Partial Density of States Representation for Accurate Deep Neural Network Predictions of X-ray Spectra

09 February 2024, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


The performance of a Machine Learning (ML) algorithm for chemistry is highly contingent upon the architect’s choice of input representation. This work introduces the partial density of states (p-DOS) descriptor: a novel, quantum- inspired structural representation which encodes relevant electronic information for machine learning models seeking to simulate X-ray spectroscopy. p-DOS uses a minimal basis set in conjunction with a guess (non-optimised) electronic configuration to extract and then discretise the density of states (DOS) of the absorbing atom to form the input vector. We demonstrate that while the electronically-focused p-DOS performs well in isolation, optimal performance is achieved when supplemented with nuclear structural information imparted via a geometric representation. p-DOS provides a description of the key electronic properties of a system which is not only concise and computationally efficient, but also independent of molecular size or choice of basis set. It can be rapidly generated, facilitating its application with large training sets. Its performance is demonstrated using a wide variety of examples at the sulphur K-edge, including the prediction of ultrafast X-ray spectroscopic signal associated with photoexcited 2(5H)-thiophenone. These results highlight the potential for ML models developed using p-DOS to contribute to the interpretation and predic- tion of experimental results made possible by emergent cutting-edge technologies, especially X-ray free electron lasers.


X-ray absorption Spectroscopy
Deep Neural Networks
Ultrafast Dynamics
Computational Spectroscopy

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