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SSA plays a major role in influencing climate however the overall impacts remain poorly understood due to the overall chemical complexity. SSA is comprised of a mixture of inorganic and organic components in varying proportions that change as a function of particle size and seawater composition. In this study, nascent SSA particles were produced using breaking waves, resulting in compositions and sizes representative of the open ocean. The composition of individual SSA particles ranging in size from ca. 0.15 to 10 μm is measured using Raman microspectroscopy, while the interfacial composition of collections of size-resolved particles is probed by sum frequency generation ( SFG). Raman spectra of single particles have bands in the 980 to 1030 cm −1 region associated with the symmetric stretch of the sulfate anion, the 2800 to 3000 cm −1 region associated with carbon–hydrogen stretches, and from 3200–3700 cm −1 associated with the oxygen–hydrogen stretches of water.

The relative intensities of these features showed a strong dependence on particle size.

In particular, submicrometer particles exhibited a larger amount of organic matter compared to supermicrometer particles. However, for external surfaces of homogeneous SSA particles ( i.e.

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