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An On-the-Fly Deep Neural Network for Simulating Time-Resolved Spectroscopy: Predicting the Ultrafast Ring Opening Dynamics of 1,2-Dithiane

Lookup NU author(s): Clelia Middleton, Conor Rankine, Professor Thomas Penfold



This work is licensed under a Creative Commons Attribution 4.0 International License (CC BY 4.0).


Revolutionary developments in ultrafast light source technology are enabling experimental spectroscopists to probe the structural dynamics of molecules and materials on the femtosecond timescale. The capacity to investigate ultrafast processes afforded by these resources accordingly inspires the- oreticians to carry out high-level simulations which facilitate the interpretation of the underlying dynamics probed during these ultrafast experiments. In this Article, we implement a Deep Neural Network (DNN) to convert excited-state molecular dynamics simulations into time-resolved spectroscopic signals. Our DNN is trained on-the-fly from first-principles theoretical data obtained from a set of time-evolving molecular dynamics. The train-test process iterates for each time-step of the dynamics data until the network can predict spectra with sufficient accuracy to replace the computationally intensive quantum chemistry calculations required to produce them, at which point it simulates the time-resolved spectra for longer timescales. The potential of this approach is demonstrated by probing dynamics of the the ring opening of 1,2-dithiane using sulphur K-edge X-ray absorption spectroscopy. The benefits of this strategy will be more markedly apparent for simulations of larger systems which will exhibit a more notable computational burden, making this approach applicable to the study of a diverse range of complex chemical dynamics.

Publication metadata

Author(s): Middleton C, Rankine C, Penfold TJ

Publication type: Article

Publication status: Published

Journal: Physical Chemistry Chemical Physics

Year: 2023

Volume: 25

Pages: 13325-13334

Online publication date: 24/04/2023

Acceptance date: 21/04/2023

Date deposited: 05/05/2023

ISSN (print): 1463-9076

ISSN (electronic): 1463-9084

Publisher: Royal Society of Chemistry


DOI: 10.1039/D3CP00510K


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Funder referenceFunder name
EP/ R51309X/1