scholarly journals Quantifying pollution transport from the Asian monsoon anticyclone into the lower stratosphere

2017 ◽  
Author(s):  
Felix Ploeger ◽  
Paul Konopka ◽  
Kaley Walker ◽  
Martin Riese

Abstract. Pollution transport from the surface to the stratosphere within the Asian monsoon circulation may cause harmful effects on stratospheric chemistry and climate. Here, we investigate air mass transport from the monsoon anticyclone into the stratosphere using a Lagrangian chemistry transport model. We show how two main transport pathways from the anticyclone emerge: (i) into the tropical stratosphere (tropical pipe), and (ii) into the Northern hemisphere (NH) extra-tropical lower stratosphere. Maximum anticyclone air mass fractions reach around 5 % in the tropical pipe and 15 % in the extra-tropical lowermost stratosphere over the course of a year. The anticyclone air mass fraction correlates well with satellite hydrogen cyanide (HCN) and carbon monoxide (CO) observations, corroborating that pollution is transported deep into the tropical stratosphere from the Asian monsoon anticyclone. Cross-tropopause transport occurs in a vertical chimney, but with the emissions transported quasi-horizontally along isentropes above the tropopause into the tropics and NH.

2017 ◽  
Vol 17 (11) ◽  
pp. 7055-7066 ◽  
Author(s):  
Felix Ploeger ◽  
Paul Konopka ◽  
Kaley Walker ◽  
Martin Riese

Abstract. Pollution transport from the surface to the stratosphere within the Asian monsoon circulation may cause harmful effects on stratospheric chemistry and climate. Here, we investigate air mass transport from the monsoon anticyclone into the stratosphere using a Lagrangian chemistry transport model. We show how two main transport pathways from the anticyclone emerge: (i) into the tropical stratosphere (tropical pipe), and (ii) into the Northern Hemisphere (NH) extratropical lower stratosphere. Maximum anticyclone air mass fractions reach around 5 % in the tropical pipe and 15 % in the extratropical lowermost stratosphere over the course of a year. The anticyclone air mass fraction correlates well with satellite hydrogen cyanide (HCN) and carbon monoxide (CO) observations, confirming that pollution is transported deep into the tropical stratosphere from the Asian monsoon anticyclone. Cross-tropopause transport occurs in a vertical chimney, but with the pollutants transported quasi-horizontally along isentropes above the tropopause into the tropics and NH.


2019 ◽  
Vol 19 (24) ◽  
pp. 15629-15649 ◽  
Author(s):  
Xiaolu Yan ◽  
Paul Konopka ◽  
Felix Ploeger ◽  
Aurélien Podglajen ◽  
Jonathon S. Wright ◽  
...  

Abstract. Transport of pollutants into the stratosphere via the Asian summer monsoon (ASM) or North American summer monsoon (NASM) may affect the atmospheric composition and climate both locally and globally. We identify and study the robust characteristics of transport from the ASM and NASM regions to the stratosphere using the Lagrangian chemistry transport model CLaMS driven by both the ERA-Interim and MERRA-2 reanalyses. In particular, we quantify the relative influences of the ASM and NASM on stratospheric composition and investigate the transport pathways and efficiencies of transport of air masses originating at different altitudes in these two monsoon regions to the stratosphere. We release artificial tracers in several vertical layers from the middle troposphere to the lower stratosphere in both ASM and NASM source regions during July and August 2010–2013 and track their evolution until the following summer. We find that more air mass is transported from the ASM and NASM regions to the tropical stratosphere, and even to the southern hemispheric stratosphere, when the tracers are released clearly below the tropopause (350–360 K) than when they are released close to the tropopause (370–380 K). For tracers released close to the tropopause (370–380 K), transport is primarily into the northern hemispheric lower stratosphere. Results for different vertical layers of air origin reveal two transport pathways from the upper troposphere over the ASM and NASM regions to the tropical pipe: (i) quasi-horizontal transport to the tropics below the tropopause followed by ascent to the stratosphere via tropical upwelling, and (ii) ascent into the stratosphere inside the ASM/NASM followed by quasi-horizontal transport to the tropical lower stratosphere and further to the tropical pipe. Overall, the tropical pathway (i) is faster than the monsoon pathway (ii), particularly in the ascending branch. The abundance of air in the tropical pipe that originates in the ASM upper troposphere (350–360 K) is comparable to the abundance of air ascending directly from the tropics to the tropical pipe 10 months after (the following early summer) the release of the source tracers. The air mass contributions from the ASM to the tropical pipe are about 3 times larger than the corresponding contributions from the NASM. The transport efficiency into the tropical pipe, the air mass fraction inside this destination region normalized by the mass of the domain of origin, is greatest from the ASM region at 370–380 K. Although the contribution from the NASM to the stratosphere is less than that from either the ASM or the tropics, the transport efficiency from the NASM is comparable to that from the tropics.


