Johannes Niskanen, Mattis Fondell, Christoph J. Sahle, Sebastian Eckert, Raphael Martin Jay, Keith Gilmore, Annette Pietzsch, Marcus Dantz, Xingye Lu, Daniel E. McNally, Thorsten Schmitt, Vinicius Vaz da Cruz, Victor Kimberg, Alexander Föhlisch, Faris Gel’mukhanov
- 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-lengthThe 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.…
MetadatenAuthor details: | Johannes Niskanen, Mattis FondellORCiD, Christoph J. SahleORCiD, Sebastian EckertORCiDGND, Raphael Martin JayORCiDGND, Keith GilmoreORCiD, Annette PietzschORCiD, Marcus Dantz, Xingye LuORCiD, Daniel E. McNally, Thorsten Schmitt, Vinicius Vaz da CruzORCiD, Victor KimbergORCiD, Alexander FöhlischORCiDGND, Faris Gel’mukhanovORCiD |
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DOI: | https://doi.org/10.1073/pnas.1815701116 |
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ISSN: | 0027-8424 |
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Pubmed ID: | https://pubmed.ncbi.nlm.nih.gov/30782822 |
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Title of parent work (English): | Proceedings of the National Academy of Sciences of the United States of America |
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Publisher: | National Acad. of Sciences |
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Place of publishing: | Washington |
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Publication type: | Article |
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Language: | English |
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Date of first publication: | 2019/02/19 |
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Publication year: | 2019 |
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Release date: | 2021/03/17 |
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Tag: | X-ray spectroscopy; continuous distribution model; structure of water |
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Volume: | 116 |
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Issue: | 10 |
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Number of pages: | 6 |
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First page: | 4058 |
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Last Page: | 4063 |
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Funding institution: | European Research Council under the Horizon 2020 European Union Framework Program for Research and Innovation [669531]; Swiss National Science Foundation (SNSF) through the National Centre for Competence in Research MARVEL [51NF40_141828]; Swiss National Science Foundation (SNSF) through the Sinergia network Mott Physics Beyond the Heisenberg Model [CRSII2_160765/1]; Swiss National Science Foundation (SNSF) through the Deutschland-Austria-Confoederatio Helvetica project [200021L [290605]; Ministry of Education and Science of the Russian FederationMinistry of Education and Science, Russian Federation [3.2662.2017]; Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation [KAW-2013.0020]; Swedish Research CouncilSwedish Research Council |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Physik und Astronomie |
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DDC classification: | 5 Naturwissenschaften und Mathematik / 52 Astronomie / 520 Astronomie und zugeordnete Wissenschaften |
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| 5 Naturwissenschaften und Mathematik / 53 Physik / 530 Physik |
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Peer review: | Referiert |
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Publishing method: | Open Access / Hybrid Open-Access |
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License (German): | CC-BY - Namensnennung 4.0 International |
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