Fine Tuning Classical and Quantum Molecular Dynamics using a Generalized Langevin Equation
arXiv:1704.05099 · doi:10.1063/1.4990536
Abstract
Generalized Langevin Equation (GLE) thermostats have been used very effectively as a tool to manipulate and optimize the sampling of thermodynamic ensembles and the associated static properties. Here we show that a similar, exquisite level of control can be achieved for the dynamical properties computed from thermostatted trajectories. By developing quantitative measures of the disturbance induced by the GLE to the Hamiltonian dynamics of a harmonic oscillator, we show that these analytical results accurately predict the behavior of strongly anharmonic systems. We also show that it is possible to correct, to a significant extent, the effects of the GLE term onto the corresponding microcanonical dynamics, which puts on more solid grounds the use of non-equilibrium Langevin dynamics to approximate quantum nuclear effects and could help improve the prediction of dynamical quantities from techniques that use a Langevin term to stabilize dynamics. Finally we address the use of thermostats in the context of approximate path-integral-based models of quantum nuclear dynamics. We demonstrate that a custom-tailored GLE can alleviate some of the artifacts associated with these techniques, improving the quality of results for the modelling of vibrational dynamics of molecules, liquids and solids.
References in corpus (13)
- How van der Waals interactions determine the unique properties of water
- An Efficient and Accurate Car-Parrinello-like Approach to Born-Oppenheimer Molecular Dynamics
- How to remove the spurious resonances from ring polymer molecular dynamics
- Nuclear quantum effects in solids using a colored-noise thermostat
- Colored-noise thermostats à la carte
- Full dimensional (15D) quantum-dynamical simulation of the protonated water-dimer II: infrared spectrum and vibrational dynamics
- Efficient multiple time scale molecular dynamics: using colored noise thermostats to stabilize resonances
- Relation of centroid molecular dynamics and ring-polymer molecular dynamics to exact quantum dynamics
- On the Consistency of Approximate Quantum Dynamics Simulation Methods for Vibrational Spectra in the Condensed Phase
- Unexpectedly high pressure for molecular dissociation in liquid hydrogen by a reliable electronic simulation
- High Order Path Integrals Made Easy
- How to obtain thermostatted ring polymer molecular dynamics from exact quantum dynamics and when to use it
- Uncertainty quantification for generalized Langevin dynamics
Cited by in corpus (30)
- Nuclear quantum effects enter the mainstream
- i-PI 2.0: A Universal Force Engine for Advanced Molecular Simulations
- Elucidating the NuclearQuantum Dynamics of Intramolecular Double Hydrogen Transfer in Porphycene
- i-PI 3.0: a flexible and efficient framework for advanced atomistic simulations
- Cayley modification for strongly stable path-integral and ring-polymer molecular dynamics
- Path-integral dynamics of water using curvilinear centroids
- Inexpensive modelling of quantum dynamics using path integral generalized Langevin equation thermostats
- Dimension-free path-integral molecular dynamics without preconditioning
- All-Electron, Real-Space Perturbation Theory for Homogeneous Electric Fields: Theory, Implementation, and Application within DFT
- Quantum dynamics using path integral coarse-graining
- Microcanonical and finite temperature ab initio molecular dynamics simulations on quantum computers
- Fully First-Principles Surface Spectroscopy with Machine Learning
- Incorporating Nuclear Quantum Effects in Molecular Dynamics with a Constrained Minimized Energy Surface
- A generalized class of strongly stable and dimension-free T-RPMD integrators
- Two-dimensional infrared-Raman spectroscopy as a probe of water's tetrahedrality
- Progress and Challenges in Ab Initio Simulations of Quantum Nuclei in Weakly Bonded Systems
- Nuclear Quantum Effects in liquid water at near classical computational cost using the adaptive Quantum Thermal Bath
- Reduced Rovibrational Coupling Cartesian Dynamics for Semiclassical Calculations: Application to the Spectrum of the Zundel Cation
- Mean-field Matsubara dynamics: Analysis of path-integral curvature effects in rovibrational spectra
- Testing the quasicentroid molecular dynamics method on gas-phase ammonia
- Improving Condensed Phase Water Dynamics with Explicit Nuclear Quantum Effects: the Polarizable Q-AMOEBA Force Field
- Probing anharmonic phonons by quantum correlators: A path integral approach
- Fast-Forward Langevin Dynamics with Momentum Flips
- Effective Mass Path Integral Simulations of Quasiparticles in Condensed Phases
- Improved torque estimator for condensed-phase quasicentroid molecular dynamics
- Path Integral Brownian Chain Molecular Dynamics: A Simple Approximation of Quantum Vibrational Dynamics
- The quantum nature of ubiquitous vibrational features revealed for ethylene glycol
- Nuclear Quantum Effects in Multi-Step Condensed Matter Chemistry: A Path Integral Molecular Dynamics Study of Thermal Decomposition
- Connection between water's dynamical and structural properties: insights from ab initio simulations
- Quantitative Molecular Simulations