scholarly journals Trace gas composition in the Asian summer monsoon anticyclone: a case study based on aircraft observations and model simulations

2017 ◽  
Vol 17 (9) ◽  
pp. 6091-6111 ◽  
Author(s):  
Klaus-D. Gottschaldt ◽  
Hans Schlager ◽  
Robert Baumann ◽  
Heiko Bozem ◽  
Veronika Eyring ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Asian Summer Monsoon ◽  
Trace Gas ◽  
Gas Composition ◽  
Back Trajectories ◽  
Air Masses ◽  
Mixing Ratios ◽  
Asian Summer ◽  
In Situ Observations

Abstract. We present in situ measurements of the trace gas composition of the upper tropospheric (UT) Asian summer monsoon anticyclone (ASMA) performed with the High Altitude and Long Range Research Aircraft (HALO) in the frame of the Earth System Model Validation (ESMVal) campaign. Air masses with enhanced O3 mixing ratios were encountered after entering the ASMA at its southern edge at about 150 hPa on 18 September 2012. This is in contrast to the presumption that the anticyclone's interior is dominated by recently uplifted air with low O3 in the monsoon season. We also observed enhanced CO and HCl in the ASMA, which are tracers for boundary layer pollution and tropopause layer (TL) air or stratospheric in-mixing respectively. In addition, reactive nitrogen was enhanced in the ASMA. Along the HALO flight track across the ASMA boundary, strong gradients of these tracers separate anticyclonic from outside air. Lagrangian trajectory calculations using HYSPLIT show that HALO sampled a filament of UT air three times, which included air masses uplifted from the lower or mid-troposphere north of the Bay of Bengal. The trace gas gradients between UT and uplifted air masses were preserved during transport within a belt of streamlines fringing the central part of the anticyclone (fringe), but are smaller than the gradients across the ASMA boundary. Our data represent the first in situ observations across the southern part and downstream of the eastern ASMA flank. Back-trajectories starting at the flight track furthermore indicate that HALO transected the ASMA where it was just splitting into a Tibetan and an Iranian part. The O3-rich filament is diverted from the fringe towards the interior of the original anticyclone, and is at least partially bound to become part of the new Iranian eddy. A simulation with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model is found to reproduce the observations reasonably well. It shows that O3-rich air is entrained by the outer streamlines of the anticyclone at its eastern flank. Back-trajectories and increased HCl mixing ratios indicate that the entrained air originates in the stratospherically influenced TL. Photochemical ageing of air masses in the ASMA additionally increases O3 in originally O3-poor, but CO-rich air. Simulated monthly mean trace gas distributions show decreased O3 in the ASMA centre only at the 100 hPa level in July and August, but at lower altitudes and in September the ASMA is dominated by increased O3. The combination of entrainment from the tropopause region, photochemistry and dynamical instabilities can explain the in situ observations, and might have a larger impact on the highly variable trace gas composition of the anticyclone than previously thought.

scholarly journals Trace gas composition in the Asian summer monsoon anticyclone: A case study based on aircraft observations and model simulations

2016 ◽  
Author(s):  
Klaus-D. Gottschaldt ◽  
Hans Schlager ◽  
Robert Baumann ◽  
Heiko Bozem ◽  
Veronika Eyring ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Atmospheric Chemistry ◽  
Asian Summer Monsoon ◽  
Trace Gas ◽  
Gas Composition ◽  
Back Trajectories ◽  
Air Masses ◽  
Mixing Ratios ◽  
Asian Summer

