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Neural network-based classification of X-ray fluorescence spectra of artists’ pigments: an approach leveraging a synthetic dataset created using the fundamental parameters method

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AbstractX-ray fluorescence (XRF) spectroscopy is an analytical technique used to identify chemical elements that has found widespread use in the cultural heritage sector to characterise artists' materials including the pigments in paintings. It generates a spectrum with characteristic emission lines relating to the elements present, which is interpreted by an expert to understand the materials therein. Convolutional neural networks (CNNs) are an effective method for automating such classification tasks—an increasingly important feature as XRF datasets continue to grow in size—but they require large libraries that capture the natural variation of each class for training. As an alternative to having to acquire such a large library of XRF spectra of artists' materials a physical model, the Fundamental Parameters (FP) method, was used to generate a synthetic dataset of XRF spectra representative of pigments typically encountered in Renaissance paintings that could then be used to train a neural network. The synthetic spectra generated—modelled as single layers of individual pigments—had characteristic element lines closely matching those found in real XRF spectra. However, as the method did not incorporate effects from the X-ray source, the synthetic spectra lacked the continuum and Rayleigh and Compton scatter peaks. Nevertheless, the network trained on the synthetic dataset achieved 100% accuracy when tested on synthetic XRF data. Whilst this initial network only attained 55% accuracy when tested on real XRF spectra obtained from reference samples, applying transfer learning using a small quantity of such real XRF spectra increased the accuracy to 96%. Due to these promising results, the network was also tested on select data acquired during macro XRF (MA-XRF) scanning of a painting to challenge the model with noisier spectra Although only tested on spectra from relatively simple paint passages, the results obtained suggest that the FP method can be used to create accurate synthetic XRF spectra of individual artists' pigments, free from X-ray tube effects, on which a classification model could be trained for application to real XRF data and that the method has potential to be extended to deal with more complex paint mixtures and stratigraphies.
Title: Neural network-based classification of X-ray fluorescence spectra of artists’ pigments: an approach leveraging a synthetic dataset created using the fundamental parameters method
Description:
AbstractX-ray fluorescence (XRF) spectroscopy is an analytical technique used to identify chemical elements that has found widespread use in the cultural heritage sector to characterise artists' materials including the pigments in paintings.
It generates a spectrum with characteristic emission lines relating to the elements present, which is interpreted by an expert to understand the materials therein.
Convolutional neural networks (CNNs) are an effective method for automating such classification tasks—an increasingly important feature as XRF datasets continue to grow in size—but they require large libraries that capture the natural variation of each class for training.
As an alternative to having to acquire such a large library of XRF spectra of artists' materials a physical model, the Fundamental Parameters (FP) method, was used to generate a synthetic dataset of XRF spectra representative of pigments typically encountered in Renaissance paintings that could then be used to train a neural network.
The synthetic spectra generated—modelled as single layers of individual pigments—had characteristic element lines closely matching those found in real XRF spectra.
However, as the method did not incorporate effects from the X-ray source, the synthetic spectra lacked the continuum and Rayleigh and Compton scatter peaks.
Nevertheless, the network trained on the synthetic dataset achieved 100% accuracy when tested on synthetic XRF data.
Whilst this initial network only attained 55% accuracy when tested on real XRF spectra obtained from reference samples, applying transfer learning using a small quantity of such real XRF spectra increased the accuracy to 96%.
Due to these promising results, the network was also tested on select data acquired during macro XRF (MA-XRF) scanning of a painting to challenge the model with noisier spectra Although only tested on spectra from relatively simple paint passages, the results obtained suggest that the FP method can be used to create accurate synthetic XRF spectra of individual artists' pigments, free from X-ray tube effects, on which a classification model could be trained for application to real XRF data and that the method has potential to be extended to deal with more complex paint mixtures and stratigraphies.

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