scholarly journals Trends in peroxyacetyl nitrate (PAN) in the upper troposphere and lower stratosphere over southern Asia during the summer monsoon season: regional impacts

2014 ◽  
Vol 14 (23) ◽  
pp. 12725-12743 ◽  
Author(s):  
S. Fadnavis ◽  
M. G. Schultz ◽  
K. Semeniuk ◽  
A. S. Mahajan ◽  
L. Pozzoli ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Lower Stratosphere ◽  
Monsoon Season ◽  
Michelson Interferometer ◽  
Temporal Trends ◽  
Nox Emissions ◽  
Summer Monsoon Season ◽  
Peroxyacetyl Nitrate ◽  
Upper Troposphere ◽  
India And China

Abstract. We analyze temporal trends of peroxyacetyl nitrate (PAN) retrievals from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) during 2002–2011 in the altitude range 8–23 km over the Asian summer monsoon (ASM) region. The greatest enhancements of PAN mixing ratios in the upper troposphere and lower stratosphere (UTLS) are seen during the summer monsoon season from June to September. During the monsoon season, the mole fractions of PAN show statistically significant (at 2σ) positive trends from 0.2 ± 0.05 to 4.6 ± 3.1 ppt yr−1 (except between 12 and 14 km) which is higher than the annual mean trends of 0.1 ± 0.05 to 2.7 ± 0.8 ppt yr−1. These rising concentrations point to increasing NOx (= NO + NO2) and volatile organic compound (VOC) emissions from developing nations in Asia, notably India and China. We analyze the influence of monsoon convection on the distribution of PAN in UTLS with simulations using the global chemistry–climate model ECHAM5-HAMMOZ. During the monsoon, transport into the UTLS over the Asian region primarily occurs from two convective zones, one the South China Sea and the other over the southern flank of the Himalayas. India and China host NOx-limited regimes for ozone photochemical production, and thus we use the model to evaluate the contributions from enhanced NOx emissions to the changes in PAN, HNO3 and O3 concentrations in the UTLS. From a set of sensitivity experiments with emission changes in particular regions, it can be concluded that Chinese emissions have a greater impact on the concentrations of these species than Indian emissions. According to SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY) NO2 retrievals NOx emissions increases over India have been about half of those over China between 2002 and 2011.

scholarly journals Trends in Peroxyacetyl Nitrate (PAN) in the upper troposphere and lower stratosphere over Southern Asia during the summer monsoon season: regional impacts

2014 ◽  
Vol 14 (13) ◽  
pp. 19055-19094 ◽  
Author(s):  
S. Fadnavis ◽  
M. G. Schultz ◽  
K. Semeniuk ◽  
A. S. Mahajan ◽  
L. Pozzoli ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Lower Stratosphere ◽  
Monsoon Season ◽  
Michelson Interferometer ◽  
Temporal Trends ◽  
Nox Emissions ◽  
Summer Monsoon Season ◽  
Peroxyacetyl Nitrate ◽  
Upper Troposphere ◽  
India And China

Abstract. We analyze temporal trends of Peroxyacetyl Nitrate (PAN) retrievals from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) during 2002–2011 in the altitude range 8–23 km over the Asian summer monsoon (ASM) region. The greatest enhancements of PAN mixing ratios in the upper troposphere and lower stratosphere (UTLS) are seen during the summer monsoon season from June to September. During the monsoon season, the mole fractions of PAN show statistically significant (at 2 sigma level) positive trends from 0.2 ± 0.05 to 4.6 ± 3.1 ppt year−1 (except between 12–14 km) which is higher than the annual mean trends of 0.1 ± 0.05 to 2.7 ± 0.8 ppt year−1. These rising concentrations point to increasing NOx (=NO+NO2) and volatile organic compound (VOC) emissions from developing nations in Asia, notably India and China. We analyze the influence of monsoon convection on the distribution of PAN in UTLS with simulations using the global chemistry-climate model ECHAM5-HAMMOZ. During the monsoon, transport into the UTLS over the Asian region primarily occurs from two convective zones, one extending from the Bay of Bengal to the South China Sea and the other over the southern flank of the Himalayas. India and China are NOx limited regions, and thus we use the model to evaluate the contributions from enhanced NOx emissions to the changes in PAN, HNO3 and O3 concentrations in the UTLS. From a set of sensitivity experiments with emission changes in particular regions it can be concluded that Chinese emissions have a greater impact on the concentrations of these species than Indian emissions. NOx emissions increases over India are about half of those over China.

