LAMBE UMR8587, Université d'Evry val d'Essonne, Boulevard F Mitterrand, Bâtiment Maupertuis, F-91025 Evry, France.
J Phys Condens Matter. 2012 Mar 28;24(12):124106. doi: 10.1088/0953-8984/24/12/124106. Epub 2012 Mar 6.
The organization of water at the interface with silica and alumina oxides is analysed using density functional theory-based molecular dynamics simulation (DFT-MD). The interfacial hydrogen bonding is investigated in detail and related to the chemistry of the oxide surfaces by computing the surface charge density and acidity. We find that water molecules hydrogen-bonded to the surface have different orientations depending on the strength of the hydrogen bonds and use this observation to explain the features in the surface vibrational spectra measured by sum frequency generation spectroscopy. In particular, 'ice-like' and 'liquid-like' features in these spectra are interpreted as the result of hydrogen bonds of different strengths between surface silanols/aluminols and water.
使用基于密度泛函理论的分子动力学模拟（DFT-MD）分析了与二氧化硅和氧化铝氧化物界面处的水的组织。详细研究了界面氢键，并通过计算表面电荷密度和酸度将其与氧化物表面的化学性质相关联。我们发现，与表面氢键合的水分子的取向取决于氢键的强度，并利用这一观察结果来解释通过和频产生光谱测量得到的表面振动光谱中的特征。特别是，这些光谱中的“冰状”和“液态”特征被解释为表面硅醇/铝醇与水之间不同强度氢键的结果。
