Chalcogen bonds: Hierarchical ab initio benchmark and density functional theory performance study

Lucas de Azevedo Santos; Teodorico C. Ramalho; Trevor A. Hamlin; F. Matthias Bickelhaupt

doi:10.1002/jcc.26489

Chalcogen bonds: Hierarchical ab initio benchmark and density functional theory performance study

Lucas de Azevedo Santos^*, Teodorico C. Ramalho^*, Trevor A. Hamlin^*, F. Matthias Bickelhaupt^*

^*Corresponding author for this work

Research output: Contribution to Journal › Article › Academic › peer-review

Abstract

We have performed a hierarchical ab initio benchmark and DFT performance study of D₂Ch•••A⁻ chalcogen bonds (Ch = S, Se; D, A = F, Cl). The ab initio benchmark study is based on a series of ZORA-relativistic quantum chemical methods [HF, MP2, CCSD, CCSD(T)], and all-electron relativistically contracted variants of Karlsruhe basis sets (ZORA-def2-SVP, ZORA-def2-TZVPP, ZORA-def2-QZVPP) with and without diffuse functions. The highest-level ZORA-CCSD(T)/ma-ZORA-def2-QZVPP counterpoise-corrected complexation energies (ΔE_CPC) are converged within 1.1–3.4 kcal mol⁻¹ and 1.5–3.1 kcal mol⁻¹ with respect to the method and basis set, respectively. Next, we used the ZORA-CCSD(T)/ma-ZORA-def2-QZVPP (ΔE_CPC) as reference data for analyzing the performance of 13 different ZORA-relativistic DFT approaches in combination with the Slater-type QZ4P basis set. We find that the three-best performing functionals are M06-2X, B3LYP, and M06, with mean absolute errors (MAE) of 4.1, 4.2, and 4.3 kcal mol⁻¹, respectively. The MAE for BLYP-D3(BJ) and PBE amount to 8.5 and 9.3 kcal mol⁻¹, respectively.

Original language	English
Pages (from-to)	688-698
Number of pages	11
Journal	Journal of Computational Chemistry
Volume	42
Issue number	10
Early online date	5 Feb 2021
DOIs	https://doi.org/10.1002/jcc.26489
Publication status	Published - 15 Apr 2021

Bibliographical note

Funding Information:
We thank the Brazilian agencies Fundação de Amparo à Pesquisa do Estado de Minas Gerais (FAPEMIG) and Coordenação de Aperfeiçoamento de Pessoal de Nível Superior (CAPES) for the scholarship to LAS, Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) for the fellowship to TCR, and the Netherlands Organization for Scientific Research (NWO) for support. This work was carried out on the Dutch national e‐infrastructure with the support of SURF Cooperative.

Funding Information:
We thank the Brazilian agencies Funda??o de Amparo ? Pesquisa do Estado de Minas Gerais (FAPEMIG) and Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior (CAPES) for the scholarship to LAS, Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico (CNPq) for the fellowship to TCR, and the Netherlands Organization for Scientific Research (NWO) for support. This work was carried out on the Dutch national e-infrastructure with the support of SURF Cooperative.

Publisher Copyright:
© 2021 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.

Copyright:
Copyright 2021 Elsevier B.V., All rights reserved.

Keywords

benchmark study
chalcogen bonds
coupled-cluster
density functional calculations
noncovalent interactions

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title = "Chalcogen bonds: Hierarchical ab initio benchmark and density functional theory performance study",

abstract = "We have performed a hierarchical ab initio benchmark and DFT performance study of D2Ch•••A− chalcogen bonds (Ch = S, Se; D, A = F, Cl). The ab initio benchmark study is based on a series of ZORA-relativistic quantum chemical methods [HF, MP2, CCSD, CCSD(T)], and all-electron relativistically contracted variants of Karlsruhe basis sets (ZORA-def2-SVP, ZORA-def2-TZVPP, ZORA-def2-QZVPP) with and without diffuse functions. The highest-level ZORA-CCSD(T)/ma-ZORA-def2-QZVPP counterpoise-corrected complexation energies (ΔECPC) are converged within 1.1–3.4 kcal mol−1 and 1.5–3.1 kcal mol−1 with respect to the method and basis set, respectively. Next, we used the ZORA-CCSD(T)/ma-ZORA-def2-QZVPP (ΔECPC) as reference data for analyzing the performance of 13 different ZORA-relativistic DFT approaches in combination with the Slater-type QZ4P basis set. We find that the three-best performing functionals are M06-2X, B3LYP, and M06, with mean absolute errors (MAE) of 4.1, 4.2, and 4.3 kcal mol−1, respectively. The MAE for BLYP-D3(BJ) and PBE amount to 8.5 and 9.3 kcal mol−1, respectively.",

