scholarly journals First detection of ammonia (NH<sub>3</sub>) in the Asian summer monsoon upper troposphere

2016 ◽  
Vol 16 (22) ◽  
pp. 14357-14369 ◽  
Author(s):  
Michael Höpfner ◽  
Rainer Volkamer ◽  
Udo Grabowski ◽  
Michel Grutter ◽  
Johannes Orphal ◽  
...  

Abstract. Ammonia (NH3) has been detected in the upper troposphere by the analysis of averaged MIPAS (Michelson Interferometer for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian summer monsoon at 12–15 km altitude. Three-monthly, 10° longitude  ×  10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved, with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aerosol layer by the formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations.

2011 ◽  
Vol 11 (2) ◽  
pp. 503-518 ◽  
Author(s):  
A. K. Baker ◽  
T. J. Schuck ◽  
F. Slemr ◽  
P. van Velthoven ◽  
A. Zahn ◽  
...  

Abstract. Between April and December 2008 the CARIBIC commercial aircraft conducted monthly measurement flights between Frankfurt, Germany and Chennai, India. These flights covered the period of the Asian summer monsoon (June–September), during which enhancements in a number of atmospheric species were observed in the upper troposphere over southwestern Asia. In addition to in situ measurements of trace gases and aerosols, whole air samples were collected during the flights, and these were subsequently analyzed for a suite of trace gases that included a number of C2–C8 non-methane hydrocarbons. Non-methane hydrocarbons are relatively short-lived compounds and the large enhancements in their mixing ratios in the upper troposphere over southwestern Asia during the monsoon, sometimes more than double their spring and fall means, provides qualitative evidence for the influence of convectively uplifted boundary layer air. The particularly large enhancements of the combustion tracers benzene and ethyne, along with the similarity of their ratios with carbon monoxide and emission ratios from the burning of household biofuels, indicate a strong influence of biofuel burning to NMHC emissions in this region. Conversely, the ratios of ethane and propane to carbon monoxide, along with the ratio between i-butane and n-butane, indicate a significant source of these compounds from the use of fossil fuels, and comparison to previous campaigns suggests that this source could be increasing. Photochemical aging patterns of NMHCs showed that the CARIBIC samples were collected in two distinctly different regions of the monsoon circulation: a southern region where air masses had been recently influenced by low level contact and a northern region, where air parcels had spent substantial time in transit in the upper troposphere before being probed. Estimates of age using ratios of individual NMHCs have ranges of 3–6 days in the south and 9–12 days in the north.


2012 ◽  
Vol 12 (11) ◽  
pp. 30081-30117 ◽  
Author(s):  
S. Fadnavis ◽  
K. Semeniuk ◽  
L. Pozzoli ◽  
M. G. Schultz ◽  
S. D. Ghude ◽  
...  

Abstract. An eight member ensemble of ECHAM5-HAMMOZ simulations for the year 2003 is analyzed to study the transport of aerosols in the Upper Troposphere and Lower Stratosphere (UTLS) during the Asian Summer Monsoon (ASM). Simulations show persistent maxima in black carbon, organic carbon, sulfate, and mineral dust aerosols within the anticyclone in the UTLS throughout the ASM (period from July to September) when convective activity over the Indian subcontinent is highest. Model simulations indicate boundary layer aerosol pollution as the source of this UTLS aerosol layer and identify ASM convection as the dominant transport process. Evidence of ASM transport of aerosols into the stratosphere is observed in HALogen Occultation Experiment (HALOE) and Stratospheric Aerosol and Gas Experiment (SAGE) II aerosol extinction. The impact of aerosols in the UTLS region is analyzed by evaluating the differences between simulations with (CTRL) and without aerosol (HAM-off) loading. The transport of anthropogenic aerosols in the UTLS increases cloud ice, water vapour and temperature, indicating that aerosols play an important role in enhancement of cloud ice in the Upper-Troposphere (UT). Aerosol induced circulation changes include a weakening of the main branch of the Hadley circulation and increased vertical transport around the southern flank of the Himalayas and reduction in monsoon precipitation over the India region.


2020 ◽  
Author(s):  
Masatomo Fujiwara ◽  
Tetsu Sakai ◽  
Koichi Shiraishi ◽  
Yoichi Inai ◽  
Sergey Khaykin ◽  
...  

