Hydrogen bonding and coordination in normal and supercritical water from x-ray inelastic scattering

A direct measure of hydrogen bonding in water under conditions ranging from the normal state to the supercritical regime is derived from first-principles calculations for the Compton scattering of inelastically scattered x rays. First, we show that a measure of the number of electrons n(e) involved...

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Bibliographic Details
Published in:Physical review. B, Condensed matter and materials physics Condensed matter and materials physics, 2007-12, Vol.76 (24), Article 245413
Main Authors: Sit, Patrick H.-L., Bellin, Christophe, Barbiellini, Bernardo, Testemale, D., Hazemann, J.-L., Buslaps, T., Marzari, Nicola, Shukla, Abhay
Format: Article
Language:English
Subjects:
BONDING
COMPTON EFFECT
CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY
Earth Sciences
ELECTRONS
Environmental Sciences
Geochemistry
Global Changes
HYDROGEN
INELASTIC SCATTERING
Sciences of the Universe
SIMULATION
SUPERCRITICAL STATE
THERMODYNAMICS
WATER
X RADIATION
X-RAY DIFFRACTION
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Summary:A direct measure of hydrogen bonding in water under conditions ranging from the normal state to the supercritical regime is derived from first-principles calculations for the Compton scattering of inelastically scattered x rays. First, we show that a measure of the number of electrons n(e) involved in hydrogen bonding at varying thermodynamic conditions can be directly obtained from Compton profile differences. Then, we use first-principles simulations to provide a connection between n(e) and the number of hydrogen bonds n(HB). Our study shows that over the broad range studied, the relationship between n(e) and n(HB) is linear, allowing for a direct measure of bonding and coordination in water by coupling simulations with experiments. In particular, the transition to supercritical state is characterized by a sharp increase in the number of water monomers but also displays a significant number of residual dimers and trimers.
ISSN:1098-0121
1550-235X
DOI:10.1103/PhysRevB.76.245413