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

Venkat Kapil1*, David Wilkins1, Jinggang Lan2, Michele Ceriotti1

1 Laboratory of Computational Science and Modelling, Institute of Materials, Ecole Polytechnique Fédérale de Lausanne, Lausanne 1015, Switzerland

2 Department of Chemistry, University of Zürich, Zürich, Switzerland

* Corresponding authors emails: venkat.kapil@gmail.com
DOI10.24435/materialscloud:td-wp [version v2]

Publication date: Nov 23, 2021

How to cite this record

Venkat Kapil, David Wilkins, Jinggang Lan, Michele Ceriotti, Inexpensive modeling of quantum dynamics using path integral generalized Langevin equation thermostats, Materials Cloud Archive 2021.196 (2021), doi: 10.24435/materialscloud:td-wp.

Description

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.

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Keywords

Nuclear quantum effects Vibrational spectra Molecular dynamics EPFL ERC MARVEL

Version history:

2021.196 (version v2) [This version] Nov 23, 2021 DOI10.24435/materialscloud:td-wp
2021.195 (version v1) Nov 22, 2021 DOI10.24435/materialscloud:6z-f5