Tripodo Antonio, Giuntoli Andrea, Malvaldi Marco, Leporini Dino
Dipartimento di Fisica "Enrico Fermi", Università di Pisa, Largo B. Pontecorvo 3, I-56127 Pisa, Italy.
Soft Matter. 2019 Aug 28;15(34):6784-6790. doi: 10.1039/c9sm01143a.
The dynamical spatial correlations detected by the mutual information (MI) in the isoconfigurational particle displacements of a monodisperse molecular viscous liquid are studied via molecular-dynamics simulations by changing considerably both the molecular mobility and the degree of dynamical heterogeneity. Different from atomic liquids, the MI correlation length does not grow on approaching the glass transition by considering the liquid both in full detail as a collection of monomers and as a coarse-grained ensemble of molecular centers of mass. In the detailed picture, it is found that: (i) the MI correlations between monomers are largely due to inter-molecular correlations, (ii) the MI length scale is numerically identical, within the errors, to the correlation length scale of the displacement direction, as drawn by conventional correlation functions. The time evolution of the MI spatial correlations complies with the scaling between the fast vibrational dynamics and the long-time relaxation. Our findings suggest that the characteristics of the MI length scale are markedly system-dependent and not obviously related to dynamical heterogeneity.
通过分子动力学模拟,通过大幅改变分子迁移率和动力学非均匀性程度,研究了单分散分子粘性液体等构型粒子位移中由互信息(MI)检测到的动态空间相关性。与原子液体不同,通过将液体既详细地视为单体集合,又视为分子质心的粗粒化系综,MI相关长度在接近玻璃化转变时不会增长。在详细的图景中,发现:(i)单体之间的MI相关性很大程度上归因于分子间相关性,(ii)在误差范围内,MI长度尺度在数值上与传统相关函数绘制的位移方向相关长度尺度相同。MI空间相关性的时间演化符合快速振动动力学与长时间弛豫之间的标度关系。我们的发现表明,MI长度尺度的特征明显依赖于系统,且与动力学非均匀性没有明显关系。