Abstract. Eastward airmass transport from the Asian summer monsoon (ASM) anticyclone in the upper troposphere and lower stratosphere (UTLS) often involves eastward shedding vortices, which can cover most of the Japanese archipelago. We investigated the aerosol characteristics of these vortices by analysing data from two lidar systems in Japan, at Tsukuba (36.1° N, 140.1° E) and Fukuoka (33.55° N, 130.36° E), during the summer of 2018. We observed several events with enhanced particle signals at Tsukuba at 15.5–18 km altitude (at or above the local tropopause) during August–September 2018, with a backscattering ratio of ~1.10 and particle depolarization of ~5 % (i.e., not spherical, but more spherical than ice crystals). These particle characteristics may be consistent with those of solid aerosol particles, such as ammonium nitrate. Each event had a timescale of a few days. During the same study period, we also observed similar enhanced particle signals in the lower stratosphere at Fukuoka. The upper troposphere is often covered by cirrus clouds at both lidar sites. Backward trajectory calculations for these sites for days with enhanced particle signals in the lower stratosphere and days without indicate that the former airmasses originated within the ASM anticyclone, and the latter more from edge regions. Reanalysis carbon-monoxide and satellite water-vapour data indicate that eastward shedding vortices were involved in the observed aerosol enhancements. Satellite aerosol data confirm that the period and latitudinal region were free from the direct influence of documented volcanic eruptions and high latitude forest fires. Our results indicate that the Asian Tropopause Aerosol Layer (ATAL) over the ASM region extends east towards Japan in association with the eastward shedding vortices, and that lidar systems in Japan can detect at least the lower stratospheric portion of the ATAL during periods when the lower stratosphere is undisturbed by volcanic eruptions and forest fires. The upper tropospheric portion of the ATAL is either depleted by tropospheric processes (convection and wet scavenging) during eastward transport or is obscured by much stronger cirrus cloud signals.


2021 ◽  
Vol 21 (4) ◽  
pp. 3073-3090
Author(s):  
Masatomo Fujiwara ◽  
Tetsu Sakai ◽  
Tomohiro Nagai ◽  
Koichi Shiraishi ◽  
Yoichi Inai ◽  
...  

Abstract. Eastward air-mass transport from the Asian summer monsoon (ASM) anticyclone in the upper troposphere and lower stratosphere (UTLS) often involves eastward-shedding vortices, which can cover most of the Japanese archipelago. We investigated the aerosol characteristics of these vortices by analysing data from two lidar systems in Japan, at Tsukuba (36.1∘ N, 140.1∘ E) and Fukuoka (33.55∘ N, 130.36∘ E), during the summer of 2018. We observed several events with enhanced particle signals at Tsukuba at 15.5–18 km of altitude (at or above the local tropopause) during August–September 2018, with a backscattering ratio of ∼ 1.10 and particle depolarization of ∼ 5 % (i.e. not spherical, but more spherical than ice crystals). These particle characteristics may be consistent with those of solid aerosol particles, such as ammonium nitrate. Each event had a timescale of a few days. During the same study period, we also observed similar enhanced particle signals in the lower stratosphere at Fukuoka. The upper troposphere is often covered by cirrus clouds at both lidar sites. Backward trajectory calculations for these sites for days with enhanced particle signals in the lower stratosphere and days without indicate that the former air masses originated within the ASM anticyclone and the latter more from edge regions. Reanalysis carbon monoxide and satellite water vapour data indicate that eastward-shedding vortices were involved in the observed aerosol enhancements. Satellite aerosol data confirm that the period and latitudinal region were free from the direct influence of documented volcanic eruptions and high-latitude forest fires. Our results indicate that the Asian tropopause aerosol layer (ATAL) over the ASM region extends east towards Japan in association with the eastward-shedding vortices and that lidar systems in Japan can detect at least the lower-stratospheric portion of the ATAL during periods when the lower stratosphere is undisturbed by volcanic eruptions and forest fires. The upper-tropospheric portion of the ATAL is either depleted by tropospheric processes (convection and wet scavenging) during eastward transport or is obscured by much stronger cirrus cloud signals.


2017 ◽  
Vol 114 (27) ◽  
pp. 6972-6977 ◽  
Author(s):  
Pengfei Yu ◽  
Karen H. Rosenlof ◽  
Shang Liu ◽  
Hagen Telg ◽  
Troy D. Thornberry ◽  
...  