2010 ◽  
Vol 10 (3) ◽  
pp. 1345-1359 ◽  
Author(s):  
G. G. Pfister ◽  
L. K. Emmons ◽  
D. P. Edwards ◽  
A. Arellano ◽  
T. Campos ◽  
...  

Abstract. We analyze the transport of pollution across the Pacific during the NASA INTEX-B (Intercontinental Chemical Transport Experiment Part B) campaign in spring 2006 and examine how this year compares to the time period for 2000 through 2006. In addition to aircraft measurements of carbon monoxide (CO) collected during INTEX-B, we include in this study multi-year satellite retrievals of CO from the Measurements of Pollution in the Troposphere (MOPITT) instrument and simulations from the chemistry transport model MOZART-4. Model tracers are used to examine the contributions of different source regions and source types to pollution levels over the Pacific. Additional modeling studies are performed to separate the impacts of inter-annual variability in meteorology and dynamics from changes in source strength. Interannual variability in the tropospheric CO burden over the Pacific and the US as estimated from the MOPITT data range up to 7% and a somewhat smaller estimate (5%) is derived from the model. When keeping the emissions in the model constant between years, the year-to-year changes are reduced (2%), but show that in addition to changes in emissions, variable meteorological conditions also impact transpacific pollution transport. We estimate that about 1/3 of the variability in the tropospheric CO loading over the contiguous US is explained by changes in emissions and about 2/3 by changes in meteorology and transport. Biomass burning sources are found to be a larger driver for inter-annual variability in the CO loading compared to fossil and biofuel sources or photochemical CO production even though their absolute contributions are smaller. Source contribution analysis shows that the aircraft sampling during INTEX-B was fairly representative of the larger scale region, but with a slight bias towards higher influence from Asian contributions.


2011 ◽  
Vol 11 (1) ◽  
pp. 363-373 ◽  
Author(s):  
H. Bencherif ◽  
L. El Amraoui ◽  
G. Kirgis ◽  
J. Leclair De Bellevue ◽  
A. Hauchecorne ◽  
...  