keywords = "benchmark study, chalcogen bonds, coupled-cluster, density functional calculations, noncovalent interactions",

author = "{de Azevedo Santos}, Lucas and Ramalho, {Teodorico C.} and Hamlin, {Trevor A.} and Bickelhaupt, {F. Matthias}",

note = "Funding Information: We thank the Brazilian agencies Funda{\c c}{\~a}o de Amparo {\`a} Pesquisa do Estado de Minas Gerais (FAPEMIG) and Coordena{\c c}{\~a}o de Aperfei{\c c}oamento de Pessoal de N{\'i}vel Superior (CAPES) for the scholarship to LAS, Conselho Nacional de Desenvolvimento Cient{\'i}fico e Tecnol{\'o}gico (CNPq) for the fellowship to TCR, and the Netherlands Organization for Scientific Research (NWO) for support. This work was carried out on the Dutch national e‐infrastructure with the support of SURF Cooperative. Funding Information: We thank the Brazilian agencies Funda??o de Amparo ? Pesquisa do Estado de Minas Gerais (FAPEMIG) and Coordena??o de Aperfei?oamento de Pessoal de N?vel Superior (CAPES) for the scholarship to LAS, Conselho Nacional de Desenvolvimento Cient?fico e Tecnol?gico (CNPq) for the fellowship to TCR, and the Netherlands Organization for Scientific Research (NWO) for support. This work was carried out on the Dutch national e-infrastructure with the support of SURF Cooperative. Publisher Copyright: {\textcopyright} 2021 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC. Copyright: Copyright 2021 Elsevier B.V., All rights reserved.",

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doi = "10.1002/jcc.26489",

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AU - Bickelhaupt, F. Matthias

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PY - 2021/4/15

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N2 - We have performed a hierarchical ab initio benchmark and DFT performance study of D2Ch•••A− chalcogen bonds (Ch = S, Se; D, A = F, Cl). The ab initio benchmark study is based on a series of ZORA-relativistic quantum chemical methods [HF, MP2, CCSD, CCSD(T)], and all-electron relativistically contracted variants of Karlsruhe basis sets (ZORA-def2-SVP, ZORA-def2-TZVPP, ZORA-def2-QZVPP) with and without diffuse functions. The highest-level ZORA-CCSD(T)/ma-ZORA-def2-QZVPP counterpoise-corrected complexation energies (ΔECPC) are converged within 1.1–3.4 kcal mol−1 and 1.5–3.1 kcal mol−1 with respect to the method and basis set, respectively. Next, we used the ZORA-CCSD(T)/ma-ZORA-def2-QZVPP (ΔECPC) as reference data for analyzing the performance of 13 different ZORA-relativistic DFT approaches in combination with the Slater-type QZ4P basis set. We find that the three-best performing functionals are M06-2X, B3LYP, and M06, with mean absolute errors (MAE) of 4.1, 4.2, and 4.3 kcal mol−1, respectively. The MAE for BLYP-D3(BJ) and PBE amount to 8.5 and 9.3 kcal mol−1, respectively.

AB - We have performed a hierarchical ab initio benchmark and DFT performance study of D2Ch•••A− chalcogen bonds (Ch = S, Se; D, A = F, Cl). The ab initio benchmark study is based on a series of ZORA-relativistic quantum chemical methods [HF, MP2, CCSD, CCSD(T)], and all-electron relativistically contracted variants of Karlsruhe basis sets (ZORA-def2-SVP, ZORA-def2-TZVPP, ZORA-def2-QZVPP) with and without diffuse functions. The highest-level ZORA-CCSD(T)/ma-ZORA-def2-QZVPP counterpoise-corrected complexation energies (ΔECPC) are converged within 1.1–3.4 kcal mol−1 and 1.5–3.1 kcal mol−1 with respect to the method and basis set, respectively. Next, we used the ZORA-CCSD(T)/ma-ZORA-def2-QZVPP (ΔECPC) as reference data for analyzing the performance of 13 different ZORA-relativistic DFT approaches in combination with the Slater-type QZ4P basis set. We find that the three-best performing functionals are M06-2X, B3LYP, and M06, with mean absolute errors (MAE) of 4.1, 4.2, and 4.3 kcal mol−1, respectively. The MAE for BLYP-D3(BJ) and PBE amount to 8.5 and 9.3 kcal mol−1, respectively.

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Chalcogen bonds: Hierarchical ab initio benchmark and density functional theory performance study

Abstract

Bibliographical note

Keywords

UN SDGs

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