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Due to the similar chemical composition and matrix effect, the accurate identification of mineral pigments on wall paintings has brought great challenges. This work implemented an identification study on three mineral pigments with similar chemical compositions by combining LIBS technology with the K-nearest neighbor algorithm (KNN), random forest (RF support vector machine (SVM), back propagation artificial neural network (Bp-ANN) and convolutional neural network (CNN) to find the most suitable identification method for mural research. Using the SelectKBest algorithm, 300 characteristic lines with the largest difference among the three pigments were determined. The identification models of KNN, RF, SVM, Bp-ANN and CNN were established and optimized. The results showed that, except for the KNN model, the identification accuracy of other models for mock-up mural samples was above 99%. However, only the identification accuracy of 2D-CNN models reached above 94% for actual mural samples. Therefore, the 2D-CNN model was determined as the most suitable model for the identification and analysis of mural pigments.
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