Solution of a Puzzle: High-Level Quantum-Chemical Treatment of Pseudocontact Chemical Shifts Confirms Classic Semiempirical Theory.
Journal
The journal of physical chemistry letters
ISSN: 1948-7185
Titre abrégé: J Phys Chem Lett
Pays: United States
ID NLM: 101526034
Informations de publication
Date de publication:
15 Oct 2020
15 Oct 2020
Historique:
pubmed:
16
9
2020
medline:
16
9
2020
entrez:
15
9
2020
Statut:
ppublish
Résumé
A recently popularized approach for the calculation of pseudocontact shifts (PCSs) based on first-principles quantum chemistry (QC) leads to different results than the classic "semiempirical" equation involving the susceptibility tensor. Studies that attempted a comparison of theory and experiment led to conflicting conclusions with respect to the preferred theoretical approach. In this Letter, we show that after inclusion of previously neglected terms in the full Hamiltonian, one can deduce the semiempirical equations from a rigorous QC-based treatment. It also turns out that in the long-distance limit, one can approximate the complete
Identifiants
pubmed: 32930598
doi: 10.1021/acs.jpclett.0c02462
pmc: PMC7584370
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
8735-8744Références
J Chem Phys. 2013 Mar 14;138(10):104102
pubmed: 23514460
J Comput Chem. 2002 Jun;23(8):794-803
pubmed: 12012356
Proc Natl Acad Sci U S A. 2004 Jun 8;101(23):8637-42
pubmed: 15161973
Angew Chem Int Ed Engl. 2015 Sep 7;54(37):10783-6
pubmed: 26223970
Phys Rev B Condens Matter. 1986 Jun 15;33(12):8822-8824
pubmed: 9938299
Angew Chem Int Ed Engl. 2016 Nov 14;55(47):14713-14717
pubmed: 27781358
Sci Rep. 2013;3:2538
pubmed: 23985776
Chemistry. 2019 Aug 9;25(45):10668-10677
pubmed: 31050369
J Phys Chem Lett. 2019 Jul 5;10(13):3610-3614
pubmed: 31181162
Chemistry. 2004 Sep 20;10(18):4594-8
pubmed: 15378638
J Phys Chem Lett. 2015 Jun 18;6(12):2183-8
pubmed: 26266589
Inorg Chem. 2017 Dec 18;56(24):15285-15294
pubmed: 29200279
Protein Sci. 1995 Feb;4(2):296-305
pubmed: 7757018
J Chem Theory Comput. 2015 Oct 13;11(10):4840-9
pubmed: 26574272
J Chem Phys. 2013 Jan 14;138(2):021103
pubmed: 23320659
J Am Chem Soc. 2003 May 7;125(18):5549-58
pubmed: 12720469
Prog Nucl Magn Reson Spectrosc. 2019 Apr;111:1-271
pubmed: 31146806
Phys Chem Chem Phys. 2019 Mar 6;21(10):5661-5673
pubmed: 30794275
Chemistry. 2004 Sep 20;10(18):4627-39
pubmed: 15378642
J Chem Theory Comput. 2011 Jul 12;7(7):2175-88
pubmed: 26606487
J Chem Phys. 2015 Feb 7;142(5):054108
pubmed: 25662637
J Biomol NMR. 2011 Jul;50(3):263-6
pubmed: 21626213
J Am Chem Soc. 2017 Oct 11;139(40):14166-14172
pubmed: 28884581
Prog Nucl Magn Reson Spectrosc. 2017 Feb;98-99:20-49
pubmed: 28283085
J Chem Phys. 2004 Feb 1;120(5):2127-39
pubmed: 15268351
Phys Chem Chem Phys. 2018 Sep 12;20(35):22547-22555
pubmed: 30141806
J Chem Phys. 2019 Apr 14;150(14):144101
pubmed: 30981251
Prog Nucl Magn Reson Spectrosc. 2019 Oct - Dec;114-115:211-236
pubmed: 31779881
Inorg Chem. 2018 Aug 6;57(15):8735-8747
pubmed: 29620874
Acc Chem Res. 2020 Aug 18;53(8):1520-1534
pubmed: 32667187
Prog Nucl Magn Reson Spectrosc. 2011 Feb;58(1-2):88-96
pubmed: 21241885
Phys Rev A Gen Phys. 1988 Sep 15;38(6):3098-3100
pubmed: 9900728
J Magn Reson. 2019 Sep;306:173-179
pubmed: 31331762
J Phys Chem Lett. 2014 Nov 6;5(21):3799-803
pubmed: 26278750
J Chem Theory Comput. 2018 Jan 9;14(1):377-394
pubmed: 29182320
J Chem Phys. 2013 Feb 7;138(5):054113
pubmed: 23406104
J Chem Phys. 2005 Aug 8;123(6):64107
pubmed: 16122300