4.7 Article

Broad chemical transferability in structure-based coarse-graining

Journal

JOURNAL OF CHEMICAL PHYSICS
Volume 157, Issue 10, Pages -

Publisher

AIP Publishing
DOI: 10.1063/5.0104914

Keywords

-

Funding

  1. Max Planck Graduate Center
  2. Emmy Noether program of the Deutsche Forschungsgemeinschaft (DFG)

Ask authors/readers for more resources

Compared to top-down coarse-grained models, bottom-up approaches offer higher structural accuracy but may lack chemical transferability. This study presents a method that combines bottom-up, structure-preserving coarse-grained models with chemical transferability, using a set of CG bead types to construct new molecules.
Compared to top-down coarse-grained (CG) models, bottom-up approaches are capable of offering higher structural fidelity. This fidelity results from the tight link to a higher resolution reference, making the CG model chemically specific. Unfortunately, chemical specificity can be at odds with compound-screening strategies, which call for transferable parameterizations. Here, we present an approach to reconcile bottom-up, structure-preserving CG models with chemical transferability. We consider the bottom-up CG parameterization of 3441 C7O2 small-molecule isomers. Our approach combines atomic representations, unsupervised learning, and a large-scale extended-ensemble force-matching parameterization. We first identify a subset of 19 representative molecules, which maximally encode the local environment of all gas-phase conformers. Reference interactions between the 19 representative molecules were obtained from both homogeneous bulk liquids and various binary mixtures. An extended-ensemble parameterization over all 703 state points leads to a CG model that is both structure-based and chemically transferable. Remarkably, the resulting force field is on average more structurally accurate than single-state-point equivalents. Averaging over the extended ensemble acts as a mean-force regularizer, smoothing out both force and structural correlations that are overly specific to a single-state point. Our approach aims at transferability through a set of CG bead types that can be used to easily construct new molecules while retaining the benefits of a structure-based parameterization. (C) 2022 Author(s)

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.7
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

No Data Available
No Data Available