Ab Initio Quality NMR Parameters in Solid-State Materials Using a High-Dimensional Neural-Network Representation

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• 作者：Jér?me Cuny ; Yu Xie ; Chris J. Pickard ; Ali A. Hassanali
• 刊名：Journal of Chemical Theory and Computation
• 出版年：2016
• 出版时间：February 9, 2016
• 年：2016
• 卷：12
• 期：2
• 页码：765-773
• 全文大小：601K
• ISSN：1549-9626

文摘

Nuclear magnetic resonance (NMR) spectroscopy is one of the most powerful experimental tools to probe the local atomic order of a wide range of solid-state compounds. However, due to the complexity of the related spectra, in particular for amorphous materials, their interpretation in terms of structural information is often challenging. These difficulties can be overcome by combining molecular dynamics simulations to generate realistic structural models with an ab initio evaluation of the corresponding chemical shift and quadrupolar coupling tensors. However, due to computational constraints, this approach is limited to relatively small system sizes which, for amorphous materials, prevents an adequate statistical sampling of the distribution of the local environments that is required to quantitatively describe the system. In this work, we present an approach to efficiently and accurately predict the NMR parameters of very large systems. This is achieved by using a high-dimensional neural-network representation of NMR parameters that are calculated using an ab initio formalism. To illustrate the potential of this approach, we applied this neural-network NMR (NN-NMR) method on the ¹⁷O and ²⁹Si quadrupolar coupling and chemical shift parameters of various crystalline silica polymorphs and silica glasses. This approach is, in principal, general and has the potential to be applied to predict the NMR properties of various materials.