Organic molecules
at the gas-particle interface of atmospheric
aerosols influence the heterogeneous chemistry of the aerosol and
impact climate properties. The ability to probe the molecules at the
aerosol particle surface in situ therefore is important but has been
proven challenging. We report the first successful observations of
molecules at the surface of laboratory-generated aerosols suspended
in air using the surface-sensitive technique second harmonic light
scattering (SHS). As a demonstration, we detect trans-4-[4-(dibutylamino)styryl]-1-methylpyridinium
iodide and determine its population and adsorption free energy at
the surface of submicron aerosol particles. This work illustrates
a new and versatile experimental approach for studying how aerosol
composition may affect the atmospheric properties