Accurate Structure-Based Coarse Graining Leads to Consistent Barrier-Crossing Dynamics
Classical molecular dynamics strategies are inherently limited by the molecular-mechanics basis set employed. Here we extend the concept of multisurface dynamics, initially developed to describe electronic transitions in chemical reactions, to 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. A structural criterion for the surface selection effectively introduces coupling beyond the additivity of the Hamiltonian. We illustrate the method through a systematic coarse-graining of two molecular systems that give rise to notoriously challenging many-body potentials of mean force. Incorporating more surfaces leads systematically towards unimodal distributions within each basin, resulting in structural improvements that also yield kinetic consistency.
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@article{Bereau_2018,
doi = {10.1103/physrevlett.121.256002},
url = {https://doi.org/10.1103%2Fphysrevlett.121.256002},
year = 2018,
month = {dec},
publisher = {American Physical Society ({APS})},
volume = {121},
number = {25},
author = {Tristan Bereau and Joseph F. Rudzinski},
title = {Accurate Structure-Based Coarse Graining Leads to Consistent Barrier-Crossing Dynamics},
journal = {Physical Review Letters}
}