Chemical composition and mixing state of aerosols collected over an 11,000 km latitudinal cruise in the Pacific Ocean are reported here as determined by a new application of Raman spectroscopy. The Raman microspectroscopy technique employs a Raman spectrometer coupled to an optical microscope to identify the chemical composition and internal mixing state of single particles. By analyzing multiple particles in a collected ensemble, the degree of external mixing of particles was also determined. To lend context to the Pacific aerosol population sampled, atmospheric aerosol concentration, and the critical supersaturation required for the aerosols to activate as cloud condensation nuclei, and chlorophyll a concentration in the underlying water (a metric for phytoplankton biomass in the ocean) were also obtained. Our results indicate that long chain organic molecules were prevalent in the marine aerosol samples throughout the cruise, including during coastal and open ocean locations, in both hemispheres, and in the seasons of autumn and spring. Long chain organic compounds tended to be present in internal mixtures with other organic and inorganic components. Although variations in the fraction of aerosols activated as CCN were observed, no simple correlation between organics and CCN activation was found. According to our measurements, marine aerosol in the Pacific Ocean may be generally characterized as multicomponent aerosol containing and often dominated by a high organic fraction. Our results suggest that the prevalence of organics and the high degree of internal mixing of aerosol must be accounted for in accurate modeling of the role of marine aerosols in cloud formation and climate.
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