Understanding Dynamics in Coarse-Grained Models: I. Universal Excess Entropy Scaling Relationship

Abstract

Coarse-grained (CG) models facilitate an efficient exploration of complex systems by reducing the unnecessary degrees of freedom of the fine-grained (FG) system while recapitulating major structural correlations. Unlike structural properties, assessing dynamic properties in CG modeling is often unfeasible due to the accelerated dynamics of the CG models, which allows for more efficient structural sampling. Therefore, the ultimate goal of the present series of articles is to establish a better correspondence between the FG and CG dynamics. To assess and compare dynamical properties in the FG and the corresponding CG models, we utilize the excess entropy scaling relationship. For Paper I of this series, we provide evidence that the FG and the corresponding CG counterpart follow the same universal scaling relationship. By carefully reviewing and examining the literature, we develop a new theory to calculate excess entropies for the FG and CG systems while accounting for entropy representability. We demonstrate that the excess entropy scaling idea can be readily applied to liquid water and methanol systems at both the FG and CG resolutions. For both liquids, we reveal that the scaling exponents remain unchanged from the coarse-graining process, indicating that the scaling behavior is universal for the same underlying molecular systems. Combining this finding with the concept of mapping entropy in CG models, we show that the missing entropy plays an important role in accelerating the CG dynamics.

31 pages, 9 figures

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Cited by in corpus (9)

• Understanding Dynamics in Coarse-Grained Models: II. Coarse-Grained Diffusion Modeled Using Hard Sphere Theory
• Universal Relation between Entropy and Kinetics
• A Gauss-Newton method for iterative optimization of memory kernels for generalized Langevin thermostats in coarse-grained molecular dynamics simulations
• Understanding Dynamics in Coarse-Grained Models: IV. Connection of Fine-Grained and Coarse-Grained Dynamics with the Stokes-Einstein and Stokes-Einstein-Debye Relations
• Understanding Dynamics in Coarse-Grained Models: V. Extension of Coarse-Grained Dynamics Theory to Non-Hard Sphere Systems
• Finite-size excess-entropy scaling for simple liquids
• Hierarchical Framework for Predicting Entropies in Bottom-Up Coarse-Grained Models
• A Bottom-Up Field-Theoretic Framework via Hierarchical Coarse-Graining: Generalized Mode Theory
• Knowledge Distillation of Noisy Force Labels for Improved Coarse-Grained Force Fields