Inexpensive modeling of quantum dynamics using path integral generalized Langevin equation thermostats

Venkat Kapil*, David M. Wilkins, Jinggang Lan, Michele Ceriotti

*Corresponding author for this work

Research output: Contribution to journalArticle

2 Citations (Scopus)

Abstract

The properties of molecules and materials containing light nuclei are affected by their quantum mechanical nature. Accurate modeling of these quantum nuclear effects requires computationally demanding path integral techniques. Considerable success has been achieved in reducing the cost of such simulations by using generalized Langevin dynamics to induce frequency-dependent fluctuations. Path integral generalized Langevin equation methods, however, have this far been limited to the study of static, thermodynamic properties due to the large perturbation to the system's dynamics induced by the aggressive thermostatting. Here, we introduce a post-processing scheme, based on analytical estimates of the dynamical perturbation induced by the generalized Langevin dynamics, which makes it possible to recover meaningful time correlation properties from a thermostatted trajectory. We show that this approach yields spectroscopic observables for model and realistic systems that have an accuracy comparable to much more demanding approximate quantum dynamics techniques based on full path integral simulations.

Original languageEnglish
Article number124104
JournalJournal of Chemical Physics
Volume152
Issue number12
DOIs
Publication statusPublished - 24 Mar 2020
Externally publishedYes

Keywords

  • Spectroscopy
  • Molecular Dynamics
  • Path Integrals
  • Water
  • Machine Learning
  • Langevin Dynamics
  • Nuclear Quantum Effects

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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