Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model

In this work, we explore the applicability and limitations of the current third order density functional tight binding (DFTB3) formalism for treating transition metal ions using nickel as an example. To be consistent with recent parameterization of DFTB3 for copper, the parametrization for nickel is...

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Autores: Vujovic, Milena, Huynh, Mioy T., Steiner, Sebastian, García Fernández, Pablo (físico)|||0000-0002-4901-0811, Elstner, Marcus, Cui, Qiang, Gruden, Maja
Formato: artículo
Fecha de publicación:2019
País:España
Recursos:Universidad de Cantabria (UC)
Repositorio:UCrea Repositorio Abierto de la Universidad de Cantabria
Idioma:inglés
OAI Identifier:oai:repositorio.unican.es:10902/32617
Acesso em linha:https://hdl.handle.net/10902/32617
Access Level:acceso abierto
Palavra-chave:DFTB3
DFT
Hubbard parameters
Nickel
Spin states
Jahn-Teller distortion
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spelling Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 modelVujovic, MilenaHuynh, Mioy T.Steiner, SebastianGarcía Fernández, Pablo (físico)|||0000-0002-4901-0811Elstner, MarcusCui, QiangGruden, MajaDFTB3DFTHubbard parametersNickelSpin statesJahn-Teller distortionIn this work, we explore the applicability and limitations of the current third order density functional tight binding (DFTB3) formalism for treating transition metal ions using nickel as an example. To be consistent with recent parameterization of DFTB3 for copper, the parametrization for nickel is conducted in a spin-polarized formulation and with orbital-resolved Hubbard parameters and their charge derivatives. The performance of the current parameter set is evaluated based on structural and energetic properties of a set of nickel-containing compounds that involve biologically relevant ligands. Qualitatively similar to findings in previous studies of copper complexes, the DFTB3 results are more reliable for nickel complexes with neutral ligands than for charged ligands; nevertheless, encouraging agreement is noted in comparison to the reference method, B3LYP/aug-cc-pVTZ, especially for structural properties, including cases that exhibit Jahn-Teller distortions; the structures also compare favorably to available X-ray data in the Cambridge Crystallographic Database for a number of nickel-containing compounds. As to limitations, we find it is necessary to use different d shell Hubbard charge derivatives for Ni(I) and Ni(II), due to the distinct electronic configurations for the nickel ion in the respective complexes, and substantial errors are observed for ligand binding energies, especially for charged ligands, d orbital splitting energies and splitting between singlet and triplet spin states for Ni(II) compounds. These observations highlight that future improvement in intra-d correlation and ligand polarization is required to enable the application of the DFTB3 model to complex transition metal ions.This project was supported by the Serbian-German collaboration project (DAAD) number 451-03-01038/2015-09/7 (to MG and ME), the Serbian Ministry of Science under project 172035 (to MG), NIH grant R01-GM106443 (QC) and the Spanish Ministry of Economy and Competitiveness through Grant FIS2015–64886-C5–2-P (P.G.-F.). P.G.-F. recognizes support from Ramón y Cajal Grant RyC-2013–12515.WileyUniversidad de Cantabria20192019-01-01journal articlehttp://purl.org/coar/resource_type/c_6501NAhttp://purl.org/coar/version/c_be7fb7dd8ff6fe43info:eu-repo/semantics/articlehttps://hdl.handle.net/10902/32617Journal of Computational Chemistry, 2019, 40(2), 400-413reponame:UCrea Repositorio Abierto de la Universidad de Cantabriainstname:Universidad de Cantabria (UC)Inglésengopen accesshttp://purl.org/coar/access_right/c_abf2info:eu-repo/semantics/openAccessoai:repositorio.unican.es:10902/326172026-06-02T12:39:31Z
dc.title.none.fl_str_mv Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
title Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
spellingShingle Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
Vujovic, Milena
DFTB3
DFT
Hubbard parameters
