The growth of aerosol particles is intimately related to chemical reactions in the gas phase and particle phase and at gas-aerosol particle interfaces. While chemical reactions in gas and particle phases are well documented, there is very little information regarding interface-related reactions. The interface of gas-aerosol particles not only facilitates a physical channel for organic species to enter and exit but also provides a necessary lane for culturing chemical reactions. The physical and chemical properties of gas-particle interfaces have not been studied extensively, nor have the reactions occurring at the interfaces been well researched. This is mainly due to the fact that there is a lack of suitable in situ interface-sensitive analytical techniques for direct measurements of interfacial properties. The motivation behind this research is to understand how interfaces play a role in the growth of aerosol particles. We have developed in situ interface-specific second harmonic scattering to examine interfacial behaviors of molecules of aerosol particles under different relative humidity (RH) and salt concentrations. Both the relative humidity and salt concentration can change the particle size and the phase of the aerosol. RH not only varies the concentration of solutes inside aerosol particles but also changes interfacial hydration in local regions. Organic molecules were found to exhibit distinct behaviors at the interfaces and bulk on NaCl particles under different RH levels. Our quantitative analyses showed that the interfacial adsorption free energies remain unchanged while interfacial areas increase as the relative humidity increases. Furthermore, the surface tension of NaCl particles decreases as the RH increases. Our experimental findings from the novel nonlinear optical scattering technique stress the importance of interfacial water behaviors on aerosol particles in the atmosphere.