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Simulating the Ghost: Quantum Dynamics of the Solvated Electron

preprint
submitted on 23.06.2020 and posted on 26.06.2020 by Jinggang Lan, Venkat Kapil, Piero Gasparotto, Michele Ceriotti, Marcella Iannuzzi, Vladimir V. Rybkin
The nature of bulk hydrated electron has been a challenge for both experiment and theory due to its short life time and high reactivity, and the need for a high-level of electronic structure theory to achieve predictive accuracy. The lack of a classical atomistic structural formula makes it exceedingly difficult to model the solvated electron using conventional empirical force fields, which describe the system in terms of interactions between point particles associated with atomic nuclei. Here we overcome this problem using a machine-learning model, that is sufficiently flexible to describe the effect of the excess electron on the structure of the surrounding water, without including the electron in the model explicitly. The resulting potential is not only able to reproduce the stable cavity structure, but also recovers the correct localization dynamics that follows the injection of an electron in neat water. The machine learning model achieves the accuracy of the state-of-the-art correlated wave function method it is trained on. It is sufficiently inexpensive to afford a full quantum statistical and dynamical description, and allows us to achieve a highly accurate determination of the structure, diffusion mechanisms and vibrational spectroscopy of the solvated electron

Funding

SNF

History

Email Address of Submitting Author

jinggang.lan@chem.uzh.ch

Institution

University of Zurich

Country

Switzerland

ORCID For Submitting Author

0000-0001-6353-2539

Declaration of Conflict of Interest

no conflict of interest

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