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

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

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

Alexander Föhlisch
Keith Gilmore
Victor Kimberg
Christoph J. Sahle
Raphael M. Jay
Faris Gel’mukhanov
Marcus Dantz
Annette Pietzsch
Daniel E. McNally
Vinicius Vaz da Cruz
Sebastian Eckert
Xingye Lu
Johannes Niskanen
Thorsten Schmitt
Mattis Fondell
Katso/Avaa
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NATL ACAD SCIENCES
doi:10.1073/pnas.1815701116
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Julkaisun pysyvä osoite on:
https://urn.fi/URN:NBN:fi-fe2021042823958
Tiivistelmä
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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