Abstract. This paper reports on an increase of ozone event observed over Kerguelen (49.4° S, 70.3° E) in relationship with large-scale isentropic transport. This is evidenced by ground-based observations (co-localised radiosonde and SAOZ experiments) together with satellite global observations (Aura/MLS) assimilated into MOCAGE, a Méteo-France model. The study is based on the analyses of the first ozonesonde experiment never recorded at the Kerguelen site within the framework of a French campaign called ROCK that took place from April to August 2008. Comparisons and interpretations of the observed event are supported by co-localised SAOZ observations, by global mapping of tracers (O3, N2O and columns of O3) from Aura/MLS and Aura/OMI experiments, and by model simulations of Ertel Potential Vorticity initialised by the ECMWF (European Centre for Medium-Range Weather Forecasts) data reanalyses. Satellite and ground-based observational data revealed a consistent increase of ozone in the local stratosphere by mid-April 2008. Additionally, Ozone (O3) and nitrous oxide (N2O) profiles obtained during January–May 2008 using the Microwave Limb Sounder (MLS) aboard the Aura satellite are assimilated into MOCAGE (MOdèle de Chimie Atmosphérique à Grande Echelle), a global three-dimensional chemistry transport model of Météo-France. The assimilated total O3 values are consistent with SAOZ ground observations (within ±5%), and isentropic distributions of O3 match well with maps of advected potential vorticity (APV) derived from the MIMOSA model, a high-resolution advection transport model, and from the ECMWF reanalysis. The event studied seems to be related to the isentropic transport of air masses that took place simultaneously in the lower- and middle-stratosphere, respectively from the polar region and from the tropics to the mid-latitudes. In fact, the ozone increase observed by mid April 2008 resulted simultaneously: (1) from an equator-ward departure of polar air masses characterised with a high-ozone layer in the lower stratosphere (near the 475 K isentropic level), and (2) from a reverse isentropic transport from the tropics to mid- and high-latitudes in the upper stratosphere (nearby the 700 K level). The increase of ozone observed over Kerguelen from the 16-April ozonesonde profile is thus attributed to a concomitant isentropic transport of ozone in two stratospheric layers: the tropical air moving southward and reaching over Kerguelen in the upper stratosphere, and the polar air passing over the same area but in the lower stratosphere.


2021 ◽  
Author(s):  
Meike Rotermund ◽  
Vera Bense ◽  
Martyn Chipperfield ◽  
Andreas Engel ◽  
Jens-Uwe Grooß ◽  
...  

<p>We report on measurements of total bromine (Br<sup>tot</sup>) in the upper troposphere and lower stratosphere (UTLS) taken from the German High Altitude and LOng range research aircraft (HALO) over the North Atlantic, Norwegian Sea and north-western Europe in September/ October 2017 during the WISE (Wave-driven ISentropic Exchange) research campaign. Br<sup>tot</sup> is calculated from measured total organic bromine (Br<sup>org</sup>) (i.e., the sum of bromine contained in CH<sub>3</sub>Br, the halons and the major very short-lived brominated substances) added to inorganic bromine (Br<sub>y</sub><sup>inorg</sup>), evaluated from measured BrO and photochemical modelling. Combining these data, the weighted mean [Br<sup>tot</sup>] is 19.2 ± 1.2 ppt in the extratropical lower stratosphere (Ex-LS) of the northern hemisphere. The inferred average Br<sup>tot</sup> for the Ex-LS is slightly smaller than expected for the middle stratosphere in 2016 (~19.6 ppt (ranging from 19-20 ppt) as reported by the WMO/UNEP Assessment (2018)). However, it reflects the expected variability in Br<sup>tot</sup> in the Ex-LS due to influxes of shorter lived brominated source and product gases from different regions of entry. A closer look into Br<sup>org</sup> and Br<sub>y</sub><sup>inorg</sup> as well as simultaneously measured transport tracers (CO, N<sub>2</sub>O, ...) and an air mass lag-time tracer (SF<sub>6</sub>), suggests that a filament of air with elevated Br<sup>tot</sup> protruded into the extratropical lowermost stratosphere (Ex-LMS) from 350-385 K and between equivalent latitudes of 55-80˚N (high bromine filament – HBrF). Lagrangian transport modelling shows the multi-pathway contributions to Ex-LMS bromine. According to CLaMS air mass origin simulations, contributions to the HBrF consist of predominantly isentropic transport from the tropical troposphere (also with elevated [Br<sup>tot</sup>] = 21.6 ± 0.7 ppt) as well as a smaller contribution from an exchange across the extratropical tropopause which are mixed into the stratospheric background air. In contrast, the surrounding LS above and below the HBrF has less tropical tropospheric air, but instead additional stratospheric background air. Of the tropical tropospheric air in the HBrF, the majority is from the outflow of the Asian monsoon anticyclone and the adjacent tropical regions, which greatly influences concentrations of trace gases transported into the Ex-LMS in boreal summer and fall. The resulting increase of Br<sup>tot</sup> in the Ex-LMS and its consequences for ozone is investigated through the TOMCAT/SLIMCAT model simulations. However, more extensive monitoring of total stratospheric bromine in more aged air (i.e., in the middle stratosphere) as well as globally and seasonally is required in addition to model simulations to fully understand its impact on Ex-LMS ozone and the radiative forcing of climate.</p>


2019 ◽  
Vol 19 (21) ◽  
pp. 13547-13567 ◽  
Author(s):  
Corinna Kloss ◽  
Gwenaël Berthet ◽  
Pasquale Sellitto ◽  
Felix Ploeger ◽  
Silvia Bucci ◽  
...  

