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|a 10.1002/jcc.27185
|2 doi
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|a pubmed24n1196.xml
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|a (DE-627)NLM359027288
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|a (NLM)37401535
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|a DE-627
|b ger
|c DE-627
|e rakwb
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|a eng
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|a Neugebauer, Hagen
|e verfasserin
|4 aut
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|a High-throughput screening of spin states for transition metal complexes with spin-polarized extended tight-binding methods
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|c 2023
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|a Text
|b txt
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|a ƒaComputermedien
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|2 rdamedia
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|a ƒa Online-Ressource
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|2 rdacarrier
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|a Date Revised 12.08.2023
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2023 The Authors. Journal of Computational Chemistry published by Wiley Periodicals LLC.
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|a The semiempirical GFNn-xTB ( n = 1 , 2 ) tight-binding methods are extended with a spin-dependent energy term (spin-polarization), enabling the fast and efficient screening of different spin states for transition metal complexes. While GFNn-xTB methods inherently can not differentiate properly between high-spin (HS) and low-spin (LS) states, this shortcoming is corrected with the presented methods termed spGFNn-xTB. The performance of spGFNn-xTB methods for spin state energy splittings is evaluated on a newly compiled benchmark set of 90 complexes (27 HS and 63 LS complexes) containing 3d, 4d, and 5d transition metals (termed TM90S) employing DFT references at the TPSSh-D4/def2-QZVPP level of theory. The challenging TM90S set contains complexes with charges between - 4 and +3, spin multiplicities between 1 and 6, and spin-splitting energies that range from - 47.8 to 146.6 kcal/mol with a mean average of 32.2 kcal/mol. On this set the (sp)GFNn-xTB methods, the PM6-D3H4 method, and the PM7 method are evaluated with spGFN1-xTB yielding the lowest MAD of 19.6 kcal/mol followed by spGFN2-xTB with 24.8 kcal/mol. While for the 4d and 5d subsets small or no improvements are observed with spin-polarization, large improvements are obtained for the 3d subset with spGFN1-xTB yielding the smallest MAD of 14.2 kcal/mol followed by spGFN2-xTB with 17.9 kcal/mol and PM6-D3H4 with 28.4 kcal/mol. The correct sign of the spin state splittings is obtained with spGFN2-xTB in 89% of all cases closely followed by spGFN1-xTB with 88%. On the full set, a pure semiempirical vertical spGFN2-xTB//GFN2-xTB-based workflow for screening purposes yields a slightly better MAD of 22.2 kcal/mol due to error compensation, while being qualitative correct for one additional case. In combination with their low computational cost (scanning spin states in seconds), the spGFNn-xTB methods represent robust tools for pre-screening steps of spin state calculations and high-throughput workflows
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|a Journal Article
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|a GFN-xTB
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|a semiempirical methods
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|a spin state-splitting
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|a tight-binding
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|a transition metal complexes
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|a Bädorf, Benedikt
|e verfasserin
|4 aut
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|a Ehlert, Sebastian
|e verfasserin
|4 aut
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|a Hansen, Andreas
|e verfasserin
|4 aut
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|a Grimme, Stefan
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Journal of computational chemistry
|d 1984
|g 44(2023), 27 vom: 15. Okt., Seite 2120-2129
|w (DE-627)NLM098138448
|x 1096-987X
|7 nnns
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| 773 |
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|g volume:44
|g year:2023
|g number:27
|g day:15
|g month:10
|g pages:2120-2129
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|u http://dx.doi.org/10.1002/jcc.27185
|3 Volltext
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