Compatibility of quantitative X-ray spectroscopy with continuous distribution models of water at ambient conditions.
- Niskanen J Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz Zentrum Berlin für Materialien und Energie, D-12489 Berlin, Germany.
- Fondell M Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz Zentrum Berlin für Materialien und Energie, D-12489 Berlin, Germany.
- Sahle CJ European Synchrotron Radiation Facility 71, F-38043 Grenoble Cedex 9, France.
- Eckert S Institut für Physik und Astronomie, Universität Potsdam, D-14476 Potsdam-Golm, Germany.
- Jay RM Institut für Physik und Astronomie, Universität Potsdam, D-14476 Potsdam-Golm, Germany.
- Gilmore K European Synchrotron Radiation Facility 71, F-38043 Grenoble Cedex 9, France.
- Pietzsch A Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz Zentrum Berlin für Materialien und Energie, D-12489 Berlin, Germany.
- Dantz M Swiss Light Source, Photon Science Division, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
- Lu X Swiss Light Source, Photon Science Division, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
- McNally DE Swiss Light Source, Photon Science Division, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
- Schmitt T Swiss Light Source, Photon Science Division, Paul Scherrer Institut, 5232 Villigen PSI, Switzerland.
- Vaz da Cruz V Theoretical Chemistry and Biology, Royal Institute of Technology, SE-10691 Stockholm, Sweden.
- Kimberg V Theoretical Chemistry and Biology, Royal Institute of Technology, SE-10691 Stockholm, Sweden.
- Gel'mukhanov F Theoretical Chemistry and Biology, Royal Institute of Technology, SE-10691 Stockholm, Sweden.
- Föhlisch A Institute for Methods and Instrumentation for Synchrotron Radiation Research, Helmholtz Zentrum Berlin für Materialien und Energie, D-12489 Berlin, Germany; alexander.foehlisch@helmholtz-berlin.de.
- 2019-02-21
Published in:
- Proceedings of the National Academy of Sciences of the United States of America. - 2019
English
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.
- Language
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- English
- Open access status
- hybrid
- Identifiers
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- DOI 10.1073/pnas.1815701116
- PMID 30782822
- Persistent URL
- https://sonar.ch/global/documents/278543
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