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Title: From plane waves to local Gaussians for the simulation of correlated periodic systems

Here, we present a simple, robust, and black-box approach to the implementation and use of local, periodic, atom-centered Gaussian basis functions within a plane wave code, in a computationally efficient manner. The procedure outlined is based on the representation of the Gaussians within a finite bandwidth by their underlying plane wave coefficients. The core region is handled within the projected augment wave framework, by pseudizing the Gaussian functions within a cutoff radius around each nucleus, smoothing the functions so that they are faithfully represented by a plane wave basis with only moderate kinetic energy cutoff. To mitigate the effects of the basis set superposition error and incompleteness at the mean-field level introduced by the Gaussian basis, we also propose a hybrid approach, whereby the complete occupied space is first converged within a large plane wave basis, and the Gaussian basis used to construct a complementary virtual space for the application of correlated methods. We demonstrate that these pseudized Gaussians yield compact and systematically improvable spaces with an accuracy comparable to their non-pseudized Gaussian counterparts. A key advantage of the described method is its ability to efficiently capture and describe electronic correlation effects of weakly bound and low-dimensional systems, where planemore » waves are not sufficiently compact or able to be truncated without unphysical artifacts. We investigate the accuracy of the pseudized Gaussians for the water dimer interaction, neon solid, and water adsorption on a LiH surface, at the level of second-order Møller–Plesset perturbation theory.« less
Authors:
 [1] ;  [2] ;  [3] ;  [2]
  1. King's College London (United Kingdom). Dept. of Physics
  2. Max Planck Inst. for Solid State Research, Stuttgart (Germany)
  3. Princeton Univ., Princeton, NJ (United States). Frick Lab. and Dept. of Chemistry
Publication Date:
Grant/Contract Number:
SC0010530; SC0008624
Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 8; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Research Org:
Princeton Univ., NJ (United States)
Sponsoring Org:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21). Scientific Discovery through Advanced Computing (SciDAC); Royal Society (United Kingdom)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; statistical properties; basis sets; number theory; electron correlation calculations; mean field theory; set theory; manifolds; adsorption; wave functions; equations of state
OSTI Identifier:
1467868
Alternate Identifier(s):
OSTI ID: 1310831

Booth, George H., Tsatsoulis, Theodoros, Chan, Garnet Kin-Lic, and Grüneis, Andreas. From plane waves to local Gaussians for the simulation of correlated periodic systems. United States: N. p., Web. doi:10.1063/1.4961301.
Booth, George H., Tsatsoulis, Theodoros, Chan, Garnet Kin-Lic, & Grüneis, Andreas. From plane waves to local Gaussians for the simulation of correlated periodic systems. United States. doi:10.1063/1.4961301.
Booth, George H., Tsatsoulis, Theodoros, Chan, Garnet Kin-Lic, and Grüneis, Andreas. 2016. "From plane waves to local Gaussians for the simulation of correlated periodic systems". United States. doi:10.1063/1.4961301. https://www.osti.gov/servlets/purl/1467868.
@article{osti_1467868,
title = {From plane waves to local Gaussians for the simulation of correlated periodic systems},
author = {Booth, George H. and Tsatsoulis, Theodoros and Chan, Garnet Kin-Lic and Grüneis, Andreas},
abstractNote = {Here, we present a simple, robust, and black-box approach to the implementation and use of local, periodic, atom-centered Gaussian basis functions within a plane wave code, in a computationally efficient manner. The procedure outlined is based on the representation of the Gaussians within a finite bandwidth by their underlying plane wave coefficients. The core region is handled within the projected augment wave framework, by pseudizing the Gaussian functions within a cutoff radius around each nucleus, smoothing the functions so that they are faithfully represented by a plane wave basis with only moderate kinetic energy cutoff. To mitigate the effects of the basis set superposition error and incompleteness at the mean-field level introduced by the Gaussian basis, we also propose a hybrid approach, whereby the complete occupied space is first converged within a large plane wave basis, and the Gaussian basis used to construct a complementary virtual space for the application of correlated methods. We demonstrate that these pseudized Gaussians yield compact and systematically improvable spaces with an accuracy comparable to their non-pseudized Gaussian counterparts. A key advantage of the described method is its ability to efficiently capture and describe electronic correlation effects of weakly bound and low-dimensional systems, where plane waves are not sufficiently compact or able to be truncated without unphysical artifacts. We investigate the accuracy of the pseudized Gaussians for the water dimer interaction, neon solid, and water adsorption on a LiH surface, at the level of second-order Møller–Plesset perturbation theory.},
doi = {10.1063/1.4961301},
journal = {Journal of Chemical Physics},
number = 8,
volume = 145,
place = {United States},
year = {2016},
month = {8}
}

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