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

2015 ◽  
Vol 15 (20) ◽  
pp. 11477-11499 ◽  
Author(s):  
S. Fadnavis ◽  
K. Semeniuk ◽  
M. G. Schultz ◽  
M. Kiefer ◽  
A. Mahajan ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Lower Stratosphere ◽  
Asian Summer Monsoon ◽  
Monsoon Season ◽  
Peroxyacetyl Nitrate ◽  
Transport Pathways ◽  
Upper Troposphere ◽  
Asian Summer ◽  
Emission Change ◽  
Transport Patterns

Abstract. 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.

scholarly journals Weakening Trend of the Tropical Easterly Jet Stream of the Boreal Summer Monsoon Season 1950–2009

2013 ◽  
Vol 26 (23) ◽  
pp. 9408-9414 ◽  
Author(s):  
B. Abish ◽  
P. V. Joseph ◽  
Ola M. Johannessen
Keyword(s):  
Indian Ocean ◽  
Summer Monsoon ◽  
Monsoon Season ◽  
Equatorial Indian Ocean ◽  
Boreal Summer ◽  
Jet Stream ◽  
Moist Convection ◽  
Summer Monsoon Season ◽  
Upper Troposphere ◽  
Tropical Easterly Jet

Recent research has reported that the tropical easterly jet stream (TEJ) of the boreal summer monsoon season is weakening. The analysis herein using 60 yr (1950–2009) of data reveals that this weakening of the TEJ is due to the decreasing trend in the upper tropospheric meridional temperature gradient over the area covered by the TEJ. During this period, the upper troposphere over the equatorial Indian Ocean has warmed due to enhanced deep moist convection associated with the rapid warming of the equatorial Indian Ocean. At the same time, a cooling of the upper troposphere has taken place over the Northern Hemisphere subtropics including the Tibetan anticyclone. The simultaneous cooling of the subtropics and the equatorial heating has caused a decrease in the upper tropospheric meridional thermal gradient. The consequent reduction in the strength of the easterly thermal wind has resulted in the weakening of the TEJ.

scholarly journals Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere – lower stratosphere

2016 ◽  
Author(s):  
R. J. Pope ◽  
N. A. D. Richards ◽  
M. P. Chipperfield ◽  
D. P. Moore ◽  
S. A. Monks ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Regional Distribution ◽  
Michelson Interferometer ◽  
Lower Atmosphere ◽  
Chemical Transport Model ◽  
Peroxyacetyl Nitrate ◽  
Subsequent Formation ◽  
Upper Troposphere

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere – lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board ENVISAT from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS), insitu aircraft data and the TOMCAT 3-D chemical transport model. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to > 200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT-MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results show that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.

scholarly journals Influences of the Indian Summer Monsoon on Water Vapor and Ozone Concentrations in the UTLS as Simulated by Chemistry–Climate Models

2010 ◽  
Vol 23 (13) ◽  
pp. 3525-3544 ◽  
Author(s):  
Markus Kunze ◽  
Peter Braesicke ◽  
Ulrike Langematz ◽  
Gabriele Stiller ◽  
Slimane Bekki ◽  
...  
Keyword(s):  
Water Vapor ◽  
Summer Monsoon ◽  
Indian Summer Monsoon ◽  
Large Scale ◽  
Climate Models ◽  
Lower Stratosphere ◽  
Activity Index ◽  
Michelson Interferometer ◽  
Upper Troposphere ◽  
Atmospheric Sounding

