long-lived stress and dynamically couples with the hydrodynamic fluctuations; therefore, the dynamics of this cluster is the origin of the mesoscopic nature of anomalous hydrodynamic transport. Based on this argument, we derive a dynamic scaling law for τ(α) (or η, where η is the macroscopic shear viscosity) as a function of ξ: τ(α)([proportionality]η)[proportionality]ξ(4). We provide a simple explanation for basic features of anomalous transport, such as the breakdown of the Stokes-Einstein relation and the length-scale-dependent decoupling between viscosity and diffusion. The present study further suggests a different physical picture: Through the coarse graining of smaller-scale fluctuations (</~ξ), the supercooled liquid dynamics can be regarded as the dynamics of normal (cluster) liquids composed of units with a typical size of ξ. Although the correlation length of hydrodynamic transport ξ and the dynamic heterogeneity size ξ(DH), which is determined by the usual four-point correlation function, reflect some aspects of the cooperative effects, the correspondence between ξ and ξ(DH) is not one to one. We highlight the possibility that ξ(DH) overestimates the actual collective transport range at a low degree of supercooling.
尽管现在已经充分证实,在玻璃态液体中,缓慢的结构弛豫伴随着相关的结构重排,但这种相关性在输运异常中,进而在缓慢动力学中的作用仍不明确。在本文中,我们从流体动力学的角度认为,具有特征尺寸ξ的相关结构(团簇)维持着长寿命应力,并与流体动力学涨落动态耦合;因此,该团簇的动力学是反常流体动力学输运介观性质的起源。基于这一观点,我们推导出τ(α)(或η,其中η是宏观剪切粘度)作为ξ的函数的动态标度律:τ(α)(∝η)∝ξ⁴。我们对反常输运的基本特征,如斯托克斯 - 爱因斯坦关系的失效以及粘度与扩散之间与长度尺度相关的解耦,给出了一个简单解释。本研究进一步提出了一种不同的物理图像:通过对较小尺度涨落(<~ξ)的粗粒化,过冷液体动力学可被视为由典型尺寸为ξ的单元组成的正常(团簇)液体的动力学。尽管流体动力学输运的关联长度ξ和由通常的四点关联函数确定的动态非均匀性尺寸ξ(DH)反映了协同效应的某些方面,但ξ与ξ(DH)之间并非一一对应。我们强调了在低过冷度下ξ(DH)高估实际集体输运范围的可能性。