Forces and stress in second order MøllerPlesset perturbation theory for condensed phase systems within the resolutionofidentity Gaussian and plane waves approach
Abstract
The forces acting on the atoms as well as the stress tensor are crucial ingredients for calculating the structural and dynamical properties of systems in the condensed phase. Here, these derivatives of the total energy are evaluated for the secondorder MøllerPlesset perturbation energy (MP2) in the framework of the resolution of identity Gaussian and plane waves method, in a way that is fully consistent with how the total energy is computed. This consistency is nontrivial, given the different ways employed to compute Coulomb, exchange, and canonical four center integrals, and allows, for example, for energy conserving dynamics in various ensembles. Based on this formalism, a massively parallel algorithm has been developed for finite and extended system. The designed parallel algorithm displays, with respect to the system size, cubic, quartic, and quintic requirements, respectively, for the memory, communication, and computation. All these requirements are reduced with an increasing number of processes, and the measured performance shows excellent parallel scalability and efficiency up to thousands of nodes. Additionally, the computationally more demanding quintic scaling steps can be accelerated by employing graphics processing units (GPU’s) showing, for large systems, a gain of almost a factor two compared to the standard central processing unitonlymore »
 Authors:
 Department of Chemistry, University of Zürich, Winterthurerstrasse 190, CH8057 Zürich (Switzerland)
 Department of Materials, ETH Zürich, WolfgangPauliStrasse 27, CH8093 Zürich (Switzerland)
 Publication Date:
 OSTI Identifier:
 22416233
 Resource Type:
 Journal Article
 Resource Relation:
 Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 10; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
 Country of Publication:
 United States
 Language:
 English
 Subject:
 37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ALGORITHMS; AMMONIA; ATOMS; BENZENE; CARBON DIOXIDE; COMPUTERIZED SIMULATION; GAIN; MOLECULAR CRYSTALS; MOLECULAR DYNAMICS METHOD; RELAXATION; RESOLUTION; STRESSES; TENSORS; WAVE PROPAGATION
Citation Formats
Del Ben, Mauro, Email: mauro.delben@chem.uzh.ch, Hutter, Jürg, Email: hutter@chem.uzh.ch, and VandeVondele, Joost, Email: Joost.VandeVondele@mat.ethz.ch. Forces and stress in second order MøllerPlesset perturbation theory for condensed phase systems within the resolutionofidentity Gaussian and plane waves approach. United States: N. p., 2015.
Web. doi:10.1063/1.4919238.
Del Ben, Mauro, Email: mauro.delben@chem.uzh.ch, Hutter, Jürg, Email: hutter@chem.uzh.ch, & VandeVondele, Joost, Email: Joost.VandeVondele@mat.ethz.ch. Forces and stress in second order MøllerPlesset perturbation theory for condensed phase systems within the resolutionofidentity Gaussian and plane waves approach. United States. doi:10.1063/1.4919238.
Del Ben, Mauro, Email: mauro.delben@chem.uzh.ch, Hutter, Jürg, Email: hutter@chem.uzh.ch, and VandeVondele, Joost, Email: Joost.VandeVondele@mat.ethz.ch. Mon .
"Forces and stress in second order MøllerPlesset perturbation theory for condensed phase systems within the resolutionofidentity Gaussian and plane waves approach". United States.
doi:10.1063/1.4919238.
@article{osti_22416233,
title = {Forces and stress in second order MøllerPlesset perturbation theory for condensed phase systems within the resolutionofidentity Gaussian and plane waves approach},
author = {Del Ben, Mauro, Email: mauro.delben@chem.uzh.ch and Hutter, Jürg, Email: hutter@chem.uzh.ch and VandeVondele, Joost, Email: Joost.VandeVondele@mat.ethz.ch},
abstractNote = {The forces acting on the atoms as well as the stress tensor are crucial ingredients for calculating the structural and dynamical properties of systems in the condensed phase. Here, these derivatives of the total energy are evaluated for the secondorder MøllerPlesset perturbation energy (MP2) in the framework of the resolution of identity Gaussian and plane waves method, in a way that is fully consistent with how the total energy is computed. This consistency is nontrivial, given the different ways employed to compute Coulomb, exchange, and canonical four center integrals, and allows, for example, for energy conserving dynamics in various ensembles. Based on this formalism, a massively parallel algorithm has been developed for finite and extended system. The designed parallel algorithm displays, with respect to the system size, cubic, quartic, and quintic requirements, respectively, for the memory, communication, and computation. All these requirements are reduced with an increasing number of processes, and the measured performance shows excellent parallel scalability and efficiency up to thousands of nodes. Additionally, the computationally more demanding quintic scaling steps can be accelerated by employing graphics processing units (GPU’s) showing, for large systems, a gain of almost a factor two compared to the standard central processing unitonly case. In this way, the evaluation of the derivatives of the RIMP2 energy can be performed within a few minutes for systems containing hundreds of atoms and thousands of basis functions. With good time to solution, the implementation thus opens the possibility to perform molecular dynamics (MD) simulations in various ensembles (microcanonical ensemble and isobaricisothermal ensemble) at the MP2 level of theory. Geometry optimization, full cell relaxation, and energy conserving MD simulations have been performed for a variety of molecular crystals including NH{sub 3}, CO{sub 2}, formic acid, and benzene.},
doi = {10.1063/1.4919238},
journal = {Journal of Chemical Physics},
number = 10,
volume = 143,
place = {United States},
year = {Mon Sep 14 00:00:00 EDT 2015},
month = {Mon Sep 14 00:00:00 EDT 2015}
}

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