Abstract The representation of the Indian summer monsoon (ISM) circulation in some current chemistry–climate models (CCMs) is assessed. The main assessment focuses on the anticyclone that forms in the upper troposphere and lower stratosphere and the related changes in water vapor and ozone during July and August for the recent past. The synoptic structures are described and CCMs and reanalysis models are compared. Multiannual means and weak versus strong monsoon cases as classified by the Monsoon–Hadley index (MHI) are discussed. The authors find that current CCMs capture the average synoptic structure of the ISM anticyclone well as compared to the 40-yr ECMWF Re-Analysis (ERA-40) and NCEP–NCAR reanalyses. The associated impact on water vapor and ozone in the upper troposphere and lower stratosphere as observed with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat is captured by most models to some degree. The similarities for the strong versus weak monsoon cases are limited, and even for present-day conditions the models do not agree well for extreme events. Nevertheless, some features are present in the reanalyses and more than one CCM, for example, ozone increases at 380 K eastward of the ISM. With the database available for this study, future changes of the ISM are hard to assess. The modeled monsoon activity index used here shows slight weakening of the ISM circulation in a future climate, and some of the modeled water vapor increase seems to be contained in the anticyclone at 360 K and sometimes above. The authors conclude that current CCMs capture the average large-scale synoptic structure of the ISM well during July and August, but large differences for the interannual variability make assessments of likely future changes of the ISM highly uncertain.

scholarly journals Intercomparison and evaluation of satellite peroxyacetyl nitrate observations in the upper troposphere–lower stratosphere

2016 ◽  
Vol 16 (21) ◽  
pp. 13541-13559 ◽  
Author(s):  
Richard J. Pope ◽  
Nigel A. D. Richards ◽  
Martyn P. Chipperfield ◽  
David P. Moore ◽  
Sarah A. Monks ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Regional Distribution ◽  
Michelson Interferometer ◽  
Lower Atmosphere ◽  
Chemical Transport Model ◽  
Peroxyacetyl Nitrate ◽  
Subsequent Formation ◽  
Upper Troposphere

Abstract. Peroxyacetyl nitrate (PAN) is an important chemical species in the troposphere as it aids the long-range transport of NOx and subsequent formation of O3 in relatively clean remote regions. Over the past few decades observations from aircraft campaigns and surface sites have been used to better understand the regional distribution of PAN. However, recent measurements made by satellites allow for a global assessment of PAN in the upper troposphere–lower stratosphere (UTLS). In this study, we investigate global PAN distributions from two independent retrieval methodologies, based on measurements from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument, on board Envisat from the Institute of Meteorology and Climate Research (IMK), Karlsruhe Institute of Technology, and the Department of Physics and Astronomy, University of Leicester (UoL). Retrieving PAN from MIPAS is challenging due to the weak signal in the measurements and contamination from other species. Therefore, we compare the two MIPAS datasets with observations from the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS), in situ aircraft data and the 3-D chemical transport model TOMCAT. MIPAS shows peak UTLS PAN concentrations over the biomass burning regions (e.g. ranging from 150 to  >  200 pptv at 150 hPa) and during the summertime Asian monsoon as enhanced convection aids the vertical transport of PAN from the lower atmosphere. At 150 hPa, we find significant differences between the two MIPAS datasets in the tropics, where IMK PAN concentrations are larger by 50–100 pptv. Comparisons between MIPAS and ACE-FTS show better agreement with the UoL MIPAS PAN concentrations at 200 hPa, but with mixed results above this altitude. TOMCAT generally captures the magnitude and structure of climatological aircraft PAN profiles within the observational variability allowing it to be used to investigate the MIPAS PAN differences. TOMCAT–MIPAS comparisons show that the model is both positively (UoL) and negatively (IMK) biased against the satellite products. These results indicate that satellite PAN observations are able to detect realistic spatial variations in PAN in the UTLS, but further work is needed to resolve differences in existing retrievals to allow quantitative use of the products.

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

2014 ◽  
Vol 14 (14) ◽  
pp. 20159-20195 ◽  
Author(s):  
S. Fadnavis ◽  
K. Semeniuk ◽  
M. G. Schultz ◽  
A. Mahajan ◽  
L. Pozzoli ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
North American ◽  
Lower Stratosphere ◽  
Asian Summer Monsoon ◽  
Monsoon Season ◽  
Convective Transport ◽  
Pollution Transport ◽  
Transport Pathways ◽  
Upper Troposphere ◽  
Asian Summer

