Szamel Grzegorz
Department of Chemistry, Colorado State University, Fort Collins, Colorado 80523, USA.
J Chem Phys. 2022 May 21;156(19):191102. doi: 10.1063/5.0091385.
We propose an alternative theory for the relaxation of density fluctuations in glass-forming fluids. We derive an equation of motion for the density correlation function that is local in time and is similar in spirit to the equation of motion for the average non-uniform density profile derived within the dynamic density functional theory. We identify the Franz-Parisi free energy functional as the non-equilibrium free energy for the evolution of the density correlation function. An appearance of a local minimum of this functional leads to a dynamic arrest. Thus, the ergodicity breaking transition predicted by our theory coincides with the dynamic transition of the static approach based on the same non-equilibrium free energy functional.
我们提出了一种关于玻璃形成流体中密度涨落弛豫的替代理论。我们推导了密度关联函数的运动方程,该方程在时间上是局部的,并且在精神上类似于动态密度泛函理论中导出的平均非均匀密度分布的运动方程。我们将弗朗茨 - 帕里西自由能泛函确定为密度关联函数演化的非平衡自由能。该泛函局部最小值的出现导致动态停滞。因此,我们理论预测的遍历性破缺转变与基于相同非平衡自由能泛函的静态方法的动态转变相吻合。