Measurements of the Size-Resolved Chemical Composition of Marine Boundary Layer Aerosols in Asian Outflow During the ACE-Asia Campaign

The size and chemical composition of individual particles were evaluated with high temporal resolution during the Asian Pacific Regional Aerosol Chemical Characterization Experiment (ACE-Asia) using a transportable aerosol time-of-flight mass spectrometer (ATOFMS) aboard the NOAA Research Vessel Ronald H. Brown. ATOFMS allows characterization of the aerodynamic diameter and chemical composition of individual particles from a polydisperse aerosol. This technique couples aerodynamic particle sizing with time-of-flight mass spectrometry in a single instrument, providing both positive and negative ion mass spectra for each detected particle which are employed to classify the particles into different classes using criteria based searches and a neural network algorithm, ART-2a. Size-resolved chemical characteristics of sampled particles under different synoptic meteorological patterns and at various locations and distances from continental influences are discussed in detail, with special focus given to the associations among different species and the variability in the degrees of aging, reaction, and/or mixing, which can alter the optical properties of these particles. Changes in the aerosol chemical characteristics due to heterogeneous reactions are evidenced in the mass spectra of detected particles by the presence and intensity of specific ion markers (e.g., sulfate, nitrate). The ability to differentiate between particles that have undergone heterogeneous reactions is relevant since these reactions affect several aerosol attributes, such as hygroscopic, optical, and radiative properties. Particularly, heterogeneous reactions/ nucleation on sea-salt and dust particles are discussed together with results of comparison efforts with some relevant laboratory and source characterization studies that allow determination of corresponding ion markers, relative ratios among species, and probable sources from a single particle perspective.