Abstract. 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 reservoir species PAN, NOx, and HNO3 from various monsoon regions, to the UTLS over Southern Asia and vice versa. The model is evaluated with trace gas retrievals from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS-E) and aircraft campaigns during the monsoon season (June–September). There are three regions which contribute substantial pollution to the UTLS during the monsoon: the Asian summer monsoon (ASM), the North American Monsoon (NAM) and the West African monsoon (WAM). However, penetration due to ASM convection is deeper into the UTLS as compared to NAM and WAM outflow. The circulation in these monsoon regions distributes PAN into the tropical latitude belt in the upper troposphere. Remote transport also occurs in the extratropical upper troposphere where westerly winds drive North American and European pollutants eastward to partly merge with the ASM plume. Strong ASM convection transports these remote and regional pollutants into the lower stratosphere. In the lower stratosphere the injected pollutants are transported westward by easterly winds. The intense convective activity in the monsoon regions is associated with lightning generation and thereby the emission of NOy species. This will affect the distribution of PAN in the UTLS. The estimates of lightning produced PAN, HNO3, NOx and ozone obtained from control and lightning-off simulations shows high percentage changes over the regions of convective transport especially equatorial Africa and America and comparatively less over the ASM. This indicates higher anthropogenic pollution transport from the ASM region into the UTLS.

scholarly journals Influence of enhanced Asian NO<sub>x</sub> emissions on ozone in the Upper Troposphere and Lower Stratosphere (UTLS) in chemistry climate model simulations

2016 ◽  
Author(s):  
Chaitri Roy ◽  
Suvarna Fadnavis ◽  
Rolf Müller ◽  
Ayantika Dey Chaudhary ◽  
Felix Ploeger
Keyword(s):  
Lower Stratosphere ◽  
Climate Model ◽  
Hadley Circulation ◽  
Convective Transport ◽  
Vertical Transport ◽  
Nox Emission ◽  
The Tibetan Plateau ◽  
Nox Emissions ◽  
Upper Troposphere ◽  
India And China

Abstract. Asian summer monsoon convection plays an important role in efficient vertical transport from the surface to the anticyclone. In this paper we investigate the potential impact of convectively transported anthropogenic nitrogen oxides (NOx) on the distribution of ozone in the Upper Troposphere and Lower Stratosphere (UTLS) from simulations with the fully-coupled aerosol chemistry climate model, ECHAM5-HAMMOZ. We performed anthropogenic NOx emission sensitivity experiments over India and China. In these simulations, anthropogenic NOx emissions for the period 2000–2010 have been increased by 38 % over India and by 73 % over China in accordance with satellite observed trends over India of 3.8 % per year and China of 7.3 % per year. These NOx emission sensitivity simulations show that strong convection over the Bay of Bengal and the Southern slopes of the Himalayas transports Indian emissions into the UTLS. Convective transport from the South China Sea injects Chinese emissions into the lower stratosphere. Indian and Chinese emissions are partially transported over the Arabian Sea and west Asia by the tropical easterly jet. Enhanced NOx emissions over India and China increase the ozone radiative forcing over India by 0.112 W/m2 and 0.121 W/m2 respectively. These elevated emissions produces significant warming over the Tibetan Plateau and increase precipitation over India due to a strengthening of the monsoon Hadley circulation. However doubling of NOx emissions over India (73 %); equal to China, produced high ozone in the lower troposphere. It induced a reverse monsoon Hadley circulation and negative precipitation anomalies over India. The associated subsidence suppressed vertical transport of NOx and ozone into the anticyclone.

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

2015 ◽  
Vol 15 (11) ◽  
pp. 15087-15135 ◽  
Author(s):  
S. Fadnavis ◽  
K. Semeniuk ◽  
M. G. Schultz ◽  
M. Kiefer ◽  
A. Mahajan ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
North American ◽  
Lower Stratosphere ◽  
Asian Summer Monsoon ◽  
Monsoon Season ◽  
Convective Transport ◽  
Transport Pathways ◽  
Upper Troposphere ◽  
Asian Summer ◽  
Transport Patterns

Abstract. 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 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 as compared to NAM and WAM outflow. The circulation in all three monsoon regions distributes PAN into the tropical latitude belt in the upper troposphere. Remote transport also occurs in the extratropical upper troposphere where westerly winds drive North American and European pollutants eastward where they can become part of the ASM convection and be lifted into the lower stratosphere. In the lower stratosphere the injected pollutants are transported westward by easterly winds. 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. According to sensitivity simulations with and without lightning, increase in concentrations of PAN (~ 40%), HNO3 (75%), NOx (70%) and ozone (30%) over the regions of convective transport, especially over equatorial Africa and America and comparatively less over the ASM. This indicates that PAN in the UTLS over the ASM region is primarily of anthropogenic origin.

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