The influence of multi-dimensionality and off-diagonal non-Markovian friction coupling on coarse-grained dynamics

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Main Authors: Kiefer, Henrik, Ayaz, Cihan, Dalton, Benjamin A., Netz, Roland R.
Format: Preprint
Published: 2025
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author Kiefer, Henrik
Ayaz, Cihan
Dalton, Benjamin A.
Netz, Roland R.
author_facet Kiefer, Henrik
Ayaz, Cihan
Dalton, Benjamin A.
Netz, Roland R.
contents Coarse-graining complex molecular systems to lower-dimensional reaction coordinates is a powerful approach for capturing their effective dynamics. The generalized Langevin equation (GLE) provides an exact framework for modeling coarse-grained dynamics, and is particularly useful when non-Markovian effects are significant. While one-dimensional GLE models are commonly used, many systems require multi-dimensional reaction coordinates to account for coupled dynamics. Here, we study the GLE formalism for multi-dimensional reaction coordinates, incorporating a memory matrix to quantify non-Markovian frictional coupling between coordinates, and a multi-dimensional potential. Using the GLE model, in conjunction with a multi-dimensional Markovian embedding scheme, we investigate different systems that are characterized by two-dimensional reaction coordinates, namely the dihedral dynamics of pentane and alanine dipeptide, obtained from molecular dynamics simulations in explicit water. We identify significant off-diagonal friction couplings arising from intramolecular and hydrodynamic interactions. Unlike previous studies, our results highlight the critical role of different terms in the multi-dimensional GLE in accurately capturing key dynamical properties, including mean first-passage times and mean-squared displacements, particularly in systems with coupled non-Markovian coordinates.
format Preprint
id arxiv_https___arxiv_org_abs_2506_05966
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle The influence of multi-dimensionality and off-diagonal non-Markovian friction coupling on coarse-grained dynamics
Kiefer, Henrik
Ayaz, Cihan
Dalton, Benjamin A.
Netz, Roland R.
Chemical Physics
Statistical Mechanics
Coarse-graining complex molecular systems to lower-dimensional reaction coordinates is a powerful approach for capturing their effective dynamics. The generalized Langevin equation (GLE) provides an exact framework for modeling coarse-grained dynamics, and is particularly useful when non-Markovian effects are significant. While one-dimensional GLE models are commonly used, many systems require multi-dimensional reaction coordinates to account for coupled dynamics. Here, we study the GLE formalism for multi-dimensional reaction coordinates, incorporating a memory matrix to quantify non-Markovian frictional coupling between coordinates, and a multi-dimensional potential. Using the GLE model, in conjunction with a multi-dimensional Markovian embedding scheme, we investigate different systems that are characterized by two-dimensional reaction coordinates, namely the dihedral dynamics of pentane and alanine dipeptide, obtained from molecular dynamics simulations in explicit water. We identify significant off-diagonal friction couplings arising from intramolecular and hydrodynamic interactions. Unlike previous studies, our results highlight the critical role of different terms in the multi-dimensional GLE in accurately capturing key dynamical properties, including mean first-passage times and mean-squared displacements, particularly in systems with coupled non-Markovian coordinates.
title The influence of multi-dimensionality and off-diagonal non-Markovian friction coupling on coarse-grained dynamics
topic Chemical Physics
Statistical Mechanics
url https://arxiv.org/abs/2506.05966