Long Range Transport was a Bigger NSS Source than DMS in the Remote Tropical MBL during PASE

DMS was not the principal source of non-sea salt sulfate (NSS) mass in the remote marine boundary layer during the Pacific Atmospheric Sulfur Experiment (PASE), according to an Eulerian sulfur budget model based on chemical concentrations measured from the NCAR C-130 in the tropical Pacific. Each of our three (DMS, SO2, and NSS) self-consistent monthly- average budgets includes terms for surface exchange, entrainment, divergence, chemical formation, and chemical loss. The budget-derived DMS emission was (2.7 × 0.5 μmol m-2 d-1, our budget 'units'). SO2 sources include DMS + OH (1.4 × 0.4 units, assuming γ = 0.75) and entrainment from the free troposphere (FT) (0.8 × 0.2 units). Clouds were the most important chemical reactors for SO2 (-1.0 × 0.5 units). SO2 loss terms also include divergence (-0.9 × 0.3 units), dry deposition (-0.5 × 0.2 units), and OH + SO2 (-0.22 × 0.05 units). The total SO2 loss balanced the SO2 source. We found negligible NSS on particles from 2.6 μm to 10 μm diameter, the sea salt mass peak. Fine-particle NSS sources include in-cloud oxidation of SO2 by H2O2 (1.0 × 0.5 units), OH + SO2 (0.19 × 0.05 units), and entrainment (1.1 × 0.3 units in clean conditions; twice that when continental pollution is present). Only about 1/4 of emitted DMS becomes NSS. The NSS sources from entrainment and from DMS are similar in magnitude.