An enhanced aerosol layer near the tropopause over Asia during the June–September period of the Asian summer monsoon (ASM) was recently identified using satellite observations. Its sources and climate impact are presently not well-characterized. To improve understanding of this phenomenon, we made in situ aerosol measurements during summer 2015 from Kunming, China, then followed with a modeling study to assess the global significance. The in situ measurements revealed a robust enhancement in aerosol concentration that extended up to 2 km above the tropopause. A climate model simulation demonstrates that the abundant anthropogenic aerosol precursor emissions from Asia coupled with rapid vertical transport associated with monsoon convection leads to significant particle formation in the upper troposphere within the ASM anticyclone. These particles subsequently spread throughout the entire Northern Hemispheric (NH) lower stratosphere and contribute significantly (∼15%) to the NH stratospheric column aerosol surface area on an annual basis. This contribution is comparable to that from the sum of small volcanic eruptions in the period between 2000 and 2015. Although the ASM contribution is smaller than that from tropical upwelling (∼35%), we find that this region is about three times as efficient per unit area and time in populating the NH stratosphere with aerosol. With a substantial amount of organic and sulfur emissions in Asia, the ASM anticyclone serves as an efficient smokestack venting aerosols to the upper troposphere and lower stratosphere. As economic growth continues in Asia, the relative importance of Asian emissions to stratospheric aerosol is likely to increase.


2016 ◽  
Author(s):  
Michael Höpfner ◽  
Rainer Volkamer ◽  
Udo Grabowski ◽  
Michel Grutter ◽  
Johannes Orphal ◽  
...  

Abstract. Ammonia (NH3) has been detected in the upper troposphere by analysis of averaged MIPAS (Michelson Interferomter for Passive Atmospheric Sounding) infrared limb-emission spectra. We have found enhanced amounts of NH3 within the region of the Asian monsoon at 12–15 km altitude. Three-monthly, 10° longitude x 10° latitude average profiles reaching maximum mixing ratios of around 30 pptv in this altitude range have been retrieved with a vertical resolution of 3–8 km and estimated errors of about 5 pptv. These observations show that loss processes during transport from the boundary layer to the upper troposphere within the Asian monsoon do not deplete the air entirely of NH3. Thus, ammonia might contribute to the so-called Asian tropopause aersol layer by formation of ammonium aerosol particles. On a global scale, outside the monsoon area and during different seasons, we could not detect enhanced values of NH3 above the actual detection limit of about 3–5 pptv. This upper bound helps to constrain global model simulations.


2021 ◽  
Author(s):  
William K.M. Lau ◽  
Kyu-Myong Kim

&lt;p&gt;Using MERRA2 reanalyses, we have examined the long-term (2000-2019) trends and transport of surface pollutants, CO, BC and OC from surface to the upper troposphere and lower stratosphere (UTLS) during the Asian summer monsoon. &amp;#160;&amp;#160;&amp;#160;We find a strong linear trend indicating an expansion and strengthening of the Asian Monsoon Anticyclone (AMA), in conjunction with increased concentration of CO, BC and OC in the UTLS, including the Aerosol Tropopause Aerosol Layer (ATAL).&amp;#160;&lt;/p&gt;&lt;p&gt;The UTLS trend in CO can be tracked to increased upward transport primarily from surface sources near 25-35&lt;sup&gt;o&lt;/sup&gt;N, in association with the expansion/strengthening of the AMA, and a northward displacement of ascending branch of the monsoon meridional circulation.&amp;#160; In contrast, near 25-35&lt;sup&gt;o&lt;/sup&gt;N, BC and OC trends show significant reduction from surface to mid-troposphere, coupled a weak increase at UTLS (above 250 -100 hPa).&amp;#160; The reduction in surface and tropospheric BC and OC likely reflects reduced emission due to the clean air acts in East Asia.&amp;#160; Additionally, heavier rainfall associated with the enhanced ascent and wet scavenging may also contribute to the strong reduction in tropospheric BC and OC.&amp;#160; The increase in UTLS OC/BC appears to stem from increased and extended biomass burning near surface sources located in extratropical latitudes (70-130&lt;sup&gt;o&lt;/sup&gt; E, 55-70&lt;sup&gt;o&lt;/sup&gt; N).&amp;#160; The OC/BC aerosols are transported upward by vertical mixing over the source regions, and enter the tropical UTLS through horizonal diffusive processes.&amp;#160;&amp;#160; Additionally, enhanced penetrative convection in the anomalous ascent regions during the peak monsoon season may also play a role in further enhancing the monsoon ascent, lifting ambient hydrophobic OC/BC and water vapor in the mid-to-upper troposphere to higher elevations, resulting in enhanced ice-cloud fraction, increased latent and radiative heating in the UTLS/ATAL region.&lt;/p&gt;&lt;p&gt;&amp;#160;&lt;/p&gt;


