Site-Selective Functional Group Classification of Auger-Electron Spectra and Core-Electron Binding Energies with Convolutional Neural Networks

RESUMO

X-ray spectroscopy techniques probe chemical states in systems with atom-site specificity; however, the site-selective characterization of local bond environments in novel research materials often relies on a combination of reference spectra, multiple complementary spectroscopic techniques and electronic structure calculations. Auger-electron spectroscopy has long accompanied x-ray photoelectron spectroscopy as a second modality to resolve chemical states with overlapping core-electron binding energies. Here I show that the wealth of information encoded in the Auger spectrum offers the opportunity to train convolutional neural networks for site-selective functional group classification in organic molecules directly from the Auger spectrum lineshape. Furthermore, the inclusion of the core-electron binding energy as an additional modality improves the classification, either by augmenting the input fitted intensities with the binding energy or by conditioning the classification on the binding energy via feature-wise linear modulation layers. The latter approach was previously developed for visual reasoning in image classification, and the present results show that this is the more robust approach for including the binding energy. This work demonstrates the potential for new data-driven characterization capabilities in spectroscopic techniques that are information-rich but difficult to interpret.