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Title: Combining Pseudopotential and All Electron Density Functional Theory for the Efficient Calculation of Core Spectra Using a Multiresolution Approach

Abstract

Broadly speaking, the calculation of core spectra such as electron energy loss spectra (EELS) at the level of density functional theory (DFT) usually relies on one of two approaches: conceptually more complex but computationally efficient projector augmented wave based approaches or more straightforward but computationally more intensive all electron (AE) based approaches. In this work we present an alternative method, which aims to find a middle ground between the two. Specifically, we have implemented an approach in the multiwavelet MADNESS molecular DFT code that permits a combination of atoms treated at the AE and pseudopotential (PSP) level. Atoms for which one wishes to calculate the core edges are thus treated at an AE level, while the remainder can be treated at the PSP level. This is made possible thanks to the multiresolution approach of MADNESS, which permits accurate and efficient calculations at both the AE and PSP level. Through examples of a small molecule and a carbon nanotube, this study demonstrates the potential applications of our approach.

Authors:
ORCiD logo [1];  [2];  [3];  [3]
+ Show Author Affiliations
  1. Imperial College of London, London (United Kingdom). Dept. of Materials; Argonne National Lab. (ANL), Argonne, IL (United States). Argonne Leadership Computing Facility
  2. Stony Brook Univ., Stony Brook, NY (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Argonne Leadership Computing Facility, and Computational Science Division
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1531170
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 123; Journal Issue: 20; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Ratcliff, Laura E., Thornton, W. Scott, Mayagoitia, Álvaro Vázquez, and Romero, Nichols A. Combining Pseudopotential and All Electron Density Functional Theory for the Efficient Calculation of Core Spectra Using a Multiresolution Approach. United States: N. p., 2019. Web. doi:10.1021/acs.jpca.8b11310.
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Ratcliff, Laura E., Thornton, W. Scott, Mayagoitia, Álvaro Vázquez, & Romero, Nichols A. Combining Pseudopotential and All Electron Density Functional Theory for the Efficient Calculation of Core Spectra Using a Multiresolution Approach. United States. https://doi.org/10.1021/acs.jpca.8b11310
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Ratcliff, Laura E., Thornton, W. Scott, Mayagoitia, Álvaro Vázquez, and Romero, Nichols A. Tue . "Combining Pseudopotential and All Electron Density Functional Theory for the Efficient Calculation of Core Spectra Using a Multiresolution Approach". United States. https://doi.org/10.1021/acs.jpca.8b11310. https://www.osti.gov/servlets/purl/1531170.
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@article{osti_1531170,
title = {Combining Pseudopotential and All Electron Density Functional Theory for the Efficient Calculation of Core Spectra Using a Multiresolution Approach},
author = {Ratcliff, Laura E. and Thornton, W. Scott and Mayagoitia, Álvaro Vázquez and Romero, Nichols A.},
abstractNote = {Broadly speaking, the calculation of core spectra such as electron energy loss spectra (EELS) at the level of density functional theory (DFT) usually relies on one of two approaches: conceptually more complex but computationally efficient projector augmented wave based approaches or more straightforward but computationally more intensive all electron (AE) based approaches. In this work we present an alternative method, which aims to find a middle ground between the two. Specifically, we have implemented an approach in the multiwavelet MADNESS molecular DFT code that permits a combination of atoms treated at the AE and pseudopotential (PSP) level. Atoms for which one wishes to calculate the core edges are thus treated at an AE level, while the remainder can be treated at the PSP level. This is made possible thanks to the multiresolution approach of MADNESS, which permits accurate and efficient calculations at both the AE and PSP level. Through examples of a small molecule and a carbon nanotube, this study demonstrates the potential applications of our approach.},
doi = {10.1021/acs.jpca.8b11310},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 20,
volume = 123,
place = {United States},
year = {Tue May 07 00:00:00 EDT 2019},
month = {Tue May 07 00:00:00 EDT 2019}
}
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https://doi.org/10.1021/acs.jpca.8b11310
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