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research article

A Machine Learning Model of Chemical Shifts for Chemically and Structurally Diverse Molecular Solids

Cordova, Manuel  
•
Engel, Edgar A.
•
Stefaniuk, Artur  
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September 22, 2022
Journal Of Physical Chemistry C

Nuclear magnetic resonance (NMR) chemical shifts are a direct probe of local atomic environments and can be used to determine the structure of solid materials. However, the substantial computational cost required to predict accurate chemical shifts is a key bottleneck for NMR crystallography. We recently introduced ShiftML, a machine-learning model of chemical shifts in molecular solids, trained on minimum-energy geometries of materials composed of C, H, N, O, and S that provides rapid chemical shift predictions with density functional theory (DFT) accuracy. Here, we extend the capabilities of ShiftML to predict chemical shifts for both finite temperature structures and more chemically diverse compounds, while retaining the same speed and accuracy. For a benchmark set of 13 molecular solids, we find a root-mean-squared error of 0.47 ppm with respect to experiment for 1H shift predictions (compared to 0.35 ppm for explicit DFT calculations), while reducing the computational cost by over four orders of magnitude.

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Type
research article
DOI
10.1021/acs.jpcc.2c03854
Web of Science ID

WOS:000861634700001

Author(s)
Cordova, Manuel  
•
Engel, Edgar A.
•
Stefaniuk, Artur  
•
Paruzzo, Federico  
•
Hofstetter, Albert  
•
Ceriotti, Michele  
•
Emsley, Lyndon  
Date Issued

2022-09-22

Published in
Journal Of Physical Chemistry C
Volume

126

Issue

39

Start page

16710

End page

16720

Subjects

Chemistry, Physical

•

Nanoscience & Nanotechnology

•

Materials Science, Multidisciplinary

•

Chemistry

•

Science & Technology - Other Topics

•

Materials Science

•

crystal-structure prediction

•

density-functional theory

•

magnetic-resonance

•

nmr crystallography

•

quantum

•

pseudopotentials

•

simulations

Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
COSMO  
LRM  
FunderGrant Number

FNS

200020_178860

Available on Infoscience
October 24, 2022
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/191587
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