TY  - JOUR
AU  - Vujović, M.
AU  - Huynh, M.
AU  - Steiner, S.
AU  - Garcia-Fernandez, Pablo
AU  - Elstner, Marcus
AU  - Cui, Qiang
AU  - Gruden-Pavlović, Maja
PY  - 2019
UR  - https://cherry.chem.bg.ac.rs/handle/123456789/353
AB  - 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. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.
T2  - Journal of Computational Chemistry
T1  - Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model
VL  - 40
SP  - 400
EP  - 413
DO  - 10.1002/jcc.25614
ER  - 

@article{
author = "Vujović, M. and Huynh, M. and Steiner, S. and Garcia-Fernandez, Pablo and Elstner, Marcus and Cui, Qiang and Gruden-Pavlović, Maja",
year = "2019",
abstract = "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. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.",
journal = "Journal of Computational Chemistry",
title = "Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model",
volume = "40",
pages = "400-413",
doi = "10.1002/jcc.25614"
}

Vujović, M., Huynh, M., Steiner, S., Garcia-Fernandez, P., Elstner, M., Cui, Q.,& Gruden-Pavlović, M.. (2019). Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model. in Journal of Computational Chemistry, 40, 400-413.
https://doi.org/10.1002/jcc.25614

Vujović M, Huynh M, Steiner S, Garcia-Fernandez P, Elstner M, Cui Q, Gruden-Pavlović M. Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model. in Journal of Computational Chemistry. 2019;40:400-413.
doi:10.1002/jcc.25614 .

Vujović, M., Huynh, M., Steiner, S., Garcia-Fernandez, Pablo, Elstner, Marcus, Cui, Qiang, Gruden-Pavlović, Maja, "Exploring the applicability of density functional tight binding to transition metal ions. Parameterization for nickel with the spin-polarized DFTB3 model" in Journal of Computational Chemistry, 40 (2019):400-413,
https://doi.org/10.1002/jcc.25614 . .