Biomass burning emissions disturbances on the isoprene oxidation in a tropical forest

We present a characterization of the chemical composition of the atmosphere of the Brazilian Amazon rainforest based on trace gases measurements carried out during the South American Biomass Burning Analysis (SAMBBA) airborne experiment in September 2012. We analyzed the observations of primary biomass burning emission tracers, i.e., carbon monoxide (CO) and nitrogen oxides (NOx), ozone (O3), isoprene, and its main oxidation products, methyl vinyl ketone (MVK), methacrolein (MACR), and hydroxyhydroperoxides (ISOPOOH). The focus of SAMBBA was primarily on biomass burning emissions, but there were also several flights in areas of the Amazon forest not directly affected by biomass burning, revealing a background with a signature of biomass burning in the chemical composition due to long-range transport of biomass burning tracers from both Africa and the eastern part of Amazonia. We used the [MVK + MACR + ISOPOOH] / [Isoprene] ratio and the hydroxyl radical (OH) indirect calculation to assess the oxidative capacity of the Amazon forest atmosphere. We compared the background regions (CO

Impact of different Asian source regions on the composition of the Asian monsoon anticyclone and of the extratropical lowermost stratosphere

The impact of different boundary layer source regions in Asia on the chemical composition of the Asian monsoon anticyclone, considering its intraseasonal variability in 2012, is analysed by simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS) using artificial emission tracers. The horizontal distribution of simulated CO, O3, and artificial emission tracers for India/China are in good agreement with patterns found in satellite measurements of O3 and CO by the Aura Microwave Limb Sounder (MLS). Using in addition, correlations of artificial emission tracers with potential vorticity demonstrates that the emission tracer for India/China is a very good proxy for spatial distribution of trace gases within the Asian monsoon anticyclone. The Asian monsoon anticyclone constitutes a horizontal transport barrier for emission tracers and is highly variable in location and shape. From the end of June to early August, a northward movement of the anticyclone and, during September, a strong broadening of the spatial distribution of the emission tracer for India/China towards the tropics are found. In addition to the change of the location of the anticyclone, the contribution of different boundary source regions to the composition of the Asian monsoon anticyclone in the upper troposphere strongly depends on its intraseasonal variability and is therefore more complex than hitherto believed. The largest contributions to the composition of the air mass in the anticyclone are found from northern India and Southeast Asia at a potential temperature of 380 K. In the early (mid-June to mid-July) and late (September) period of the 2012 monsoon season, contributions of emissions from Southeast Asia are highest; in the intervening period (early August), emissions from northern India have the largest impact. Our findings show that the temporal variation of the contribution of different convective regions is imprinted in the chemical composition of the Asian monsoon anticyclone. Air masses originating in Southeast Asia are found both within and outside of the Asian monsoon anticyclone because these air masses experience, in addition to transport within the anticyclone, upward transport at the southeastern flank of the anticyclone and in the tropics. Subsequently, isentropic poleward transport of these air masses occurs at around 380 K with the result that the extratropical lowermost stratosphere in the Northern Hemisphere is flooded by the end of September with air masses originating in Southeast Asia. Even after the breakup of the anticyclonic circulation (around the end of September), significant contributions of air masses originating in India/China are still found in the upper troposphere over Asia. Our results demonstrate that emissions from India, China, and Southeast Asia have a significant impact on the chemical composition of the lowermost stratosphere of the Northern Hemisphere, in particular at the end of the monsoon season in September/October 2012.

Impact of different Asian source regions on the composition of the Asian monsoon anticyclone and on the extratropical lowermost stratosphere

The impact of different boundary layer source regions in Asia on the chemical composition of the Asian monsoon anticyclone, considering its intraseasonal variability in 2012, is analysed by CLaMS simulations using artificial emission tracers. Our simulations show that the Asian monsoon anticyclone is highly variable in location and shape and oscillates between 2 states: first a symmetric anticyclone and second, an asymmetric anticyclone either elongated or split in two smaller anticyclones. A maximum in the distribution of air originating from Indian/Chinese boundary layer sources is usually found in the core of the symmetric anticyclone, in contrast the asymmetric state is characterised by a double peak structure in the horizontal distribution of air originating from India and China. The simulated horizontal distribution of artificial emission tracers for India/China is in agreement with patterns found in satellite measurements of O3 and CO by the Aura Microwave Limb Sounder (MLS). The contribution of different boundary source regions to the Asian monsoon anticyclone strongly depends on its intraseasonal variability and is therefore more complex than hitherto believed, but in general the highest contributions are from North India and Southeast Asia at 380 K. In the early (June to mid-July) and late (mid-August to October) period of the monsoon 2012, contributions of emissions from Southeast Asia are highest and in the intervening period (≈ mid-July to mid-August) emissions from North India have the largest impact. Further, our simulations confirm that the thermal tropopause above the anticyclone constitutes a vertical transport barrier. Enhanced contributions of emission tracers for Asia are found at the northern flank of the Asian monsoon anticyclone between double tropopauses indicating an isentropic transport from the anticyclone into the lowermost stratosphere. After the breakup of the anticyclone, significant contributions of air masses originating in India/China are sill found over Asia in September/October. In addition, these air masses spread out within the mid-latitudes of the Northern Hemisphere and in the tropics at around 380 K. Moreover, air masses from Southeast Asia experienced diabatic upward transport in the tropics and subsequently isentropic poleward transport occurs at around 380 K with the result that the extratropical lowermost stratosphere is flooded by end of September with air masses originating in Southeast Asia. Our results demonstrate that emissions from Asia have a significant impact on the chemical compositions of the lowermost stratosphere of the Northern Hemisphere in particular after the end of the monsoon season in September/October 2012.