论文标题
在具有强距离景点的超密集流体中，割笼和断裂激活动力学发作的显微镜理论
Microscopic Theory of Onset of De-Caging and Bond Breaking Activated Dynamics in Ultra-Dense Fluids with Strong Short Range Attractions
论文作者
论文摘要
我们理论上研究了在超密集的粒子液体中通过强距离短距离吸引力相互作用的全结构弛豫的热激活基本动力学过程。我们的方法基于在动态自由能概念上建立的粒子轨迹水平上提出的微观理论，并明确处理了景点如何控制物理粘结。在排斥玻璃，粘合的排斥性（有吸引力的）玻璃，液体和密集的凝胶方案中分析了键断裂，笼子逃脱的早期阶段和固定的非叉位移的平均时间尺度。该理论预测，在固定堆积分数下，这些时间尺度的长度尺度依赖性依赖性依赖性，在固定堆积分数处具有吸引力的力量，在固定吸引强度下密度的较弱较弱，并且在固定吸引强度下的密度降低了，并且较短的键断裂时间与其他两个时间尺度的较短键突破了，这些时间尺度主要通过扰动的固定固定笼子控制。所有结果都与模拟良好，并做出其他可测试的预测。用一对结构确定的单个有效力代替所有裸露和排斥力的经典统计机械投影近似会导致主要误差，以描述与远离瞬时局部状态的热激活逃生相关的过程。
We theoretically study thermally activated elementary dynamical processes that precede full structural relaxation in ultra-dense particle liquids interacting via strong short range attractive forces. Our approach is based on a microscopic theory formulated at the particle trajectory level built on the dynamic free energy concept and an explicit treatment of how attractions control physical bonding. Mean time scales for bond breaking, the early stage of cage escape, and a fixed non-Fickian displacement are analyzed in the repulsive glass, bonded repulsive (attractive) glass, fluid, and dense gel regimes. The theory predicts a strong length-scale-dependent growth of these time scales with attractive force strength at fixed packing fraction, a much weaker slowing down with density at fixed attraction strength, and a strong decoupling of the shorter bond breaking time with the other two time scales that are controlled mainly by perturbed steric caging. All results are in good accord with simulations, and additional testable predictions are made. The classic statistical mechanical projection approximation of replacing all bare attractive and repulsive forces with a single effective force determined by pair structure incurs major errors for describing processes associated with thermally activated escape from transiently localized states.
