An ab Initio Molecular Dynamics Study of the Aqueous Liquid-Vapor Interface
Top Cited Papers
- 30 January 2004
- journal article
- other
- Published by American Association for the Advancement of Science (AAAS) in Science
- Vol. 303 (5658) , 658-660
- https://doi.org/10.1126/science.1092787
Abstract
We present an ab initio molecular dynamics simulation of the aqueous liquid-vapor interface. Having successfully stabilized a region of bulk water in the center of a water slab, we were able to reproduce and further quantify the experimentally observed abundance of surface “acceptor-only”(19%) and “single-donor”(66%) moieties as well as substantial surface relaxation approaching the liquid-vapor interface. Examination of the orientational dynamics points to a faster relaxation in the interfacial region. Furthermore, the average value of the dipole decreases and the average value of the highest occupied molecular orbital for each water molecule increases approaching the liquid-vapor interface. Our results support the idea that the surface contains, on average, far more reactive states than the bulk.Keywords
This publication has 28 references indexed in Scilit:
- Water in Contact with Extended Hydrophobic Surfaces: Direct Evidence of Weak DewettingPhysical Review Letters, 2003
- Temperature-Dependent Hydrogen-Bond Geometry in Liquid WaterPhysical Review Letters, 2003
- Physics of Hydrophobic CavitiesLangmuir, 2003
- Hydrogen-Bonding Interactions at the Vapor/Water Interface Investigated by Vibrational Sum-Frequency Spectroscopy of HOD/H2O/D2O Mixtures and Molecular Dynamics SimulationsThe Journal of Physical Chemistry B, 2002
- X-ray Spectroscopy of Liquid Water MicrojetsThe Journal of Physical Chemistry B, 2001
- A hybrid Gaussian and plane wave density functional schemeMolecular Physics, 1997
- Ab initio molecular dynamics simulation of liquid water: Comparison of three gradient-corrected density functionalsThe Journal of Chemical Physics, 1996
- Hydrogen-bond kinetics in liquid waterNature, 1996
- The Volume of Atoms on the Protein Surface: Calculated from Simulation, using Voronoi PolyhedraJournal of Molecular Biology, 1995
- Vibrational Spectrum of Water at the Liquid/Vapor InterfacePhysical Review Letters, 1994