A novel nonlinear Raman spectroscopic technique has been used to image the extent of hydrogen bonding at water aerosol interfaces. The aerosols probed were generated in the laboratory using the vibrating orifice technique. The spectroscopic results show that the aerosols suffer severe hydrogen bond disruption and that the structural impairment is more pronounced at the surface. Laboratory aerosols generated this way do not mimic those found naturally. Thus mass accommodation coefficients measured using such aerosols should not be used in global climate-modeling calculations. ¿ American Geophysical Union 1994