Structural Coarse-Graining via Multiobjective Optimization with Differentiable Simulation.

Abstract

In the realm of multiscale molecular simulations, structure-based coarse-graining is a prominent approach for creating efficient coarse-grained (CG) representations of soft matter systems, such as polymers. This involves optimizing CG interactions by matching static correlation functions of the corresponding degrees of freedom in all-atom (AA) models. Here, we present a versatile method, namely, differentiable coarse-graining (DiffCG), which combines multiobjective optimization and differentiable simulation. The DiffCG approach is capable of constructing robust CG models by iteratively optimizing the effective potentials to simultaneously match multiple target properties. We demonstrate our approach by concurrently optimizing bonded and nonbonded potentials of a CG model of polystyrene (PS) melts. The resulting CG-PS model effectively reproduces both the structural characteristics, such as the equilibrium probability distribution of microscopic degrees of freedom and the thermodynamic pressure of the AA counterpart. More importantly, leveraging the multiobjective optimization capability, we develop a precise and efficient CG model for PS melts that is transferable across a wide range of temperatures, i.e., from 400 to 600 K. It is achieved via optimizing a pairwise potential with nonlinear temperature dependence in the CG model to simultaneously match target data from AA-MD simulations at multiple thermodynamic states. The temperature transferable CG-PS model demonstrates its ability to accurately predict the radial distribution functions and density at different temperatures, including those that are not included in the target thermodynamic states. Our work opens up a promising route for developing accurate and transferable CG models of complex soft-matter systems through multiobjective optimization with differentiable simulation.