Understanding Dynamics in Coarse-Grained Models: I. Universal Excess Entropy Scaling Relationship
arXiv:2208.00078 · doi:10.1063/5.0116299
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.
arXiv comment31 pages, 9 figures
References in corpus (25)
- "Isomorphs" in liquid state diagrams
- Pressure-energy correlations in liquids. IV. "Isomorphs" in liquid state diagrams
- Mode-Coupling Theory (MCT) Lecture Notes
- Thermodynamics predicts how confinement modifies hard-sphere dynamics
- Iterative Reconstruction of Memory Kernels
- Pressure-energy correlations in liquids. III. Statistical mechanics and thermodynamics of liquids with hidden scale invariance
- Strong pressure-energy correlations in liquids as a configuration space property: Simulations of temperature down jumps and crystallization
- Resolving Dynamic Properties of Polymers through Coarse-Grained Computational Studies
- Breakdown of The Excess Entropy Scaling for the Systems with Thermodynamic Anomalies
- Relationship between Structure, Entropy and Diffusivity in Water and Water-like Liquids
- An analytical coarse-graining method which preserves the free energy, structural correlations, and thermodynamic state of polymer melts from the atomistic to the mesoscale
- A First Principle Approach to Rescale the Dynamics of Simulated Coarse-Grained Macromolecular Liquids
- Estimating Entropy of Liquids from Atom-Atom Radial Distribution Functions: Silica, Beryllium Fluoride and Water
- Generalized Langevin dynamics: Construction and numerical integration of non-Markovian particle-based models
- Analytical Rescaling of Polymer Dynamics from Mesoscale Simulations
- Systematic Coarse-graining of Epoxy Resins with Machine Learning-Informed Energy Renormalization
- Understanding three-body contributions to coarse-grained force-fields
- Unraveling the success and failure of mode coupling theory from consideration of entropy
- Theoretical Reconstruction of Realistic Dynamics of Highly Coarse-Grained cis-1,4-Polybutadiene Melts
- Super-Arrhenius slowing down in the metastable liquid of hard spheres
- Understanding Dynamics in Coarse-Grained Models: II. Coarse-Grained Diffusion Modeled Using Hard Sphere Theory
- Systematic parameter inference in stochastic mesoscopic modeling
- Two-phase Thermodynamic Model for Computing Entropies of Liquids Reanalyzed
- Model reduction techniques for the computation of extended Markov parameterizations for generalized Langevin equations
- Entropy scaling laws for diffusion
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