Nonequilibrium friction and free energy estimates for kinetic coarse-graining -- Driven particles in responsive media
arXiv:2501.18484 · doi:10.1063/5.0261459
Abstract
Predicting the molecular friction and energy landscapes under nonequilibrium conditions is key to coarse-graining the dynamics of selective solute transport through complex, fluctuating and responsive media, e.g., polymeric materials such as hydrogels, cellular membranes or ion channels. The analysis of equilibrium ensembles already allows such a coarse-graining for very mild nonequilibrium conditions. Yet in the presence of stronger external driving and/or inhomogeneous setups, the transport process is governed apart from a potential of mean force also by a nontrivial position- and velocity-dependent friction. It is therefore important to find suitable and efficient methods to estimate the mean force and the friction landscape, which then can be used in a low-dimensional, coarse-grained Langevin framework to predict the system's transport properties and timescales. In this work, we evaluate different coarse-graining approaches based on constant-velocity constraint simulations for generating such estimates using two model systems, which are a 1D responsive barrier as a minimalistic model and a single tracer driven through a 3D bead-spring polymer membrane as a more sophisticated problem. Finally, we demonstrate that the estimates from 3D constant-velocity simulations yield the correct velocity-dependent friction, which can be directly utilized for coarse-grained (1D) Langevin simulations with constant external driving forces.
Seven Figures. This preprint is the unedited version of a manuscript that has been published in J. Chem. Phys (see journal reference) and can be downloaded for private use only. Copyright with the authors and AIP Publishing
References in corpus (16)
- Iterative Reconstruction of Memory Kernels
- Active and Nonlinear Microrheology in Dense Colloidal Suspensions
- Coarse-Grained Modelling Out of Equilibrium
- Catalyzed bimolecular reactions in responsive nanoreactors
- Emergence of molecular friction in liquids: bridging between the atomistic and hydrodynamic pictures
- Superadiabatic forces in Brownian many-body dynamics
- On the dynamics of reaction coordinates in classical, time-dependent, many-body processes
- Active diffusion of self-propelled particles in flexible polymer networks
- Tuning the Selective Permeability of Polydisperse Polymer Networks
- Generalized Langevin dynamics simulation with non-stationary memory kernels: How to make noise
- Predicting ion channel conductance via dissipation-corrected targeted molecular dynamics and Langevin equation simulations
- Transport in polymer membranes beyond linear response: Controlling permselectivity by the driving force
- Path separation of dissipation-corrected targeted molecular dynamics simulations of protein-ligand unbinding
- The non-equilibrium solvent response force: What happens if you push a Brownian particle
- Molecular origin of driving-dependent friction in fluids
- Feedback-controlled solute transport through chemo-responsive polymer membranes