Photochemical production of ozone in the upper troposphere in association with cumulus convection over Indonesia

Abstract

The Biomass Burning and Lightning Experiment phase A (BIBLE‐A) aircraft observation campaign was conducted from 24 September to 10 October 1998, during a La Niña period. During this campaign, distributions of ozone and its precursors (NO, CO, and nonmethane hydrocarbons (NMHCs)) were observed over the tropical Pacific Ocean, Indonesia, and northern Australia. Mixing ratios of ozone and its precursors were very low at altitudes between 0 and 13.5 km over the tropical Pacific Ocean. The mixing ratios of ozone precursors above 8 km over Indonesia were often significantly higher than those over the tropical Pacific Ocean, even though the prevailing easterlies carried the air from the tropical Pacific Ocean to over Indonesia within several days. For example, median NO and CO mixing ratios in the upper troposphere were 12 parts per trillion (pptv) and 72 parts per billion (ppbv) over the tropical Pacific Ocean and were 83 pptv and 85 ppbv over western Indonesia, respectively. Meteorological analyses and high ethene (C2H4) mixing ratios indicate that the increase of the ozone precursors was caused by active convection over Indonesia through upward transport of polluted air, mixing, and lightning all within the few days prior to observation. Sources of ozone precursors are discussed by comparing correlations of some NMHCs and CH3Cl concentrations with CO between the lower and upper troposphere. Biomass burning in Indonesia was nearly inactive during BIBLE‐A and was not a dominant source of the ozone precursors, but urban pollution and lightning contributed importantly to their increases. The increase in ozone precursors raised net ozone production rates over western Indonesia in the upper troposphere, as shown by a photochemical model calculation. However, the ozone mixing ratio (∼20 ppbv) did not increase significantly over Indonesia because photochemical production of ozone did not have sufficient time since the augmentation of ozone precursors. Backward trajectories show that many air masses sampled over the ocean south of Indonesia and over northern Australia passed over western Indonesia 4–9 days prior to being measured. In these air masses the mixing ratios of ozone precursors, except for short‐lived species, were similar to those over western Indonesia. In contrast, the ozone mixing ratio was higher by about 10 ppbv than that over Indonesia, indicating that photochemical production of ozone occurred during transport from Indonesia. The average rate of ozone increase (1.8 ppbv/d) during this transport is similar to the net ozone formation rate calculated by the photochemical model. This study shows that active convection over Indonesia carried polluted air upward from the surface and had a discernable influence on the distribution of ozone in the upper troposphere over the Indian Ocean, northern Australia, and the south subtropical Pacific Ocean, combined with NO production by lightning.