水，空气相关离子及溶质的组织：汽/液，液/固界面振动和频光谱测量

he nature of water's hydrogen-bonding network is a vital in fluence on the chemistry that occurs at interfaces, but a complete understanding of interfacial water has proven elusive. Even-order nonlinear optical spectroscopies, such as vibrational sum frequency generation (VSFG) spectroscopy and heterodyne detected phase-sensitive sum frequency generation (PS-SFG) spectroscopy, are inherently surface specific. With the advent of advances in these spectroscopic techniques, researchers can now explore many longstanding questions about the dynamics and structures present at the vapor
water and water
solid interfaces. Of special interest to the atmospheric chemistry community is the accommodation of ions and solutes by water's hydrogen-bonding network. A better understanding of how ions and solutes behave in hydrogen-bonded water has afforded a fresh perspective of aqueous aerosols, because the interactions involved therein drive phenomena such as the hydrolysis of atmospheric chemical species. In this Account, we present work from our laboratory focusing on applying VSFG and the recently developed PSSFG techniques to probe the perturbation ofwater's hydrogen-bonding network at the vapor
water interface by a variety of ions and solutes. We also present very recent results from our laboratory on the direct observation of the adsorption of ions at the water
CaF2 interface.