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Published in

American Institute of Physics, The Journal of Chemical Physics, 21(153), p. 214110, 2020

DOI: 10.1063/5.0031249

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Coarse-grained conformational surface hopping: Methodology and transferability

Journal article published in 2020 by Joseph F. Rudzinski ORCID, Tristan Bereau ORCID
This paper was not found in any repository, but could be made available legally by the author.
This paper was not found in any repository, but could be made available legally by the author.

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Abstract

Coarse-grained (CG) conformational surface hopping (SH) adapts the concept of multisurface dynamics, initially developed to describe electronic transitions in chemical reactions, to accurately describe classical molecular dynamics at a reduced level. The SH scheme couples distinct conformational basins (states), each described by its own force field (surface), resulting in a significant improvement of the approximation to the many-body potential of mean force [T. Bereau and J. F. Rudzinski, Phys. Rev. Lett. 121, 256002 (2018)]. The present study first describes CG SH in more detail, through both a toy model and a three-bead model of hexane. We further extend the methodology to non-bonded interactions and report its impact on liquid properties. Finally, we investigate the transferability of the surfaces to distinct systems and thermodynamic state points, through a simple tuning of the state probabilities. In particular, applications to variations in temperature and chemical composition show good agreement with reference atomistic calculations, introducing a promising “weak-transferability regime,” where CG force fields can be shared across thermodynamic and chemical neighborhoods.