Intermediate-range order in water ices: Nonresonant inelastic x-ray scattering measurements and real-space full multiple scattering calculations

Fister, Timothy T.; Nagle, K. P.; Vila, Fernando D.; Seidler, Gerald T.; Hamner, Chris; Cross, J. O.; Rehr, J. J.

doi:10.1103/physrevb.79.174117

Cited by 27 publications

(19 citation statements)

References 106 publications

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“…The computational cost of such methods, however, forbids this approach in the current case. Using a real-space multiple scattering approach to calculate the oxygen K-edge in different ice phases results in a post-edge feature that closely resembles the experimental findings but fails to reproduce the pre-and near-edge (44). In our results, good quantitative agreement is achieved when comparing the energy loss position of the pre-edge for all p, T conditions (Fig.…”

Section: Resultsmentioning

confidence: 46%

Microscopic structure of water at elevated pressures and temperatures

Sahle

Sternemann

Schmidt

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

136

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We report on the microscopic structure of water at sub-and supercritical conditions studied using X-ray Raman spectroscopy, ab initio molecular dynamics simulations, and density functional theory. Systematic changes in the X-ray Raman spectra with increasing pressure and temperature are observed. Throughout the studied thermodynamic range, the experimental spectra can be interpreted with a structural model obtained from the molecular dynamics simulations. A spatial statistical analysis using Ripley's K-function shows that this model is homogeneous on the nanometer length scale. According to the simulations, distortions of the hydrogenbond network increase dramatically when temperature and pressure increase to the supercritical regime. In particular, the average number of hydrogen bonds per molecule decreases to ≈0.6 at 600°C and p = 134 MPa.supercritical water | water structure | X-ray scattering | X-ray scattering spectroscopy

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Section: Resultsmentioning

confidence: 46%

Microscopic structure of water at elevated pressures and temperatures

Sahle

Sternemann

Schmidt

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

136

View full text Add to dashboard Cite

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“…The fact that q can be large requires the expansion of the exponential in the matrix element beyond the dipole contributions when the condition qr << 1 is not valid. These effects have been first studied on Li by Krisch et al (65), and numerous recent studies have focused on investigating non-dipole contributions both experimentally and theoretically, including the work on water and ice by Fister et al (57). For 1s electrons the approximate magnitude of r is given by the spatial extension of the core hole wave function r ~ a/Z, where a = 0.53 Å is the Bohr radius and Z the charge of the absorbing atom.…”

Section: Ii2 Principle Of X-ray Raman Scatteringmentioning

confidence: 99%

X-ray absorption spectroscopy and X-ray Raman scattering of water and ice; an experimental view

Nilsson

Nordlund

Waluyo

et al. 2010

Journal of Electron Spectroscopy and Related Phenomena

179

290

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Here we present a review of x-ray absorption spectroscopy and x-ray Raman scattering with the perspective to understand the spectra of water including changes with temperature, mass of the water molecule and presence of monovalent ions. The different detection schemes are discussed and it is concluded that transmission x-ray absorption measurements, using a small area where the thickness is uniform, and x-ray Raman scattering give the most reliable spectra. Different model systems are discussed such as the surface and bulk of ice and various adsorbed monolayer structures on metal surfaces.

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“…Here, the study of absorption edges in the soft X-ray regime by hard X-rays, denoted as X-ray Raman scattering, provided groundbreaking results on the local structure of liquids and amorphous solids and extended results of conventional soft X-ray absorption experiments. In particular, studies of the oxygen K-edge in liquid and supercritical water, [27][28][29][30][31][32] in different ices 30,[33][34][35] and waterbased two-component systems [36][37][38][39] challenged the question of water's microscopic structure.…”

Section: Methodsmentioning

confidence: 99%

Intramolecular structure and energetics in supercooled water down to 255 K

Lehmkühler

Forov

Büning

et al. 2016

Phys. Chem. Chem. Phys.

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We studied the structure and energetics of supercooled water by means of X-ray Raman and Compton scattering. Under supercooled conditions down to 255 K, the oxygen K-edge measured by X-ray Raman scattering suggests an increase of tetrahedral order similar to the conventional temperature effect observed in non-supercooled water. Compton profile differences indicate contributions beyond the theoretically predicted temperature effect and provide a deeper insight into local structural changes. These contributions suggest a decrease of the electron mean kinetic energy by 3.3 ± 0.7 kJ (mol K)(-1) that cannot be modeled within established water models. Our surprising results emphasize the need for water models that capture in detail the intramolecular structural changes and quantum effects to explain this complex liquid.

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Intermediate-range order in water ices: Nonresonant inelastic x-ray scattering measurements and real-space full multiple scattering calculations

Cited by 27 publications

References 106 publications

Microscopic structure of water at elevated pressures and temperatures

Microscopic structure of water at elevated pressures and temperatures

X-ray absorption spectroscopy and X-ray Raman scattering of water and ice; an experimental view

Intramolecular structure and energetics in supercooled water down to 255 K

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