Visualization of a Machine Learning Framework toward Highly Sensitive Qualitative Analysis by SERS.

Journal: Analytical chemistry
Published Date: Jul 19, 2022

Abstract

Surface-enhanced Raman spectroscopy (SERS), providing near-single-molecule-level fingerprint information, is a powerful tool for the trace analysis of a target in a complicated matrix and is especially facilitated by the development of modern machine learning algorithms. However, both the high demand of mass data and the low interpretability of the mysterious black-box operation significantly limit the well-trained model to real systems in practical applications. Aiming at these two issues, we constructed a novel machine learning algorithm-based framework (Vis-CAD), integrating visual random forest, characteristic amplifier, and data augmentation. The introduction of data augmentation significantly reduced the requirement of mass data, and the visualization of the random forest clearly presented the captured features, by which one was able to determine the reliability of the algorithm. Taking the trace analysis of individual polycyclic aromatic hydrocarbons in a mixture as an example, a trustworthy accuracy no less than 99% was realized under the optimized condition. The visualization of the algorithm framework distinctly demonstrated that the captured feature was well correlated to the characteristic Raman peaks of each individual. Furthermore, the sensitivity toward the trace individual could be improved by least 1 order of magnitude as compared to that with the naked eye. The proposed algorithm distinguished by the lesser demand of mass data and the visualization of the operation process offers a new way for the indestructible application of machine learning algorithms, which would bring push-to-the-limit sensitivity toward the qualitative and quantitative analysis of trace targets, not only in the field of SERS, but also in the much wider spectroscopy world. It is implemented in the Python programming language and is open-source at https://github.com/3331822w/Vis-CAD.

Authors

  • Si-Heng Luo
    State Key Laboratory for Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian 361005, China.
  • Wei-Li Wang
    State Key Laboratory of Marine Environmental Science, Fujian Provincial Key Laboratory for Coastal Ecology and Environmental Studies, Center for Marine Environmental Chemistry & Toxicology, College of the Environment and Ecology, Xiamen University, Xiamen 361102, China.
  • Zhi-Fan Zhou
    State Key Laboratory of Marine Environmental Science, Fujian Provincial Key Laboratory for Coastal Ecology and Environmental Studies, Center for Marine Environmental Chemistry & Toxicology, College of the Environment and Ecology, Xiamen University, Xiamen 361102, China.
  • Yi Xie
    Department of Plastic Surgery Peninsula Health Melbourne Victoria Australia.
  • Bin Ren
  • Guo-Kun Liu
    State Key Laboratory of Marine Environmental Science, Fujian Provincial Key Laboratory for Coastal Ecology and Environmental Studies, Center for Marine Environmental Chemistry & Toxicology, College of the Environment and Ecology, Xiamen University, Xiamen 361102, China.
  • Zhong-Qun Tian
    State Key Laboratory for Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen, Fujian 361005, China.

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