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  Computation of NMR Shielding Constants for Solids Using an Embedded Cluster Approach with DFT, Double-Hybrid DFT, and MP2

Dittmer, A., Stoychev, G. L., Maganas, D., Auer, A. A., & Neese, F. (2020). Computation of NMR Shielding Constants for Solids Using an Embedded Cluster Approach with DFT, Double-Hybrid DFT, and MP2. Journal of Chemical Theory and Computation, 16(11), 6950-6967. doi:10.1021/acs.jctc.0c00067.

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 Creators:
Dittmer, Anneke1, Author           
Stoychev, Georgi L.2, Author           
Maganas, Dimitrios1, Author           
Auer, Alexander A.2, Author           
Neese, Frank3, Author           
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1Research Group Manganas, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541709              
2Research Group Auer, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541705              
3Research Department Neese, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2541710              

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 Abstract: In this work, we explore the accuracy of post-Hartree–Fock (HF) methods and double-hybrid density functional theory (DFT) for the computation of solid-state NMR chemical shifts. We apply an embedded cluster approach and investigate the convergence with cluster size and embedding for a series of inorganic solids with long-range electrostatic interactions. In a systematic study, we discuss the cluster design, the embedding procedure, and basis set convergence using gauge-including atomic orbital (GIAO) NMR calculations at the DFT and MP2 levels of theory. We demonstrate that the accuracy obtained for the prediction of NMR chemical shifts, which can be achieved for molecular systems, can be carried over to solid systems. An appropriate embedded cluster approach allows one to apply methods beyond standard DFT even for systems for which long-range electrostatic effects are important. We find that an embedded cluster should include at least one sphere of explicit neighbors around the nuclei of interest, given that a sufficiently large point charge and boundary effective potential embedding is applied. Using the pcSseg-3 basis set and GIAOs for the computation of nuclear shielding constants, accuracies of 1.6 ppm for 7Li, 1.5 ppm for 23Na, and 5.1 ppm for 39K as well as 9.3 ppm for 19F, 6.5 ppm for 35Cl, 7.4 ppm for 79Br, and 7.5 ppm for 25Mg as well as 3.8 ppm for 67Zn can be achieved with MP2. Comparing various DFT functionals with HF and MP2, we report the superior quality of results for methods that include post-HF correlation like MP2 and double-hybrid DFT.

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Language(s): eng - English
 Dates: 2020-01-202020-09-232020-11-10
 Publication Status: Published in print
 Pages: 18
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jctc.0c00067
 Degree: -

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Title: Journal of Chemical Theory and Computation
  Abbreviation : J. Chem. Theory Comput.
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 16 (11) Sequence Number: - Start / End Page: 6950 - 6967 Identifier: ISSN: 1549-9618
CoNE: https://pure.mpg.de/cone/journals/resource/111088195283832