Simonnet Titouan, Grangeon Sylvain, Claret Francis, Maubec Nicolas, Fall Mame Diarra, Harba Rachid, Galerne Bruno
Institut Denis Poisson, Université d'Orléans, Université de Tours, CNRS, France.
BRGM, 45060 Orléans, France.
IUCrJ. 2024 Sep 1;11(Pt 5):859-870. doi: 10.1107/S2052252524006766.
Mineral identification and quantification are key to the understanding and, hence, the capacity to predict material properties. The method of choice for mineral quantification is powder X-ray diffraction (XRD), generally using a Rietveld refinement approach. However, a successful Rietveld refinement requires preliminary identification of the phases that make up the sample. This is generally carried out manually, and this task becomes extremely long or virtually impossible in the case of very large datasets such as those from synchrotron X-ray diffraction computed tomography. To circumvent this issue, this article proposes a novel neural network (NN) method for automating phase identification and quantification. An XRD pattern calculation code was used to generate large datasets of synthetic data that are used to train the NN. This approach offers significant advantages, including the ability to construct databases with a substantial number of XRD patterns and the introduction of extensive variability into these patterns. To enhance the performance of the NN, a specifically designed loss function for proportion inference was employed during the training process, offering improved efficiency and stability compared with traditional functions. The NN, trained exclusively with synthetic data, proved its ability to identify and quantify mineral phases on synthetic and real XRD patterns. Trained NN errors were equal to 0.5% for phase quantification on the synthetic test set, and 6% on the experimental data, in a system containing four phases of contrasting crystal structures (calcite, gibbsite, dolomite and hematite). The proposed method is freely available on GitHub and allows for major advances since it can be applied to any dataset, regardless of the mineral phases present.
矿物鉴定和定量分析是理解并进而预测材料性能的关键。矿物定量分析的首选方法是粉末X射线衍射(XRD),通常采用Rietveld精修方法。然而,成功的Rietveld精修需要预先识别构成样品的物相。这通常是手动进行的,而在面对非常大的数据集(如来自同步加速器X射线衍射计算机断层扫描的数据)时,这项任务会变得极其漫长甚至几乎不可能完成。为了规避这个问题,本文提出了一种用于自动进行物相识别和定量分析的新型神经网络(NN)方法。使用XRD图谱计算代码生成大量合成数据的数据集,用于训练神经网络。这种方法具有显著优势,包括能够构建包含大量XRD图谱的数据库,并在这些图谱中引入广泛的变异性。为了提高神经网络的性能,在训练过程中采用了专门设计的比例推断损失函数,与传统函数相比,具有更高的效率和稳定性。仅使用合成数据训练的神经网络,在合成XRD图谱和真实XRD图谱上都证明了其识别和定量矿物相的能力。在一个包含四种具有不同晶体结构的物相(方解石、三水铝石、白云石和赤铁矿)的系统中,训练后的神经网络在合成测试集上进行物相定量分析时的误差为0.5% 在实验数据上的误差为6%。所提出的方法可在GitHub上免费获取,并且由于它可以应用于任何数据集,无论其中存在何种矿物相,因此能够取得重大进展。