Transport pathways of peroxyacetyl nitrate in the upper troposphere and lower stratosphere from different monsoon systems during the summer monsoon season

The Asian summer monsoon involves complex transport patterns with large-scale redistribution of trace gases in the upper troposphere and lower stratosphere (UTLS). We employ the global chemistry–climate model ECHAM5–HAMMOZ in order to evaluate the transport pathways and the contributions of nitrogen...

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Published in:Atmospheric chemistry and physics Vol. 15; no. 20; pp. 11477 - 11499
Main Authors: Fadnavis, S., Semeniuk, K., Schultz, M. G., Kiefer, M., Mahajan, A., Pozzoli, L., Sonbawane, S.
Format: Journal Article
Language:English
Published: Katlenburg-Lindau Copernicus GmbH 19.10.2015
Copernicus Publications
Subjects:
African monsoon
Aircraft
Anthropogenic factors
Atmospheric chemistry
Atmospheric sounding
Belt conveyors
Climate models
Comparative analysis
Computer simulation
Convection
Convective activity
Convective transport
Decomposition
Easterlies
Emissions
Equatorial regions
Gases
Latitude
Lightning
Lower stratosphere
Michelson interferometers
Middle atmosphere
Mixing ratio
Monsoon circulation
Monsoons
Nitrogen compounds
Nitrogen oxides
North American monsoon
Organic compounds
Outflow
Ozone
Peroxyacetyl nitrate
Photochemicals
Pollutants
Pollution
Regions
Remote sensing
Seasons
Simulation
Stratosphere
Studies
Summer
Summer monsoon
Trace gases
Transport
Tropical climate
Troposphere
Upper troposphere
VOCs
Volatile organic compounds
Wind
Winds
Asia
Africa
Northern Hemisphere
West Africa
ISSN:1680-7324, 1680-7316, 1680-7324
Online Access:Get full text
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Summary:The Asian summer monsoon involves complex transport patterns with large-scale redistribution of trace gases in the upper troposphere and lower stratosphere (UTLS). We employ the global chemistry–climate model ECHAM5–HAMMOZ in order to evaluate the transport pathways and the contributions of nitrogen oxide species peroxyacetyl nitrate (PAN), NOx and HNO3 from various monsoon regions, to the UTLS over southern Asia and vice versa. Simulated long-term seasonal mean mixing ratios are compared with trace gas retrievals from the Michelson Interferometer for Passive Atmospheric Sounding aboard ENVISAT(MIPAS-E) and aircraft campaigns during the monsoon season (June–September) in order to evaluate the model's ability to reproduce these transport patterns. The model simulations show that there are three regions which contribute substantial pollution to the South Asian UTLS: the Asian summer monsoon (ASM), the North American monsoon (NAM) and the West African monsoon (WAM). However, penetration due to ASM convection reaches deeper into the UTLS compared to NAM and WAM outflow. The circulation in all three monsoon regions distributes PAN into the tropical latitude belt in the upper troposphere (UT). Remote transport also occurs in the extratropical UT where westerly winds drive North American and European pollutants eastward where they can become part of the ASM convection and lifted into the lower stratosphere. In the lower stratosphere the injected pollutants are transported westward by easterly winds. Sensitivity experiments with ECHAM5–HAMMOZ for simultaneous NOx and non-methane volatile organic compounds (NMVOCs) emission change (−10 %) over ASM, NAM and WAM confirm similar transport. Our analysis shows that a 10 % change in Asian emissions transports ~ 5–30 ppt of PAN in the UTLS over Asia, ~ 1–10 ppt of PAN in the UTLS of northern subtropics and mid-latitudes, ~ 7–10 ppt of HNO3 and ~ 1–2 ppb of ozone in UT over Asia. Comparison of emission change over Asia, North America and Africa shows that the highest transport of HNO3 and ozone occurs in the UT over Asia and least over Africa. The intense convective activity in the monsoon regions is associated with lightning and thereby the formation of additional NOx. This also affects the distribution of PAN in the UTLS. Simulations with and without lightning show an increase in the concentrations of PAN (~ 40 %), HNO3 (75 %), NOx (70 %) and ozone (30 %) over the regions of convective transport. Lightning-induced production of these species is higher over equatorial Africa and America compared to the ASM region. This indicates that the contribution of anthropogenic emissions to PAN in the UTLS over the ASM is higher than that of lightning.
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ISSN:1680-7324
1680-7316
1680-7324
DOI:10.5194/acp-15-11477-2015