Benitez-Camacho Nohely, Olais-Govea José Manuel, López-Flores Leticia, Ruiz-Estrada Honorina
Facultad de Ciencias Físico Matemáticas, Benemérita Universidad Autónoma de Puebla, Apartado Postal 1152, 72000, Puebla, PUE, Mexico.
Tecnologico de Monterrey, Escuela de Ingeniería y Ciencias, 78211 San Luis Potosí, San Luis Potosí, México.
J Chem Phys. 2023 Jul 28;159(4). doi: 10.1063/5.0147983.
Amorphous solids, such as glasses and gels, arise as the asymptotic limit of non-equilibrium and irreversible relaxation aging processes. These amorphous solids form when the system is suddenly and deeply quenched in the dynamic arrest region. We use the non-equilibrium self-consistent generalized Langevin equation (NE-SCGLE) theory to investigate the formation of such structures via arrested spinodal decomposition in the screened symmetric restricted primitive model. We propose a direct correlation function that allows us to derive an expression for the functional derivative of the chemical potential, which serves as the necessary input in the NE-SCGLE theory. By analyzing the asymptotic localization length and the asymptotic characteristic length, we identify different classes of dynamic arrest states as a function of the density and the final quench temperature. The system features simultaneously attractive and repulsive interactions, resulting in different arrested regions in the non-equilibrium phase diagram for a given screened parameter: (i) ionic glasses, (ii) electrostatic gels, and (iii) attractive glasses. Finally, by collapsing the asymptotic effective structure factors at a typical fractal dimension of df = 3, we confirm the formation of gels slightly above the glass-gel transition in the arrested phase diagram.
非晶态固体,如玻璃和凝胶,是作为非平衡和不可逆弛豫老化过程的渐近极限而出现的。当系统在动态阻滞区域突然且深度淬火时,这些非晶态固体就会形成。我们使用非平衡自洽广义朗之万方程(NE-SCGLE)理论,通过在屏蔽对称受限原胞模型中通过阻滞的旋节线分解来研究此类结构的形成。我们提出了一个直接相关函数,它使我们能够导出化学势泛函导数的表达式,这是NE-SCGLE理论中必要的输入。通过分析渐近局域化长度和渐近特征长度,我们确定了不同类型的动态阻滞状态作为密度和最终淬火温度的函数。该系统同时具有吸引和排斥相互作用,对于给定的屏蔽参数,在非平衡相图中会产生不同的阻滞区域:(i)离子玻璃,(ii)静电凝胶,以及(iii)吸引玻璃。最后,通过在典型分形维数df = 3时折叠渐近有效结构因子,我们证实了在阻滞相图中略高于玻璃-凝胶转变温度时凝胶的形成。