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

作者：Sit Patrick H L^*; Bellin Christophe; Barbiellini Bernardo; Testemale D; Hazemann J L; Buslaps T; Marzari Nicola; Shukla Abhay

来源：Physical Review B, 2007, 76(24): 245413.

DOI：10.1103/PhysRevB.76.245413

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.

• 出版日期2007-12
• 单位东北大学