Abstract. We present in-situ measurements of the trace gas composition of the upper tropospheric (UT) Asian summer monsoon anticyclone (ASMA) performed with the High Altitude and LOng range (HALO) research aircraft in the frame of the Earth System Model Validation (ESMVal) campaign. Air masses with enhanced O3 mixing ratios were encountered after entering the ASMA at its southern edge at about 150 hPa on 18 September 2012. This is in contrast to previous studies, reporting that the anticyclone's interior is dominated by recently uplifted air with low O3 in the monsoon season. We also observed enhanced CO and HCl in the ASMA, tracers for boundary layer pollution and tropopause layer (TL) air or stratospheric inmixing, respectively. In addition, reactive nitrogen was enhanced in the ASMA. Along the HALO flight track across the ASMA boundary, strong gradients of these tracers separate anticyclonic from outside air. Lagrangian trajectory calculations using HYSPLIT show that HALO sampled three times a filament of UT air, which included air masses uplifted from the lower or mid troposphere north of the Bay of Bengal. The trace gas gradients between UT and uplifted air masses were preserved during transport within a belt of streamlines fringing the central part of the anticyclone (fringe), but are smaller than the gradients across the ASMA boundary. Our data represent the first in-situ observations across the southern and downstream the eastern ASMA flank, respectively. Back-trajectories starting at the flight track furthermore indicate that HALO transected the ASMA where it was just splitting into a Tibetan and an Iranian part. The O3-rich filament is diverted from the fringe towards the interior of the original anticyclone, and at least partially bound to become part of the new Iranian eddy. A simulation with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model is found to reproduce the observations reasonably well. It shows that O3-rich air is entrained by the outer streamlines of the anticyclone at its eastern flank. Back-trajectories and increased HCl mixing ratios indicate that the entrained air originates in the stratospherically influenced TL. Photochemical ageing of air masses in the ASMA additionally increases O3 in originally O3-poor, but CO-rich air. Simulated monthly mean trace gas distributions show decreased O3 in the ASMA centre not in general, but only at the 100 hPa level in July and August, as also reported by previous studies. However, at lower altitudes and in September the ASMA is dominated by increased O3, indicating that the above processes are more important for the ASMA trace gas budgets than previously thought.

scholarly journals Observations of PAN and its confinement in the Asian summer monsoon anticyclone in high spatial resolution

2016 ◽  
Vol 16 (13) ◽  
pp. 8389-8403 ◽  
Author(s):  
Jörn Ungermann ◽  
Mandfred Ern ◽  
Martin Kaufmann ◽  
Rolf Müller ◽  
Reinhold Spang ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Asian Summer Monsoon ◽  
Potential Temperature ◽  
Low Earth Orbit ◽  
Transport Pathway ◽  
Air Masses ◽  
Mixing Ratios ◽  
Asian Summer ◽  
The Relationship ◽  
Eddy Shedding

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.

scholarly journals Observations of PAN and its confinement in the Asian Summer Monsoon Anticyclone in high spatial resolution

2016 ◽  
Author(s):  
J. Ungermann ◽  
M. Ern ◽  
M. Kaufmann ◽  
R. Müller ◽  
R. Spang ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Asian Summer Monsoon ◽  
Low Earth Orbit ◽  
Transport Pathway ◽  
Air Masses ◽  
Mixing Ratios ◽  
Asian Summer ◽  
The Relationship ◽  
India And China ◽  
Eddy Shedding

Abstract. This paper presents a set of observations by the CRISTA infrared limb sounder in low-earth orbit taken in August 1997 and analyses of trace-gases in the Asian Summer Monsoon (ASM) region. 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 within the ASM originating in India and China. Comparing the retrieved PAN VMRs with potential vorticity (PV) on isentropes reveals that the PAN VMRs exhibit the strongest decrease at each isentrope for an increasing value of PV which may 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 its location agrees well with the limits of the area of increased PAN VMRs both horizontally on isentropes and vertically within the 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 parcels, whereas the region in between the anticyclone and the eddy contains many mixed 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 time scale of only a few days.

scholarly journals Characterization of non-methane hydrocarbons in Asian summer monsoon outflow observed by the CARIBIC aircraft

2011 ◽  
Vol 11 (2) ◽  
pp. 503-518 ◽  
Author(s):  
A. K. Baker ◽  
T. J. Schuck ◽  
F. Slemr ◽  
P. van Velthoven ◽  
A. Zahn ◽  
...  
Keyword(s):  
Carbon Monoxide ◽  
Summer Monsoon ◽  
Fossil Fuels ◽  
Asian Summer Monsoon ◽  
Trace Gases ◽  
Northern Region ◽  
Monsoon Circulation ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Asian Summer

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.

scholarly journals Dynamics and composition of the Asian summer monsoon anticyclone