2010 ◽  
Vol 10 (7) ◽  
pp. 18101-18138 ◽  
Author(s):  
A. K. Baker ◽  
T. J. Schuck ◽  
F. Slemr ◽  
P. van Velthoven ◽  
A. Zahn ◽  
...  

Abstract. Between April and December 2008 the CARIBIC commercial aircraft conducted monthly measurement flights between Frankfurt, Germany and Chennai, India. These flights covered the period of the Asian summer monsoon (June–September), during which enhancements in a number of atmospheric species were observed in monsoon outflow. In addition to in situ measurements of trace gases and aerosols, whole air samples were collected during the flights, and these were subsequently analyzed for a suite of trace gases that included the non-methane hydrocarbons. Non-methane hydrocarbons are relatively short-lived compounds and the large enhancements in their mixing ratios in the upper troposphere over Southwest Asia between June and September, sometimes more than double their spring and fall means, provides qualitative evidence for the influence of convectively uplifted boundary layer air. The particularly large enhancements of the combustion tracers benzene and ethyne, along with the similarity of their ratios to carbon monoxide and emission ratios from the burning of household biofuels, indicate a strong influence of biofuel burning to NMHC emissions in this region. Conversely, the ratios of ethane and propane to carbon monoxide, along with the ratio between i-butane and n-butane, indicate a significant source of these compounds from the use of LPG and natural gas, and comparison to previous campaigns suggests that this source could be increasing. Photochemical aging patterns of NMHCs showed that the CARIBIC samples were collected in two distinctly different regions of the monsoon circulation: a southern region where air masses had been recently influenced by low level contact and a northern region, where air parcels had spent substantial time in transit in the upper troposphere before being probed. Estimates of age using ratios of individual NMHCs have ranges of 3–6 d in the south and 9–12 d in the north.


2016 ◽  
Vol 16 (13) ◽  
pp. 8389-8403 ◽  
Author(s):  
Jörn Ungermann ◽  
Mandfred Ern ◽  
Martin Kaufmann ◽  
Rolf Müller ◽  
Reinhold Spang ◽  
...  

Abstract. This paper presents an analysis of trace gases in the Asian summer monsoon (ASM) region on the basis of observations by the CRISTA infrared limb sounder taken in low-earth orbit in August 1997. The spatially highly resolved measurements of peroxyacetyl nitrate (PAN) and O3 allow a detailed analysis of an eddy-shedding event of the ASM anticyclone. We identify enhanced PAN volume mixing ratios (VMRs) within the main anticyclone and within the eddy, which are suitable as a tracer for polluted air originating in India and China. Plotting the retrieved PAN VMRs against potential vorticity (PV) and potential temperature reveals that the PV value at which the PAN VMRs exhibit the strongest decrease with respect to PV increases with potential temperature. These PV values might be used to identify the extent of the ASM. Using temperature values also derived from CRISTA measurements, we also computed the location of the thermal tropopause according to the WMO criterion and find that it confines the PAN anomaly vertically within the main ASM anticyclone. In contrast, the shed eddy exhibits enhanced PAN VMRs for 1 to 2 km above the thermal tropopause. Using the relationship between PAN as a tropospheric tracer and O3 as a stratospheric tracer to identify mixed air parcels, we further found the anticyclone to contain few such air parcels, whereas the region between the anticyclone and the eddy as well as the eddy itself contains many mixed air parcels. In combination, this implies that while the anticyclone confines polluted air masses well, eddy shedding provides a very rapid horizontal transport pathway of Asian pollution into the extratropical lowermost stratosphere with a timescale of only a few days.


2016 ◽  
Author(s):  
B. Barret ◽  
B. Sauvage ◽  
Y. Bennouna ◽  
E. Le Flochmoen

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 modelisation 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/IAGOS 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 are responsible for the largest O3 production (10–14 ppbv). Stratosphere to Troposphere Exchanges (STE) are also important in transporting O3 in the upper part of the AMA.


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