Nickel
Spin states
Jahn-Teller distortion
title_short Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
title_full Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
title_fullStr Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
title_full_unstemmed Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
title_sort Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
dc.creator.none.fl_str_mv Vujovic, Milena
Huynh, Mioy T.
Steiner, Sebastian
García Fernández, Pablo (físico)|||0000-0002-4901-0811
Elstner, Marcus
Cui, Qiang
Gruden, Maja
author Vujovic, Milena
author_facet Vujovic, Milena
Huynh, Mioy T.
Steiner, Sebastian
García Fernández, Pablo (físico)|||0000-0002-4901-0811
Elstner, Marcus
Cui, Qiang
Gruden, Maja
author_role author
author2 Huynh, Mioy T.
Steiner, Sebastian
García Fernández, Pablo (físico)|||0000-0002-4901-0811
Elstner, Marcus
Cui, Qiang
Gruden, Maja
author2_role author
author
author
author
author
author
dc.contributor.none.fl_str_mv Universidad de Cantabria
dc.subject.none.fl_str_mv DFTB3
DFT
Hubbard parameters
Nickel
Spin states
Jahn-Teller distortion
topic DFTB3
DFT
Hubbard parameters
Nickel
Spin states
Jahn-Teller distortion
description In this work, we explore the applicability and limitations of the current third order density functional tight binding (DFTB3) formalism for treating transition metal ions using nickel as an example. To be consistent with recent parameterization of DFTB3 for copper, the parametrization for nickel is conducted in a spin-polarized formulation and with orbital-resolved Hubbard parameters and their charge derivatives. The performance of the current parameter set is evaluated based on structural and energetic properties of a set of nickel-containing compounds that involve biologically relevant ligands. Qualitatively similar to findings in previous studies of copper complexes, the DFTB3 results are more reliable for nickel complexes with neutral ligands than for charged ligands; nevertheless, encouraging agreement is noted in comparison to the reference method, B3LYP/aug-cc-pVTZ, especially for structural properties, including cases that exhibit Jahn-Teller distortions; the structures also compare favorably to available X-ray data in the Cambridge Crystallographic Database for a number of nickel-containing compounds. As to limitations, we find it is necessary to use different d shell Hubbard charge derivatives for Ni(I) and Ni(II), due to the distinct electronic configurations for the nickel ion in the respective complexes, and substantial errors are observed for ligand binding energies, especially for charged ligands, d orbital splitting energies and splitting between singlet and triplet spin states for Ni(II) compounds. These observations highlight that future improvement in intra-d correlation and ligand polarization is required to enable the application of the DFTB3 model to complex transition metal ions.
publishDate 2019
dc.date.none.fl_str_mv 2019
2019-01-01
dc.type.none.fl_str_mv journal article
http://purl.org/coar/resource_type/c_6501
NA
http://purl.org/coar/version/c_be7fb7dd8ff6fe43
dc.type.openaire.fl_str_mv info:eu-repo/semantics/article
format article
dc.identifier.none.fl_str_mv https://hdl.handle.net/10902/32617
url https://hdl.handle.net/10902/32617
dc.language.none.fl_str_mv Inglés
eng
language_invalid_str_mv Inglés
language eng
dc.rights.none.fl_str_mv open access
http://purl.org/coar/access_right/c_abf2
dc.rights.openaire.fl_str_mv info:eu-repo/semantics/openAccess
rights_invalid_str_mv open access
http://purl.org/coar/access_right/c_abf2
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Wiley
publisher.none.fl_str_mv Wiley
dc.source.none.fl_str_mv Journal of Computational Chemistry, 2019, 40(2), 400-413
reponame:UCrea Repositorio Abierto de la Universidad de Cantabria
instname:Universidad de Cantabria (UC)
instname_str Universidad de Cantabria (UC)
reponame_str UCrea Repositorio Abierto de la Universidad de Cantabria
collection UCrea Repositorio Abierto de la Universidad de Cantabria
repository.name.fl_str_mv
repository.mail.fl_str_mv
_version_ 1869424050213748736
score 15,300719

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