The gas-aerosol particle interface is believed to contribute to the growth of secondary organic aerosols in the atmosphere. Despite its importance, the chemical composition of the interface has not been probed directly because of a lack of suitable interface-specific analytical techniques. The preliminary result in our early work has demonstrated direct observations of molecules at the gas-aerosol particle interface with the development of second harmonic scattering (SHS). However, the SHS technique is far away from being an analytical tool of chemical compositions at the gas-aerosol particle interface. In this work, we continued to develop the interface-specific SHS for in situ chemical analysis of molecules at the gas-aerosol particle interface. As an example, we demonstrated coherent SHS signal of a new SHS probe, crystal violet (CV), from interfaces of aerosol particles. The development of the SHS technique includes: (1) Optimization for a more efficient femtosecond laser system in the generation of SHS from aerosol particles. A near 5 MHz repetition rate of a femtosecond laser was found to be optimal for the generation of SHS; (2) exploration of a more effective detector for SHS of aerosol particles. We found that both a CCD detector and a single-photon counter produce similar signal-to-noise ratios of the interfacial SHS signals from aerosol particles. The CCD detector is a more effective option for the detection of SHS and could greatly reduce sampling time of the interfacial responses; (3) combination of the optimal laser system with the CCD detector, which has greatly improved the detection sensitivity of interfacial molecules by more than 2 orders of magnitude and could potentially detect interfacial SHS from a single aerosol particle. These experimental results not only provided a thorough analysis of the SHS technique but also built a solid foundation for further development of a new vibrational sum frequency scattering (SFS) technique for chemical structures at the gas-aerosol particle interface.