Exploring the soft pinning effect in the dynamics and the structure-dynamics correlation in multicomponent supercooled liquids.

J Chem Phys

Polymer Science and Engineering Division, CSIR-National Chemical Laboratory, Pune 411008, India.

Published: October 2024

AI Article Synopsis

  • The study investigates how increasing the mass of 15% of particles in a binary Kob-Andersen model affects the dynamics of a multicomponent liquid.
  • At higher temperatures, heavier particles result in a decoupling of their movements from lighter particles, causing the lighter particles to slow down as they become constrained by the heavier particles.
  • Contrastingly, at lower temperatures, heavier particles couple with lighter ones, slowing down both types, with heavier masses acting more like soft pinning centers, suggesting their impact on particle dynamics depends on temperature and mass.

Article Abstract

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.

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Source
http://dx.doi.org/10.1063/5.0230932DOI Listing

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