A1 Refereed original research article in a scientific journal
Generating interstitial water within the persisting tetrahedral H-bond network explains density increase upon compressing liquid water
Authors: Förster, Mirko; Ukoji, Nnanna; Sahle, Christoph J.; Niskanen, Johannes; Sakrowski, Robin; Surmeier, Göran; Weis, Christopher; Irifune, Tetsuo; Imoto, Sho; Yavas, Hasan; Huotari, Simo; Marx, Dominik; Sternemann, Christian; Tse, John S.
Publisher: National Academy of Sciences
Publication year: 2024
Journal: Proceedings of the National Academy of Sciences of the United States of America
Article number: e2403662121
Volume: 121
Issue: 39
eISSN: 1091-6490
DOI: https://doi.org/10.1073/pnas.2403662121(external)
Web address : https://doi.org/10.1073/pnas.2403662121(external)
Self-archived copy’s web address: https://research.utu.fi/converis/portal/detail/Publication/457889120(external)
Despite its ubiquitous nature, the atomic structure of water in its liquid state is still controversially debated. We use a combination of X-ray Raman scattering spectroscopy in conjunction with ab initio and path integral molecular dynamics simulations to study the local atomic and electronic structure of water under high pressure conditions. Systematically increasing fingerprints of non-hydrogen-bonded H2O molecules in the first hydration shell are identified in the experimental and computational oxygen K-edge excitation spectra. This provides evidence for a compaction mechanism in terms of a continuous collapse of the second hydration shell with increasing pressure via generation of interstitial water within locally tetrahedral hydrogen-bonding environments.
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Funding information in the publication:
We acknowledge the European Synchrotron Radiation Facility for provision of synchrotron radiation facilities for proposal IH-SC-1598 and we would like to thank F. Gerbon for assistance and support in using beamline ID20. We acknowledge Deutsches Elektronen-Synchrotron (DESY) (Hamburg, Germany), a member of the Helmholtz Association HGF, for the provision of experimental facilities. Parts of this research were carried out at PETRA III. Beamtime at beamline P01 was allocated for proposal I-20170393. We acknowledge the Taiwan beamline BL12XU of Spring8 for initial test studies. We thank M. Paulus, F. Lehmkühler and M. Tolan for fruitful discussions. Funded by the Deutsche Forschungsgemeinschaft (German Research Foundation) under Germany’s Excellence Strategy—EXC 2033—390677874—RESOLV. The The ab initio molecular dynamics simulations were carried out using SuperMUC/NG at LRZ München as well as HPC–RESOLV, HPC@ZEMOS and BOVILAB@RUB. J.S.T and N.U. wish to thank Dr. X. Yong for assistance with the path integral centroid molecular dynamics simulations. The Natural Sciences and Engineering Research Council of Canada is acknowledged for support via a DISCOVERY grant.
