Efficient stochastic thermostatting of path integral molecular dynamics.
By Michele Ceriotti, Michele Parrinello, Thomas E. Markland, David E. Manolopoulos. Journal of Chemical Physics, 2010
367 citations recorded by the source corpus.
The path integral molecular dynamics (PIMD) method provides a convenient way to compute the quantum mechanical structural and thermodynamic properties of condensed phase systems at the expense of introducing an additional set of high frequency normal modes on top of the physical vibrations of the system. Efficiently sampling such a wide range of frequencies provides a considerable thermostatting challenge. Here we introduce a simple stochastic path integral Langevin equation (PILE) thermostat which exploits an analytic knowledge of the free path integral normal mode frequencies. We also apply a recently developed colored noise thermostat based on a generalized Langevin equation (GLE), which automatically achieves a similar, frequency-optimized sampling. The sampling efficiencies of these thermostats are compared with that of the more conventional Nosé-Hoover chain (NHC) thermostat for a number of physically relevant properties of the liquid water and hydrogen-in-palladium systems. In nearly every case, the new PILE thermostat is found to perform just as well as the NHC thermostat while allowing for a computationally more efficient implementation. The GLE thermostat also proves to be very robust delivering a near-optimum sampling efficiency in all of the cases considered. We suspect that these simple stochastic thermostats will therefore find useful application in many future PIMD simulations.
Subfields: Atomic and Molecular Physics, and Optics, Spectroscopy
View Paper: https://www.semanticscholar.org/paper/3fb2bd834f54f2597c43c2473dc018de7216c345
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In Atomic and Molecular Physics, and Optics
- Carlo Pierleoni
- Miguel A. Morales
- Thomas E. Markland
- Thomas F. Miller
- Scott Habershon
- Jeffrey M. McMahon
- David M. Ceperley
- Tim Dockhorn
In Spectroscopy
Citations in the corpus
- Score-Based Generative Modeling with Critically-Damped Langevin Diffusion (2021, methodology): “The same techniques have been used to derive molecular dynamics algorithms (Tuckerman et al., 1992; Bussi & Parrinello, 2007; Ceriotti et al., 2010; Leimkuhler & Matthews, 2013; 2015; Kreis et al., 2017).”
- Ring-polymer molecular dynamics: quantum effects in chemical dynamics from classical trajectories in an extended phase space. (2013, background): “Spurious Frequencies After a normal mode transformation (57, 58, 97), the ring-polymer Hamiltonian for a onedimensional harmonic oscillator with frequency ω can be written as”
- The Properties of Hydrogen and Helium Under Extreme Conditions (2011, methodology): “Recent developments by Ceriotti M., et al. (Ceriotti et al., 2011, 2010) represent a very promising alternative to thermalize PIMD simulations efficiently using generalized Langevin equations.”