A deep learning model for chemical shieldings in molecular organic solids including anisotropy

Fuente: arXiv
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Autores principales: Kellner, Matthias, Holmes, Jacob B., Rodriguez-Madrid, Ruben, Viscosi, Florian, Zhang, Yuxuan, Emsley, Lyndon, Ceriotti, Michele
Formato: Preprint
Publicado: 2025
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author Kellner, Matthias
Holmes, Jacob B.
Rodriguez-Madrid, Ruben
Viscosi, Florian
Zhang, Yuxuan
Emsley, Lyndon
Ceriotti, Michele
author_facet Kellner, Matthias
Holmes, Jacob B.
Rodriguez-Madrid, Ruben
Viscosi, Florian
Zhang, Yuxuan
Emsley, Lyndon
Ceriotti, Michele
contents Nuclear Magnetic Resonance (NMR) chemical shifts are powerful probes of local atomic and electronic structure that can be used to resolve the structures of powdered or amorphous molecular solids. Chemical shift driven structure elucidation depends critically on accurate and fast predictions of chemical shieldings, and machine learning (ML) models for shielding predictions are increasingly used as scalable and efficient surrogates for demanding ab initio calculations. However, the prediction accuracies of current ML models still lag behind those of the DFT reference methods they approximate, especially for nuclei such as $^{13}$C and $^{15}$N. Here, we introduce ShiftML3.0, a deep-learning model that improves the accuracy of predictions of isotropic chemical shieldings in molecular solids, and does so while also predicting the full shielding tensor. On experimental benchmark sets, we find root-mean-squared errors with respect to experiment for ShiftML3.0 that approach those of DFT reference calculations, with RMSEs of 0.53 ppm for $^{1}$H, 2.4 ppm for $^{13}$C, and 7.2 ppm for $^{15}$N, compared to DFT values of 0.49 ppm, 2.3 ppm, and 5.8 ppm, respectively.
format Preprint
id arxiv_https___arxiv_org_abs_2506_13146
institution arXiv
publishDate 2025
record_format arxiv
spellingShingle A deep learning model for chemical shieldings in molecular organic solids including anisotropy
Kellner, Matthias
Holmes, Jacob B.
Rodriguez-Madrid, Ruben
Viscosi, Florian
Zhang, Yuxuan
Emsley, Lyndon
Ceriotti, Michele
Chemical Physics
Nuclear Magnetic Resonance (NMR) chemical shifts are powerful probes of local atomic and electronic structure that can be used to resolve the structures of powdered or amorphous molecular solids. Chemical shift driven structure elucidation depends critically on accurate and fast predictions of chemical shieldings, and machine learning (ML) models for shielding predictions are increasingly used as scalable and efficient surrogates for demanding ab initio calculations. However, the prediction accuracies of current ML models still lag behind those of the DFT reference methods they approximate, especially for nuclei such as $^{13}$C and $^{15}$N. Here, we introduce ShiftML3.0, a deep-learning model that improves the accuracy of predictions of isotropic chemical shieldings in molecular solids, and does so while also predicting the full shielding tensor. On experimental benchmark sets, we find root-mean-squared errors with respect to experiment for ShiftML3.0 that approach those of DFT reference calculations, with RMSEs of 0.53 ppm for $^{1}$H, 2.4 ppm for $^{13}$C, and 7.2 ppm for $^{15}$N, compared to DFT values of 0.49 ppm, 2.3 ppm, and 5.8 ppm, respectively.
title A deep learning model for chemical shieldings in molecular organic solids including anisotropy
topic Chemical Physics
url https://arxiv.org/abs/2506.13146