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New generation of effective core potentials from correlated calculations: 2nd row elements
Abstract
Very recently, we have introduced correlation consistent effective core potentials (ccECPs) derived from many-body approaches with the main target being its use in explicitly correlated methods but also in mainstream approaches. The ccECPs are based on reproducing excitation energies for a subset of valence states, i.e., achieving a near-isospectrality between the original and pseudo Hamiltonians. Additionally, binding curves of dimer molecules have been used for refinement and overall improvement of transferability over a range of bond lengths. Here we apply similar ideas to the second row elements and study several aspects of the constructions in order to find the optimal (or nearly-optimal) solutions within the chosen ECP forms with 3s, 3p valence space (Ne-core). New constructions exhibit accurate low-lying atomic excitations and equilibrium molecular bonds (on average within ≈ 0.03 eV and 3 mA), however, the errors for A1 and Si oxide molecules at short bond lengths are notably larger for both ours and existing ECPs. Assuming this limitation, our ccECPs show a systematic balance between the criteria of atomic spectra accuracy and transferability for molecular bonds. Finally, in order to provide another option with much higher uniform accuracy, we also construct He-core ECPs for the whole row with typicalmore »
- Authors:
-
- North Carolina State Univ., Raleigh, NC (United States). Department of Physics; Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
- North Carolina State Univ., Raleigh, NC (United States). Department of Physics
- 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) (SC-22). Materials Sciences & Engineering Division; USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1441470
- Alternate Identifier(s):
- OSTI ID: 1470794
- Report Number(s):
- SAND-2018-4735J
Journal ID: ISSN 0021-9606; 662779; TRN: US1900963
- Grant/Contract Number:
- AC04-94AL85000; NA0003525
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Physics
- Additional Journal Information:
- Journal Volume: 149; Journal Issue: 10; 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; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Bennett, Michael Chandler, Melton, Cody A., Annaberdiyev, Abdulgani, Wang, Guangming, Shulenburger, Luke, and Mitas, Lubos. New generation of effective core potentials from correlated calculations: 2nd row elements. United States: N. p., 2018.
Web. doi:10.1063/1.5038135.
Bennett, Michael Chandler, Melton, Cody A., Annaberdiyev, Abdulgani, Wang, Guangming, Shulenburger, Luke, & Mitas, Lubos. New generation of effective core potentials from correlated calculations: 2nd row elements. United States. doi:10.1063/1.5038135.
Bennett, Michael Chandler, Melton, Cody A., Annaberdiyev, Abdulgani, Wang, Guangming, Shulenburger, Luke, and Mitas, Lubos. Fri .
"New generation of effective core potentials from correlated calculations: 2nd row elements". United States. doi:10.1063/1.5038135.
@article{osti_1441470,
title = {New generation of effective core potentials from correlated calculations: 2nd row elements},
author = {Bennett, Michael Chandler and Melton, Cody A. and Annaberdiyev, Abdulgani and Wang, Guangming and Shulenburger, Luke and Mitas, Lubos},
abstractNote = {Very recently, we have introduced correlation consistent effective core potentials (ccECPs) derived from many-body approaches with the main target being its use in explicitly correlated methods but also in mainstream approaches. The ccECPs are based on reproducing excitation energies for a subset of valence states, i.e., achieving a near-isospectrality between the original and pseudo Hamiltonians. Additionally, binding curves of dimer molecules have been used for refinement and overall improvement of transferability over a range of bond lengths. Here we apply similar ideas to the second row elements and study several aspects of the constructions in order to find the optimal (or nearly-optimal) solutions within the chosen ECP forms with 3s, 3p valence space (Ne-core). New constructions exhibit accurate low-lying atomic excitations and equilibrium molecular bonds (on average within ≈ 0.03 eV and 3 mA), however, the errors for A1 and Si oxide molecules at short bond lengths are notably larger for both ours and existing ECPs. Assuming this limitation, our ccECPs show a systematic balance between the criteria of atomic spectra accuracy and transferability for molecular bonds. Finally, in order to provide another option with much higher uniform accuracy, we also construct He-core ECPs for the whole row with typical discrepancies of ≈ 0.01 eV or smaller.},
doi = {10.1063/1.5038135},
journal = {Journal of Chemical Physics},
number = 10,
volume = 149,
place = {United States},
year = {2018},
month = {9}
}
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Works referenced in this record:
Ab initio relativistic effective potentials with spin?orbit operators. I. Li through Ar
journal, March 1985
- Fernandez Pacios, Luis; Christiansen, P. A.
- The Journal of Chemical Physics, Vol. 82, Issue 6, p. 2664-2671