Understanding X-ray absorption in liquid water using triple excitations in multilevel coupled cluster theory

Sarai Dery Folkestad, Alexander C. Paul, Regina Paul (Née Matveeva), Sonia Coriani, Michael Odelius, Marcella Iannuzzi and Henrik Koch ()
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Sarai Dery Folkestad: Norwegian University of Science and Technology, NTNU
Alexander C. Paul: Norwegian University of Science and Technology, NTNU
Regina Paul (Née Matveeva): Norwegian University of Science and Technology, NTNU
Sonia Coriani: Technical University of Denmark, DTU
Michael Odelius: Stockholm University
Marcella Iannuzzi: University of Zurich
Henrik Koch: Norwegian University of Science and Technology, NTNU

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract X-ray absorption (XA) spectroscopy is an essential experimental tool to investigate the local structure of liquid water. Interpretation of the experiment poses a significant challenge and requires a quantitative theoretical description. High-quality theoretical XA spectra require reliable molecular dynamics simulations and accurate electronic structure calculations. Here, we present the first successful application of coupled cluster theory to model the XA spectrum of liquid water. We overcome the computational limitations on system size by employing a multilevel coupled cluster framework for large molecular systems. Excellent agreement with the experimental spectrum is achieved by including triple excitations in the wave function and using molecular structures from state-of-the-art path-integral molecular dynamics. We demonstrate that an accurate description of the electronic structure within the first solvation shell is sufficient to successfully model the XA spectrum of liquid water within the multilevel framework. Furthermore, we present a rigorous charge transfer analysis of the XA spectrum, which is reliable due to the accuracy and robustness of the electronic structure methodology. This analysis aligns with previous studies regarding the character of the prominent features of the XA spectrum of liquid water.

Date: 2024
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DOI: 10.1038/s41467-024-47690-x

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