The impact of organic pollutants from Indonesian peatland fires on the tropospheric and lower stratospheric composition

摘要

The particularly strong dry season in Indonesia in 2015, caused by an exceptionally strong El Ni?o, led to severe peatland fires resulting in high volatile organic compound (VOC) biomass burning emissions. At the same time, the developing Asian monsoon anticyclone (ASMA) and the general upward transport in the Intertropical Convergence Zone (ITCZ) efficiently transported the resulting primary and secondary pollutants to the upper troposphere and lower stratosphere (UTLS). In this study, we assess the importance of these VOC emissions for the composition of the lower troposphere and the UTLS and investigate the effect of in-cloud oxygenated VOC (OVOC) oxidation during such a strong pollution event. This is achieved by performing multiple chemistry simulations using the global atmospheric model ECHAM/MESSy (EMAC). By comparing modelled columns of the biomass burning marker hydrogen cyanide ( HCN ) and carbon monoxide ( CO ) to spaceborne measurements from the Infrared Atmospheric Sounding Interferometer (IASI), we find that EMAC properly captures the exceptional strength of the Indonesian fires. In the lower troposphere, the increase in VOC levels is higher in Indonesia compared to other biomass burning regions. This has a direct impact on the oxidation capacity, resulting in the largest regional reduction in the hydroxyl radical ( OH ) and nitrogen oxides ( NO x ). While an increase in ozone ( O 3 ) is predicted close to the peatland fires, simulated O 3 decreases in eastern Indonesia due to particularly high phenol concentrations. In the ASMA and the ITCZ, the upward transport leads to elevated VOC concentrations in the lower stratosphere, which results in the reduction of OH and NO x and the increase in the hydroperoxyl radical ( HO 2 ). In addition, the degradation of VOC emissions from the Indonesian fires becomes a major source of lower stratospheric nitrate radicals ( NO 3 ), which increase by up to 20? % . Enhanced phenol levels in the upper troposphere result in a 20? % increase in the contribution of phenoxy radicals to the chemical destruction of O 3 , which is predicted to be as large as 40? % of the total chemical O 3 loss in the UTLS. In the months following the fires, this loss propagates into the lower stratosphere and potentially contributes to the variability of lower stratospheric O 3 observed by satellite retrievals. The Indonesian peatland fires regularly occur during El Ni?o years, and the largest perturbations of radical concentrations in the lower stratosphere are predicted for particularly strong El Ni?o years. By activating the detailed in-cloud OVOC oxidation scheme Jülich Aqueous-phase Mechanism of Organic Chemistry (JAMOC), we find that the predicted changes are dampened. Global models that neglect in-cloud OVOC oxidation tend to overestimate the impact of such extreme pollution events on the atmospheric composition.