Understanding the origin of black carbon in the atmospheric brown cloud over the Indian Ocean

Atmospheric particulate matter samples were collected at two Maldives climate observatories from 30 August 2004 to 21 January 2005. This time period encompassed both wet and dry seasons, which correspond to low and high aerosol loadings. High aerosol loadings were observed in the northern sampling site in Hanimaadhoo, caused by long‐range transport from south and Southeast Asia, whereas the southern sampling site, Gan, was not subject to as much continental inflow. The polluted period began in mid‐November and lasted through the remainder of the sampling period. Fine particulate matter during this time was characterized by relatively high concentrations of aerosol mass and elemental carbon. Concentrations of water‐soluble potassium, sulfate, levoglucosan, polyaromatic hydrocarbons, aliphatic diacids, aromatic diacids, and trace metals increased over the clean, transition, and polluted dry season. Organic speciation suggested that significant secondary organic aerosol formation occurred during the polluted dry season, meaning that traditional methods of source identification relying on fixed elemental and organic carbon ratios between source and receptors are not sufficient. Well‐studied molecular markers for combustion sources were not adequate in fully attributing elemental carbon over the northern Indian Ocean to specific sources. Further source profiling of south and Southeast Asian biofuels and fossil fuels is recommended. A receptor‐based positive matrix factorization model was applied to fine particulate matter trace metal measurements and showed that biofuel burning and fossil fuel combustion were equally important sources of elemental carbon during the polluted dry season.