Elucidation of Atmospheric Chemical Reaction Processes on the Surface of Aqueous Aerosols

基于和频产生谱的理论计算，阐述了水/气界面水的表面（氢键）结构与水气溶胶大气化学反应的关系。实验报告的光谱表明，水表面具有强氢键网络特征。然而，长期以来，人们对其产生机制知之甚少。本文通过对同位素稀释表面谱的摄动机理的研究，探讨了该谱的来源。发现特征谱出现在同位素稀释的频带中，谱源于与表面切向的强氢键网络。

Surface (hydrogen bonding) structures of water at water/vapor interface pertinent to atmospheric chemical reaction at aqueous aerosols are elucidated based on the theoretical calculations of sum frequency generation spectrum. Experiments have reported the spectrum suggesting the strong hydrogen bonding network characteristic to the water surface. However, the generation mechanism had been little understood for a long time. This study discussed origin of this spectrum by examining the perturbation mechanism of the spectrum at isotope diluted surface. It was found that the characteristic spectrum occurs in spate of the isotope dilution, and the spectrum originates from a strong hydrogen bonding network tangential to the surface.