Screening and collective effects in randomly pinned fluids: A new theoretical framework

Abstract

We propose a theoretical framework for the dynamics of bulk isotropic hard-sphere systems in the presence of randomly pinned particles and apply this theory to supercooled water to validate it. Structural relaxation is mainly governed by local and non-local activated process. As the pinned fraction grows, a local caging constraint becomes stronger and the long range collective aspect of relaxation is screened by immobile obstacles. Different responses of the local and cooperative motions results in subtle predictions for how the alpha relaxation time varies with pinning and density. Our theoretical analysis for the relaxation time of water with pinned molecules quantitatively well describe previous simulations. In addition, the thermal dependence of relaxation for unpinned bulk water is also consistent with prior computational and experimental data.

7 pages, 4 figures, accepted for publication in Journal of Physics: Condensed Matter

References in corpus (8)

• Theoretical perspective on the glass transition and amorphous materials
• Growing Dynamical Facilitation on Approaching the Random Pinning Colloidal Glass Transition
• Slow Relaxation, Spatial Mobility Gradients and Vitrification in Confined Films
• Non-linear dynamic response of glass-forming liquids to random pinning
• Effects of Cooling Rate on Structural Relaxation in Amorphous Drugs: Elastically Collective Nonlinear Langevin Equation Theory and Machine Learning Study
• Coupling between structural relaxation and diffusion in glass-forming liquids under pressure variation
• Tailoring Drug Mobility by Photothermal Heating of Graphene Plasmons
• Impact of high pressure on reversible structural relaxation of metallic glass