Accurate structure-based coarse-graining leads to consistent barrier-crossing dynamics

Abstract

Structure-based coarse graining of molecular systems offers a systematic route to reproduce the many-body potential of mean force. Unfortunately, common strategies are inherently limited by the molecular mechanics force field employed. Here, we extend the concept of multisurface dynamics, initially developed to describe electronic transitions in chemical reactions, to accurately sample the conformational ensemble of a classical system in equilibrium. In analogy to describing different electronic configurations, a surface-hopping scheme couples distinct conformational basins beyond the additivity of the Hamiltonian. The incorporation of more surfaces leads systematically toward improved cross-correlations. The resulting models naturally achieve consistent long-time dynamics for systems governed by barrier-crossing events.

6 pages, 5 figures

References in corpus (1)

• Consistent interpretation of molecular simulation kinetics using Markov state models biased with external information

Cited by in corpus (6)

• Machine learning for molecular simulation
• Dynamical properties across different coarse-grained models for ionic liquids
• Coarse-grained conformational surface hopping: Methodology and transferability
• BoltzmaNN: Predicting effective pair potentials and equations of state using neural networks
• Reweighting non-equilibrium steady-state dynamics along collective variables
• Broad chemical transferability in structure-based coarse-graining