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Title: Pseudo-fragment approach for extended systems derived from linear-scaling DFT

Abstract

We present a computational approach which is tailored for reducing the complexity of the description of extended systems at the density functional theory level. We define a recipe for generating a set of localized basis functions which arc optimized either for the accurate description of pristine, bulk-like Wannier functions, or for the in situ treatment of deformations induced by defective constituents such as boundaries or impurities. Our method enables one to identify the regions of an extended system which require dedicated optimization of the Kohn-Sham degrees of freedom, and provides the user with a reliable estimation of the errors-if any-induced by the locality of the approach. Such a method facilitates on the one hand an effective reduction of the computational degrees of freedom needed to simulate systems at the nanoscale, while in turn providing a description that can be straightforwardly put in relation to effective models, like tight binding Hamiltonians. In conclusion, we present our methodology with SiC nanotube-like cages as a test bed. Nonetheless, the wavelet-based method employed in this paper makes possible calculation of systems with different dimensionalities, including slabs and fully periodic systems.

Authors:
ORCiD logo [1]; ORCiD logo [2]
  1. Imperial College London, London (United Kingdom); Argonne National Lab. (ANL), Argonne, IL (United States)
  2. Univ. Grenoble Alpes, Grenoble (France)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Engineering and Physical Sciences Research Council (EPSRC); Argonne National Laboratory, Argonne Leadership Computing Facility; USDOE
OSTI Identifier:
1542150
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physics. Condensed Matter
Additional Journal Information:
Journal Volume: 31; Journal Issue: 28; Journal ID: ISSN 0953-8984
Publisher:
IOP Publishing
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; fragment approach; linear scaling density functional theory; nanotubes

Citation Formats

Ratcliff, Laura E., and Genovese, Luigi. Pseudo-fragment approach for extended systems derived from linear-scaling DFT. United States: N. p., 2019. Web. doi:10.1088/1361-648X/ab1664.
Ratcliff, Laura E., & Genovese, Luigi. Pseudo-fragment approach for extended systems derived from linear-scaling DFT. United States. doi:10.1088/1361-648X/ab1664.
Ratcliff, Laura E., and Genovese, Luigi. Tue . "Pseudo-fragment approach for extended systems derived from linear-scaling DFT". United States. doi:10.1088/1361-648X/ab1664. https://www.osti.gov/servlets/purl/1542150.
@article{osti_1542150,
title = {Pseudo-fragment approach for extended systems derived from linear-scaling DFT},
author = {Ratcliff, Laura E. and Genovese, Luigi},
abstractNote = {We present a computational approach which is tailored for reducing the complexity of the description of extended systems at the density functional theory level. We define a recipe for generating a set of localized basis functions which arc optimized either for the accurate description of pristine, bulk-like Wannier functions, or for the in situ treatment of deformations induced by defective constituents such as boundaries or impurities. Our method enables one to identify the regions of an extended system which require dedicated optimization of the Kohn-Sham degrees of freedom, and provides the user with a reliable estimation of the errors-if any-induced by the locality of the approach. Such a method facilitates on the one hand an effective reduction of the computational degrees of freedom needed to simulate systems at the nanoscale, while in turn providing a description that can be straightforwardly put in relation to effective models, like tight binding Hamiltonians. In conclusion, we present our methodology with SiC nanotube-like cages as a test bed. Nonetheless, the wavelet-based method employed in this paper makes possible calculation of systems with different dimensionalities, including slabs and fully periodic systems.},
doi = {10.1088/1361-648X/ab1664},
journal = {Journal of Physics. Condensed Matter},
number = 28,
volume = 31,
place = {United States},
year = {2019},
month = {4}
}

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