A1 Refereed original research article in a scientific journal

Compatibility of quantitative X-ray spectroscopy with continuous distribution models of water at ambient conditions



Authors: Johannes Niskanen, Mattis Fondell, Christoph J. Sahle, Sebastian Eckert, Raphael M. Jay, Keith Gilmore, Annette Pietzsch, Marcus Dantz, Xingye Lu, Daniel E. McNally, Thorsten Schmitt, Vinicius Vaz da Cruz, Victor Kimberg, Faris Gel’mukhanov, Alexander Föhlisch

Publisher: NATL ACAD SCIENCES

Publication year: 2019

Journal: Proceedings of the National Academy of Sciences of the United States of America

Journal name in source: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA

Journal acronym: P NATL ACAD SCI USA

Volume: 116

Issue: 10

First page : 4058

Last page: 4063

Number of pages: 6

ISSN: 0027-8424

DOI: https://doi.org/10.1073/pnas.1815701116

Self-archived copy’s web address: https://research.utu.fi/converis/portal/detail/Publication/39918592


Abstract
The phase diagram of water harbors controversial views on underlying structural properties of its constituting molecular moieties, its fluctuating hydrogen-bonding network, as well as pair-correlation functions. In this work, long energy-range detection of the X-ray absorption allows us to unambiguously calibrate the spectra for water gas, liquid, and ice by the experimental atomic ionization cross-section. In liquid water, we extract the mean value of 1.74 +/- 2.1% donated and accepted hydrogen bonds per molecule, pointing to a continuous-distribution model. In addition, resonant inelastic X-ray scattering with unprecedented energy resolution also supports continuous distribution of molecular neighborhoods within liquid water, as do X-ray emission spectra once the femtosecond scattering duration and proton dynamics in resonant X-ray-matter interaction are taken into account. Thus, X-ray spectra of liquid water in ambient conditions can be understood without a two-structure model, whereas the occurrence of nanoscale-length correlations within the continuous distribution remains open.

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