Upper-tropospheric CO and O 3 budget during the Asian summer monsoon

Abstract. During the Asian summer monsoon, the circulation in the upper troposphere/lower stratosphere (UTLS) is dominated by the Asian monsoon anticyclone (AMA). Pollutants convectively uplifted to the upper troposphere are trapped within this anticyclonic circulation that extends from the Pacific Ocean to the Eastern Mediterranean basin. Among the uplifted pollutants are ozone (O3) and its precursors, such as carbon monoxide (CO) and nitrogen oxides (NOx). Many studies based on global modeling and satellite data have documented the source regions and transport pathways of primary pollutants (CO, HCN) into the AMA. Here, we aim to quantify the O3 budget by taking into consideration anthropogenic and natural sources. We first use CO and O3 data from the MetOp-A/IASI sensor to document their tropospheric distributions over Asia, taking advantage of the useful information they provide on the vertical dimension. These satellite data are used together with MOZAIC tropospheric profiles recorded in India to validate the distributions simulated by the global GEOS-Chem chemistry transport model. Over the Asian region, UTLS monthly CO and O3 distributions from IASI and GEOS-Chem display the same large-scale features. UTLS CO columns from GEOS-Chem are in agreement with IASI, with a low bias of 11 ± 9 % and a correlation coefficient of 0.70. For O3, the model underestimates IASI UTLS columns over Asia by 14 ± 26 % but the correlation between both is high (0.94). GEOS-Chem is further used to quantify the CO and O3 budget through sensitivity simulations. For CO, these simulations confirm that South Asian anthropogenic emissions have a more important impact on enhanced concentrations within the AMA (∼  25 ppbv) than East Asian emissions (∼  10 ppbv). The correlation between enhanced emissions over the Indo-Gangetic Plain and monsoon deep convection is responsible for this larger impact. Consistently, South Asian anthropogenic NOx emissions also play a larger role in producing O3 within the AMA (∼  8 ppbv) than East Asian emissions (∼  5 ppbv), but Asian lightning-produced NOx is responsible for the largest O3 production (10–14 ppbv). Stratosphere-to-troposphere exchanges are also important in transporting O3 in the upper part of the AMA.

[1]  J. Ungermann,et al.  A potential vorticity-based determination of the transport barrier in the Asian summer monsoon anticyclone , 2015 .

[2]  J. Pyle,et al.  Impact of West African Monsoon convective transport and lightning NO x production upon the upper tropospheric composition: a multi-model study , 2010 .

[3]  C. Clerbaux,et al.  Validation of three different scientific ozone products retrieved from IASI spectra using ozonesondes , 2011 .

[4]  Johannes Orphal,et al.  Tropospheric ozone distributions over Europe during the heat wave in July 2007 observed from infrared nadir spectra recorded by IASI , 2008 .

[5]  William J. Koshak,et al.  Optimized regional and interannual variability of lightning in a global chemical transport model constrained by LIS/OTD satellite data , 2012 .

[6]  D. Jacob,et al.  Why are there large differences between models in global budgets of tropospheric ozone , 2007 .

[7]  J. Burrows,et al.  Analysis of tropospheric NOx over Asia using the model of atmospheric transport and chemistry (MATCH-MPIC) and GOME-satellite observations , 2004 .

[8]  P. V. Velthoven,et al.  Updated African biomass burning emission inventories in the framework of the AMMA-IDAF program, with an evaluation of combustion aerosols , 2010 .

[9]  W. Randel,et al.  Deep convective influence on the Asian summer monsoon anticyclone and associated tracer variability observed with Atmospheric Infrared Sounder (AIRS) , 2006 .

[10]  Tropospheric ozone variations at the Nepal Climate Observatory-Pyramid (Himalayas, 5079 m a.s.l.) and influence of deep stratospheric intrusion events , 2010 .

[11]  J. Attie,et al.  Transport pathways of CO in the African upper troposphere during the monsoon season: a study based upon the assimilation of spaceborne observations , 2008 .

[12]  J. Seinfeld,et al.  Future climate impacts of direct radiative forcing of anthropogenic aerosols, tropospheric ozone, and long‐lived greenhouse gases , 2007 .

[13]  D. Jacob,et al.  Background ozone over the United States in summer: Origin, trend, and contribution to pollution episodes , 2002 .

[14]  D. Stevenson,et al.  Influence of convective transport on tropospheric ozone and its precursors in a chemistry-climate model , 2005 .

[15]  Mijeong Park,et al.  Transport pathways of carbon monoxide in the Asian summer monsoon diagnosed from Model of Ozone and Related Tracers (MOZART) , 2009 .

[16]  Cathy Clerbaux,et al.  Global carbon monoxide vertical distributions from spaceborne high-resolution FTIR nadir measurements , 2005 .

[17]  J. Bian,et al.  Tracing the boundary layer sources of carbon monoxide in the Asian summer monsoon anticyclone using WRF-Chem , 2015, Advances in Atmospheric Sciences.

[18]  Valerie Thouret,et al.  Comparisons of ozone measurements from the MOZAIC airborne program and the ozone sounding network at eight locations , 1998 .

[19]  P. Bernath,et al.  Chemical Isolation in the Asian monsoon anticyclone observed in Atmospheric Chemistry Experiment (ACE-FTS) data , 2007 .

[20]  M. George,et al.  Retrieval of MetOp-A/IASI CO profiles and validation with MOZAIC data , 2012 .

[21]  M. Rodwell,et al.  A Model of the Asian Summer Monsoon. Part I: The Global Scale , 1995 .

[22]  Bryan N. Duncan,et al.  A tropospheric ozone maximum over the Middle East , 2001 .

[23]  Philip J. Rasch,et al.  The balance of effects of deep convective mixing on tropospheric ozone , 2003 .