2017 ◽  
Author(s):  
Klaus-Dirk Gottschaldt ◽  
Hans Schlager ◽  
Robert Baumann ◽  
Duy S. Cai ◽  
Veronika Eyring ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Atmospheric Chemistry ◽  
Asian Summer Monsoon ◽  
Monsoon Season ◽  
Lower Troposphere ◽  
Equatorial Region ◽  
Ozone Production ◽  
Trace Gas ◽  
Asian Summer ◽  
Southern Fringe

Abstract. This study places HALO research aircraft observations in the upper-tropospheric Asian summer monsoon anticyclone (ASMA) obtained during the Earth System Model Validation (ESMVal) campaign in September 2012 into the context of regional, intra-annual variability by hindcasts with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The simulations demonstrate that tropospheric trace gas profiles in the monsoon season are distinct from the rest of the year. Air uplifted from the lower troposphere to the tropopause layer dominates the eastern part of the ASMA’s interior, while the western part is characterised by subsidence down to the mid-troposphere. Soluble compounds are being washed out when uplifted by convection in the eastern part, where lightning simultaneously replenishes reactive nitrogen in the upper troposphere. Net photochemical ozone production is significantly enhanced in the ASMA, contrasted by an ozone depleting regime in the mid-troposphere and more neutral conditions in autumn and winter. An analysis of multiple monsoon seasons in the simulation shows that stratospherically influenced tropopause layer air is regularly entrained at the eastern ASMA flank, and then transported in the southern fringe around the interior region. Observed and simulated tracer-tracer relations reflect photochemical O3 production, as well as in-mixing from the lower troposphere and the tropopause layer. The simulation additionally shows entrainment of clean air from the equatorial region by northerly winds at the western ASMA flank. Although the in situ measurements were performed towards the end of summer, the main ingredients needed for their interpretation are present throughout the monsoon season. A transition between two dynamical modes of the ASMA took place during the HALO ESMVal campaign. Transport barriers of the original anticyclone are overcome effectively when it splits up. Air from the fringe is stirred into the interiors of the new anticyclones and vice versa. Instabilities of this and other types occur quite frequently. Our study emphasises their paramountcy for the trace gas composition of the ASMA and its outflow into regions around the world.

scholarly journals Trapping, chemistry and export of trace gases in the South Asian summer monsoon observed during CARIBIC flights in 2008

2015 ◽  
Vol 15 (5) ◽  
pp. 6967-7018 ◽  
Author(s):  
A. Rauthe-Schöch ◽  
A. K. Baker ◽  
T. J. Schuck ◽  
C. A. M. Brenninkmeijer ◽  
A. Zahn ◽  
...  
Keyword(s):  
South Asian ◽  
Summer Monsoon ◽  
Asian Summer Monsoon ◽  
Trace Gases ◽  
Particle Dispersion ◽  
Atmospheric Pollutants ◽  
South Asian Summer Monsoon ◽  
The South ◽  
Air Masses ◽  
Asian Summer

Abstract. The CARIBIC (Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container) passenger aircraft observatory performed in situ measurements at 10–12 km altitude in the South Asian summer monsoon anticyclone between June and September 2008. These measurements enable us to investigate this atmospheric region, which so far has mostly been observed from satellites, using the broad suite of trace gases and aerosols measured by CARIBIC. Elevated levels of a range of atmospheric pollutants were recorded e.g. carbon monoxide, total reactive nitrogen oxides, aerosol particles and several volatile organic compounds. The measurements provide detailed information about the chemical composition of air in different parts of the monsoon anticyclone, particularly of ozone precursors. While covering a range of 3500 km inside the monsoon anticyclone, CARIBIC observations show remarkable consistency, i.e. with regular latitudinal patterns of trace gases during the entire monsoon period. Trajectory calculations indicate that these air masses originated mainly from South Asia and Mainland Southeast Asia. Using the CARIBIC trace gas and aerosol measurements in combination with the Lagrangian particle dispersion model FLEXPART we investigated the characteristics of monsoon outflow and the chemical evolution of air masses during transport. Estimated photochemical ages of the air were found to agree well with transport times from a source region east of 95° E. The photochemical ages of the air in the southern part of the monsoon anticyclone were consistently younger (less than 7 days) and the air masses mostly in an ozone forming chemical regime. In its northern part the air masses were older (up to 13 days) and had unclear ozone formation or destruction potential. Based on analysis of forward trajectories several receptor regions were identified. In addition to predominantly westward transport, we found evidence for efficient transport (within 10 days) to the Pacific and North America, particularly during June and September, and also of cross-tropopause exchange, which was strongest during June and July. Westward transport to Africa and further to the Mediterranean was the main pathway during July.

