Anwar Ehtesham, Patel Palak, Sharma Mohit, Maitra Bhattacharyya Sarika
Polymer Science and Engineering Division, CSIR-National Chemical Laboratory, Pune 411008, India.
Academy of Scientific and Innovative Research (AcSIR), Ghaziabad 201002, India.
J Chem Phys. 2024 Oct 21;161(15). doi: 10.1063/5.0230932.
We study multicomponent liquids by increasing the mass of 15% of the particles in a binary Kob-Andersen model. We find that the heavy particles have dual effects on the lighter particles. At higher temperatures, there is a significant decoupling of the dynamics between heavier and lighter particles, with the former resembling a pinned particle to the latter. The dynamics of the lighter particles slow down due to the excluded volume around the nearly immobile heavier particles. Conversely, at lower temperatures, there is a coupling between the dynamics of the heavier and lighter particles. The heavier particles' mass slows down the dynamics of both types of particles. This makes the soft pinning effect of the heavy particles questionable in this regime. We demonstrate that as the mass of the heavy particles increases, the coupling of the dynamics between the lighter and heavier particles weakens. Consequently, the heavier the mass of the heavy particles, the more effectively they act as soft pinning centers in both high and low-temperature regimes. A key finding is that akin to the pinned system, the self-dynamics and collective dynamics of the lighter particles decouple from each other as the mass of the heavy particles has a more pronounced impact on the latter. We analyze the structure-dynamics correlation by considering the system under the binary and modified quaternary framework, the latter describing the pinned system. Our findings indicate that whenever the heavy mass particles function as soft pinning centers, the modified quaternary framework predicts a higher correlation.
我们通过增加二元Kob-Andersen模型中15%粒子的质量来研究多组分液体。我们发现重粒子对轻粒子有双重影响。在较高温度下,重粒子和轻粒子之间的动力学存在显著解耦,前者对后者而言类似于被固定的粒子。由于几乎不动的重粒子周围的排除体积,轻粒子的动力学减慢。相反,在较低温度下,重粒子和轻粒子的动力学之间存在耦合。重粒子的质量使两种类型粒子的动力学都减慢。这使得在这种情况下重粒子的软钉扎效应存疑。我们证明,随着重粒子质量的增加,轻粒子和重粒子之间的动力学耦合减弱。因此,重粒子的质量越大,它们在高温和低温区域作为软钉扎中心的作用就越有效。一个关键发现是,类似于被固定的系统,随着重粒子质量对后者的影响更为显著,轻粒子的自动力学和集体动力学相互解耦。我们通过在二元和修正四元框架下考虑系统来分析结构 - 动力学相关性,后者描述了被固定的系统。我们的研究结果表明,只要重质量粒子起到软钉扎中心的作用,修正四元框架就会预测出更高的相关性。