Here we describe the use of Rutherford backscattering spectrometry (RBS) to measure quantitative in situ elemental profiles with high depth resolution, online and nondestructively, in volatile substances (liquid and frozen acids, ice). Samples for analysis are held in a chamber with controlled temperature and partial pressures designed to match conditions for aerosols in Earth's atmosphere. This technique is demonstrated in studies of water solubility in sulfuric acid, hydrochloric acid (HCl) on ice surfaces, the formation of a HCl-hexahydrate surface layer on evaporating HCl-doped ice, and the diffusion of water through this layer.