scholarly journals Dynamics and composition of the Asian summer monsoon anticyclone

2018 ◽  
Vol 18 (8) ◽  
pp. 5655-5675 ◽  
Author(s):  
Klaus-Dirk Gottschaldt ◽  
Hans Schlager ◽  
Robert Baumann ◽  
Duy Sinh Cai ◽  
Veronika Eyring ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
Atmospheric Chemistry ◽  
Asian Summer Monsoon ◽  
Monsoon Season ◽  
Lower Troposphere ◽  
Trace Gas ◽  
Transport Barriers ◽  
Research Aircraft ◽  
Asian Summer ◽  
Southern Fringe

Abstract. This study places HALO research aircraft observations in the upper-tropospheric Asian summer monsoon anticyclone (ASMA) into the context of regional, intra-annual variability by hindcasts with the ECHAM/MESSy Atmospheric Chemistry (EMAC) model. The observations were obtained during the Earth System Model Validation (ESMVal) campaign in September 2012. Observed and simulated tracer–tracer relations reflect photochemical O3 production as well as in-mixing from the lower troposphere and the tropopause layer. The simulations demonstrate that tropospheric trace gas profiles in the monsoon season are distinct from those in the rest of the year, and the measurements reflect the main processes acting throughout the monsoon season. Net photochemical O3 production is significantly enhanced in the ASMA, where uplifted precursors meet increased NOx, mainly produced by lightning. An analysis of multiple monsoon seasons in the simulation shows that stratospherically influenced tropopause layer air is regularly entrained at the eastern ASMA flank and then transported in the southern fringe around the interior region. Radial transport barriers of the circulation are effectively overcome by subseasonal dynamical instabilities of the anticyclone, which occur quite frequently and are of paramount importance for the trace gas composition of the ASMA. Both the isentropic entrainment of O3-rich air and the photochemical conversion of uplifted O3-poor air tend to increase O3 in the ASMA outflow.

scholarly journals Impact of the Asian monsoon on the extratropical lower stratosphere: trace gas observations during TACTS over Europe 2012

2015 ◽  
Vol 15 (23) ◽  
pp. 34765-34812
Author(s):  
S. Müller ◽  
P. Hoor ◽  
H. Bozem ◽  
E. Gute ◽  
B. Vogel ◽  
...  
Keyword(s):  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Asian Summer Monsoon ◽  
Trace Gas ◽  
Boreal Summer ◽  
Monsoon Circulation ◽  
Transport Pathway ◽  
Air Masses ◽  
Time Period ◽  
Asian Summer

Abstract. The transport of air masses originating from the Asian monsoon anticyclone into the extratropical upper troposphere and lower stratosphere (Ex-UTLS) above potential temperatures Θ = 380 K was identified during the HALO aircraft mission TACTS in August and September 2012. In-situ measurements of CO, O3 and N2O during TACTS Flight 2 on the 30 August 2012 show the irreversible mixing of aged with younger (originating from the troposphere) stratospheric air masses within the Ex-UTLS. Backward trajectories calculated with the trajetory module of the CLaMS model indicate that these tropospherically affected air masses originate from the Asian monsoon anticyclone. From the monsoon circulation region these air masses are quasi-isentropically transported above Θ = 380 K into the Ex-UTLS where they subsequently mix with stratospheric air masses. The overall trace gas distribution measured during TACTS shows that this transport pathway has a significant impact on the Ex-UTLS during boreal summer and autumn. This leads to an intensification of the tropospheric influence on the Ex-UTLS with ΔΘ > 30 K (relative to the tropopause) within three weeks during the TACTS mission. In the same time period a weakening of the tropospheric influence on the lowermost stratosphere (LMS) is determined. Therefore, the study shows that the transport of air masses originating from the Asian summer monsoon region within the lower stratosphere above Θ = 380 K is of major importance for the change of the chemical composition of the Ex-UTLS from summer to autumn.

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