[24]  D. Jacob,et al.  Origin of ozone and NOx in the tropical troposphere: A photochemical analysis of aircraft observations over the South Atlantic basin , 1996 .

[25]  Clive D Rodgers,et al.  Inverse Methods for Atmospheric Sounding: Theory and Practice , 2000 .

[26]  R. A. Plumb,et al.  Eddy Shedding from the Upper-Tropospheric Asian Monsoon Anticyclone , 2001 .

[27]  Analysis of tropospheric ozone and carbon monoxide profiles over South America based on MOZAIC/IAGOS database and model simulations , 2015 .

[28]  S. Moorthi,et al.  Relaxed Arakawa-Schubert - A parameterization of moist convection for general circulation models , 1992 .

[29]  Richard G. Derwent,et al.  Multimodel simulations of carbon monoxide: Comparison with observations and projected near‐future changes , 2006 .

[30]  Paul Ginoux,et al.  Interpretation of TOMS observations of tropical tropospheric ozone with a global model and in-situ observations , 2002 .

[31]  Dylan B. A. Jones,et al.  Analysis of tropical tropospheric ozone, carbon monoxide, and water vapor during the 2006 El Niño using TES observations and the GEOS‐Chem model , 2009 .

[32]  J. Randerson,et al.  Global fire emissions and the contribution of deforestation, savanna, forest, agricultural, and peat fires (1997-2009) , 2010 .

[33]  D. Jacob,et al.  Asian chemical outflow to the Pacific in spring: Origins, pathways, and budgets , 2001 .

[34]  David G Streets,et al.  Modeling study of air pollution due to the manufacture of export goods in China's Pearl River Delta. , 2006, Environmental science & technology.

[35]  J. Burrows,et al.  Regional NOx emission strength for the Indian subcontinent and the impact of emissions from India and neighboring countries on regional O3 chemistry , 2006 .

[36]  R. Martin,et al.  Space‐based constraints on the production of nitric oxide by lightning , 2007 .

[37]  Merritt N. Deeter,et al.  Evidence of vertical transport of carbon monoxide from Measurements of Pollution in the Troposphere (MOPITT) , 2004 .

[38]  John A. Pyle,et al.  Measurement of ozone and water vapor by Airbus in-service aircraft: The MOZAIC airborne program, an overview , 1998 .

[39]  Guoxiong Wu,et al.  The Bimodality of the 100 hPa South Asia High and its Relationship to the Climate Anomaly over East Asia in Summer , 2002 .

[40]  M. Riese,et al.  Impact of different Asian source regions on the composition of the Asian monsoon anticyclone and of the extratropical lowermost stratosphere , 2015 .

[41]  L. Pan,et al.  Boundary layer sources for the Asian anticyclone: Regional contributions to a vertical conduit , 2013 .

[42]  W. Randel,et al.  Dynamic variability of the Asian monsoon anticyclone observed in potential vorticity and correlations with tracer distributions , 2013 .

[43]  Jean-Pierre Cammas,et al.  c ○ European Geosciences Union 2003 Atmospheric Chemistry and Physics Discussions , 2003 .

[44]  C. Mari,et al.  An upper tropospheric ‘ozone river’ from Africa to India during the 2008 Asian post-monsoon season , 2015 .

[45]  H. Worden,et al.  Carbon monoxide distributions from the IASI/METOP mission: evaluation with other space-borne remote sensors , 2009 .

[46]  Xiong Liu,et al.  Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone , 2006 .

[47]  Ulrich Schumann,et al.  The global lightning-induced nitrogen oxides source , 2007 .

[48]  Dylan B. A. Jones,et al.  Analysis of the summertime buildup of tropospheric ozone abundances over the Middle East and North Africa as observed by the Tropospheric Emission Spectrometer instrument , 2009 .

[49]  M. Schwartz,et al.  Transport analysis and source attribution of seasonal and interannual variability of CO in the tropical upper troposphere and lower stratosphere , 2012 .

[50]  Lieven Clarisse,et al.  Monitoring of atmospheric composition using the thermal infrared IASI/METOP sounder , 2009 .

[51]  H. Fuelberg,et al.  Using a WRF simulation to examine regions where convection impacts the Asian summer monsoon anticyclone , 2013 .

[52]  M. Matricardi,et al.  The detection of post-monsoon tropospheric ozone variability over south Asia using IASI data , 2011 .

[53]  Bin Wang,et al.  Convective outflow of South Asian pollution: A global CTM simulation compared with EOS MLS observations , 2005 .

[54]  V. Thouret,et al.  Tropospheric ozone over Equatorial Africa: regional aspects from the MOZAIC data , 2004 .

[55]  B. Hannegan,et al.  Stratospheric ozone in 3-D models : A simple chemistry and the cross-tropopause flux , 2000 .

[56]  D. Weisenstein,et al.  Development and evaluation of the unified tropospheric–stratospheric chemistry extension (UCX) for the global chemistry-transport model GEOS-Chem , 2014 .

[57]  Dylan B. A. Jones,et al.  Analysis of CO in the tropical troposphere using Aura satellite data and the GEOS-Chem model: insights into transport characteristics of the GEOS meteorological products , 2010 .

[58]  S. Massie,et al.  Transport above the Asian summer monsoon anticyclone inferred from Aura Microwave Limb Sounder tracers , 2007 .

[59]  R. Martin,et al.  Quantification of the factors controlling tropical tropospheric ozone and the South Atlantic maximum , 2007 .

[60]  Louisa Emmons,et al.  Asian Monsoon Transport of Pollution to the Stratosphere , 2010, Science.

[61]  D. Rind,et al.  Modeling Global Lightning Distributions in a General Circulation Model , 1994 .