Abstract. We show that a fire plume injected into the lower stratosphere at high northern latitudes during the Canadian wildfire event in August 2017 partly reached the tropics. The transport to the tropics was mediated by the anticyclonic flow of the Asian monsoon circulation. The fire plume reached the Asian monsoon area in late August/early September, when the Asian monsoon anticyclone (AMA) was still in place. While there is no evidence of mixing into the center of the AMA, we show that a substantial part of the fire plume is entrained into the anticyclonic flow at the AMA edge and is transported from the extratropics to the tropics, and possibly the Southern Hemisphere particularly following the north–south flow on the eastern side of the AMA. In the tropics the fire plume is lifted by ∼5 km in 7 months. Inside the AMA we find evidence of the Asian tropopause aerosol layer (ATAL) in August, doubling background aerosol conditions with a calculated top of the atmosphere shortwave radiative forcing of −0.05 W m−2. The regional climate impact of the fire signal in the wider Asian monsoon area in September exceeds the impact of the ATAL by a factor of 2–4 and compares to that of a plume coming from an advected moderate volcanic eruption. The stratospheric, trans-continental transport of this plume to the tropics and the related regional climate impact point to the importance of long-range dynamical interconnections of pollution sources.


2007 ◽  
Vol 7 (21) ◽  
pp. 5639-5657 ◽  
Author(s):  
P. Ricaud ◽  
B. Barret ◽  
J.-L. Attié ◽  
E. Motte ◽  
E. Le Flochmoën ◽  
...  

Abstract. The mechanism of troposphere-stratosphere exchange in the tropics was investigated from space-borne observations of the horizontal distributions of tropospheric-origin long-lived species, nitrous oxide (N2O), methane (CH4) and carbon monoxide (CO), from 150 to 70 hPa in March-April-May by the ODIN/Sub-Millimeter Radiometer (SMR), the Upper Atmosphere Research Satellite (UARS)/Halogen Occultation Experiment (HALOE) and the TERRA/Measurements Of Pollution In The Troposphere (MOPITT) instruments in 2002–2004, completed by recent observations of the AURA/Microwave Limb Sounder (MLS) instrument during the same season in 2005. The vertical resolution of the satellite measurements ranges from 2 to 4 km. The analysis has been performed on isentropic surfaces: 400 K (lower stratosphere) for all the species and 360 K (upper troposphere) only for CO. At 400 K (and 360 K for CO), all gases show significant longitudinal variations with peak-to-trough values of ~5–11 ppbv for N2O, 0.07–0.13 ppmv for CH4, and ~10 ppbv for CO (~40 ppbv at 360 K). The maximum amounts are primarily located over Africa and, depending on the species, secondary more or less pronounced maxima are reported above northern South America and South-East Asia. The lower stratosphere over the Western Pacific deep convective region where the outgoing longwave radiation is the lowest, the tropopause the highest and the coldest, appears as a region of minimum concentration of tropospheric trace species. The possible impact on trace gas concentration at the tropopause of the inhomogeneous distribution and intensity of the sources, mostly continental, of the horizontal and vertical transports in the troposphere, and of cross-tropopause transport was explored with the MOCAGE Chemistry Transport Model. In the simulations, significant longitudinal variations were found on the medium-lived CO (2-month lifetime) with peak-to-trough value of ~20 ppbv at 360 K and ~10 ppbv at 400 K, slightly weaker than observations. However, the CH4 (8–10 year lifetime) and N2O (130-year lifetime) longitudinal variations are significantly weaker than observed: peak-to-trough values of ~0.02 ppmv for CH4 and 1–2 ppbv for N2O at 400 K. The large longitudinal contrast of N2O and CH4 concentrations reported by the space-borne instruments at the tropopause and in the lower stratosphere not captured by the model thus requires another explanation. The suggestion is of strong overshooting over land convective regions, particularly Africa, very consistent with the space-borne Tropical Rainfall Measuring Mission (TRMM) radar maximum overshooting features over the same region during the same season. Compared to observations, the MOCAGE model forced by ECMWF analyses is found to ignore these fast local uplifts, but to overestimate the average uniform vertical transport in the UTLS at all longitudes in the tropics.


