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<p>NMR crystallography has emerged as a promising technique for the determination and refinement of atomic coordinates in crystal structures. The crystal structure of compounds containing quadrupolar nuclei, such as&#xa0;<sup>27</sup>Al, can be improved by directly comparing solid-state NMR measurements to DFT computations of the electric field gradient (EFG) tensor. The non-negligible computational cost of these first-principles calculations limits the applicability of this method to all but the most well-defined structures. We developed a fast, low-cost machine learning model to predict EFG parameters based on local structural motifs and elemental parameters. We computed 8081 EFG tensors from 1681 <sup>27</sup>Al crystalline solids using DFT and benchmarked them against 105 experimentally measured&#xa0;<sup>27</sup>Al sites. Surprisingly, simple local geometric features dominate the predictive performance of the resulting random-forest model, yielding an R<sup>2</sup> value of 0.98 and an RMSE of 0.61&#xa0;MHz for C<sub>Q</sub>, the quadrupolar coupling constant. This model accuracy should enable pre-refining future structural assignments before finally validating with first-principles calculations. Such a catalogue of&#xa0;<sup>27</sup>Al NMR tensors can serve as a tool for researchers assigning complex NMR spectra influenced by the nuclear electric quadrupole interaction.</p>

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Machine learning of 27Al NMR electric field gradient tensors for crystalline structures from DFT

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月21日

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  • He Sun,
  • Shyam Dwaraknath,
  • Handong Ling,
  • Kristin A. Persson,
  • Sophia E. Hayes

摘要

NMR crystallography has emerged as a promising technique for the determination and refinement of atomic coordinates in crystal structures. The crystal structure of compounds containing quadrupolar nuclei, such as 27Al, can be improved by directly comparing solid-state NMR measurements to DFT computations of the electric field gradient (EFG) tensor. The non-negligible computational cost of these first-principles calculations limits the applicability of this method to all but the most well-defined structures. We developed a fast, low-cost machine learning model to predict EFG parameters based on local structural motifs and elemental parameters. We computed 8081 EFG tensors from 1681 27Al crystalline solids using DFT and benchmarked them against 105 experimentally measured 27Al sites. Surprisingly, simple local geometric features dominate the predictive performance of the resulting random-forest model, yielding an R2 value of 0.98 and an RMSE of 0.61 MHz for CQ, the quadrupolar coupling constant. This model accuracy should enable pre-refining future structural assignments before finally validating with first-principles calculations. Such a catalogue of 27Al NMR tensors can serve as a tool for researchers assigning complex NMR spectra influenced by the nuclear electric quadrupole interaction.