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Accurate Backbone 13C and 15N Chemical Shift Tensors in Galectin-3 Determined by MAS NMR and QM/MM : Details of Structure and Environment Matter

Kraus, Jodi ; Gupta, Rupal ; Lu, Manman ; Gronenborn, Angela M. ; Akke, Mikael LU and Polenova, Tatyana (2020) In ChemPhysChem
Abstract

Chemical shift tensors obtained from solid-state NMR spectroscopy are very sensitive reporters of structure and dynamics in proteins. While accurate 13C and 15N chemical shift tensors are accessible by magic angle spinning (MAS) NMR, their quantum mechanical calculations remain challenging, particularly for 15N atoms. Here we compare experimentally determined backbone 13Cα and 15NH chemical shift tensors by MAS NMR with hybrid quantum mechanics/molecular mechanics/molecular dynamics (MD-QM/MM) calculations for the carbohydrate-binding domain of galectin-3. Excellent agreement between experimental and computed 15NH chemical shift anisotropy... (More)

Chemical shift tensors obtained from solid-state NMR spectroscopy are very sensitive reporters of structure and dynamics in proteins. While accurate 13C and 15N chemical shift tensors are accessible by magic angle spinning (MAS) NMR, their quantum mechanical calculations remain challenging, particularly for 15N atoms. Here we compare experimentally determined backbone 13Cα and 15NH chemical shift tensors by MAS NMR with hybrid quantum mechanics/molecular mechanics/molecular dynamics (MD-QM/MM) calculations for the carbohydrate-binding domain of galectin-3. Excellent agreement between experimental and computed 15NH chemical shift anisotropy values was obtained using the Amber ff15ipq force field when solvent dynamics was taken into account in the calculation. Our results establish important benchmark conditions for improving the accuracy of chemical shift calculations in proteins and may aid in the validation of protein structure models derived by MAS NMR.

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author
organization
publishing date
type
Contribution to journal
publication status
epub
subject
keywords
Chemical shift anisotropy, microcrystalline protein, QM/MM, recoupling, solid-state NMR
in
ChemPhysChem
publisher
John Wiley and Sons Inc.
external identifiers
  • pmid:32363727
  • scopus:85085997223
ISSN
1439-4235
DOI
10.1002/cphc.202000249
language
English
LU publication?
yes
id
b356855b-0feb-4f71-a945-0dcd9919e4fb
date added to LUP
2020-06-30 15:47:53
date last changed
2020-07-01 05:34:47
@article{b356855b-0feb-4f71-a945-0dcd9919e4fb,
  abstract     = {<p>Chemical shift tensors obtained from solid-state NMR spectroscopy are very sensitive reporters of structure and dynamics in proteins. While accurate <sup>13</sup>C and <sup>15</sup>N chemical shift tensors are accessible by magic angle spinning (MAS) NMR, their quantum mechanical calculations remain challenging, particularly for <sup>15</sup>N atoms. Here we compare experimentally determined backbone <sup>13</sup>C<sup>α</sup> and <sup>15</sup>N<sup>H</sup> chemical shift tensors by MAS NMR with hybrid quantum mechanics/molecular mechanics/molecular dynamics (MD-QM/MM) calculations for the carbohydrate-binding domain of galectin-3. Excellent agreement between experimental and computed <sup>15</sup>N<sup>H</sup> chemical shift anisotropy values was obtained using the Amber ff15ipq force field when solvent dynamics was taken into account in the calculation. Our results establish important benchmark conditions for improving the accuracy of chemical shift calculations in proteins and may aid in the validation of protein structure models derived by MAS NMR.</p>},
  author       = {Kraus, Jodi and Gupta, Rupal and Lu, Manman and Gronenborn, Angela M. and Akke, Mikael and Polenova, Tatyana},
  issn         = {1439-4235},
  language     = {eng},
  publisher    = {John Wiley and Sons Inc.},
  series       = {ChemPhysChem},
  title        = {Accurate Backbone <sup>13</sup>C and <sup>15</sup>N Chemical Shift Tensors in Galectin-3 Determined by MAS NMR and QM/MM : Details of Structure and Environment Matter},
  url          = {http://dx.doi.org/10.1002/cphc.202000249},
  doi          = {10.1002/cphc.202000249},
  year         = {2020},
}