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Title: A new generation of effective core potentials for correlated calculations

Abstract

Here, we outline ideas on desired properties for a new generation of effective core potentials (ECPs) that will allow valence-only calculations to reach the full potential offered by recent advances in many-body wave function methods. The key improvements include consistent use of correlated methods throughout ECP constructions and improved transferability as required for an accurate description of molecular systems over a range of geometries. The guiding principle is the isospectrality of all-electron and ECP Hamiltonians for a subset of valence states. We illustrate these concepts on a few first- and second-row atoms (B, C, N, O, S), and we obtain higher accuracy in transferability than previous constructions while using semi-local ECPs with a small number of parameters. In addition, the constructed ECPs enable many-body calculations of valence properties with higher (or same) accuracy than their all-electron counterparts with uncorrelated cores. This implies that the ECPs include also some of the impacts of core-core and core-valence correlations on valence properties. The results open further prospects for ECP improvements and refinements.

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2];  [2];  [3];  [2]
+ Show Author Affiliations
  1. North Carolina State Univ., Raleigh, NC (United States); Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  2. North Carolina State Univ., Raleigh, NC (United States)
  3. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1421640
Alternate Identifier(s):
OSTI ID: 1413026
Report Number(s):
SAND-2017-12940J
Journal ID: ISSN 0021-9606; 659151; TRN: US1801536
Grant/Contract Number:  
AC04-94AL85000; N. 4000144475; NA0003525
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 147; Journal Issue: 22; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Bennett, Michael Chandler, Melton, Cody A., Annaberdiyev, Abdulgani, Wang, Guangming, Shulenburger, Luke, and Mitas, Lubos. A new generation of effective core potentials for correlated calculations. United States: N. p., 2017. Web. doi:10.1063/1.4995643.
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Bennett, Michael Chandler, Melton, Cody A., Annaberdiyev, Abdulgani, Wang, Guangming, Shulenburger, Luke, & Mitas, Lubos. A new generation of effective core potentials for correlated calculations. United States. https://doi.org/10.1063/1.4995643
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Bennett, Michael Chandler, Melton, Cody A., Annaberdiyev, Abdulgani, Wang, Guangming, Shulenburger, Luke, and Mitas, Lubos. Tue . "A new generation of effective core potentials for correlated calculations". United States. https://doi.org/10.1063/1.4995643. https://www.osti.gov/servlets/purl/1421640.
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@article{osti_1421640,
title = {A new generation of effective core potentials for correlated calculations},
author = {Bennett, Michael Chandler and Melton, Cody A. and Annaberdiyev, Abdulgani and Wang, Guangming and Shulenburger, Luke and Mitas, Lubos},
abstractNote = {Here, we outline ideas on desired properties for a new generation of effective core potentials (ECPs) that will allow valence-only calculations to reach the full potential offered by recent advances in many-body wave function methods. The key improvements include consistent use of correlated methods throughout ECP constructions and improved transferability as required for an accurate description of molecular systems over a range of geometries. The guiding principle is the isospectrality of all-electron and ECP Hamiltonians for a subset of valence states. We illustrate these concepts on a few first- and second-row atoms (B, C, N, O, S), and we obtain higher accuracy in transferability than previous constructions while using semi-local ECPs with a small number of parameters. In addition, the constructed ECPs enable many-body calculations of valence properties with higher (or same) accuracy than their all-electron counterparts with uncorrelated cores. This implies that the ECPs include also some of the impacts of core-core and core-valence correlations on valence properties. The results open further prospects for ECP improvements and refinements.},
doi = {10.1063/1.4995643},
journal = {Journal of Chemical Physics},
number = 22,
volume = 147,
place = {United States},
year = {Tue Dec 12 00:00:00 EST 2017},
month = {Tue Dec 12 00:00:00 EST 2017}
}
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https://doi.org/10.1063/1.4995643
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