2011 ◽  
Vol 4 (7) ◽  
pp. 1491-1514 ◽  
Author(s):  
P. Valks ◽  
G. Pinardi ◽  
A. Richter ◽  
J.-C. Lambert ◽  
N. Hao ◽  
...  

Abstract. This paper presents the algorithm for the operational near real time retrieval of total and tropospheric NO2 columns from the Global Ozone Monitoring Experiment (GOME-2). The retrieval is performed with the GOME Data Processor (GDP) version 4.4 as used by the EUMETSAT Satellite Application Facility on Ozone and Atmospheric Chemistry Monitoring (O3M-SAF). The differential optical absorption spectroscopy (DOAS) method is used to determine NO2 slant columns from GOME-2 (ir)radiance data in the 425–450 nm range. Initial total NO2 columns are computed using stratospheric air mass factors, and GOME-2 derived cloud properties are used to calculate the air mass factors for scenarios in the presence of clouds. To obtain the stratospheric NO2 component, a spatial filtering approach is used, which is shown to be an improvement on the Pacific reference sector method. Tropospheric air mass factors are computed using monthly averaged NO2 profiles from the MOZART-2 chemistry transport model. An error analysis shows that the random error in the GOME-2 NO2 slant columns is approximately 0.45 × 1015 molec cm−2. As a result of the improved quartz diffuser plate used in the GOME-2 instrument, the systematic error in the slant columns is strongly reduced compared to GOME/ERS-2. The estimated uncertainty in the GOME-2 tropospheric NO2 column for polluted conditions ranges from 40 to 80 %. An end-to-end ground-based validation approach for the GOME-2 NO2 columns is illustrated based on multi-axis MAXDOAS measurements at the Observatoire de Haute Provence (OHP). The GOME-2 stratospheric NO2 columns are found to be in good overall agreement with coincident ground-based measurements at OHP. A time series of the MAXDOAS and the GOME-2 tropospheric NO2 columns shows that pollution episodes at OHP are well captured by GOME-2. Monthly mean tropospheric columns are in very good agreement, with differences generally within 0.5 × 1015 molec cm−2.


2014 ◽  
Vol 14 (7) ◽  
pp. 9951-9973 ◽  
Author(s):  
J. Aschmann ◽  
J. P. Burrows ◽  
C. Gebhardt ◽  
A. Rozanov ◽  
R. Hommel ◽  
...  

Abstract. Chemistry–climate models predict an acceleration of the upwelling branch of the Brewer–Dobson circulation as a consequence of increasing global surface temperatures, resulting from elevated levels of atmospheric greenhouse gases. The observed decrease of ozone in the tropical lower stratosphere during the last decades of the 20th century is consistent with the anticipated acceleration of upwelling. However, more recent satellite observations of ozone reveal that this decrease has unexpectedly stopped in the first decade of the 21st century, challenging the implicit assumption of a continuous acceleration of tropical upwelling. In this study we use three decades of chemistry-transport-model simulations (1980–2013) to investigate this phenomenon and resolve this apparent contradiction. Our model reproduces the observed tropical lower stratosphere ozone record, showing a significant decrease in the early period followed by a statistically robust trend-change after 2002. We demonstrate that this trend-change is correlated with corresponding changes in the vertical transport and conclude that a hiatus in the acceleration of tropical upwelling occurred during the last decade.


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