Organic and inorganic bromine measurements around the extratropical tropopause and lowermost stratosphere (Ex-LMS): Insights into transport pathways and total bromine 

2021 ◽  
Author(s):  
Meike Rotermund ◽  
Vera Bense ◽  
Martyn Chipperfield ◽  
Andreas Engel ◽  
Jens-Uwe Grooß ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Boreal Summer ◽  
Transport Modelling ◽  
Transport Pathways ◽  
Air Mass ◽  
Model Simulations ◽  
Extratropical Tropopause ◽  
Background Air ◽  
Middle Stratosphere

<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>

scholarly journals Organic and inorganic bromine measurements around the extratropical tropopause and lowermost stratosphere: Insights into the transport pathways and total bromine

2021 ◽  
Author(s):  
Meike K. Rotermund ◽  
Vera Bense ◽  
Martyn P. Chipperfield ◽  
Andreas Engel ◽  
Jens-Uwe Grooß ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Source Region ◽  
Weighted Average ◽  
Boreal Summer ◽  
Weighted Mean ◽  
Air Mass ◽  
Upper Troposphere ◽  
Middle Stratosphere

Abstract. We report on measurements of total bromine (Brtot) in the upper troposphere and lower stratosphere taken during 15 flights with the German High Altitude and LOng range research aircraft (HALO). The research campaign WISE (Wave-driven ISentropic Exchange) included regions over the North Atlantic, Norwegian Sea and north-western Europe in fall 2017. Brtot is calculated from measured total organic bromine (Brorg) added to inorganic bromine (Bryinorg), evaluated from measured BrO and photochemical modelling. Combining these data, the weighted-mean [Brtot] is 19.2 ± 1.2 ppt in the northern hemispheric lower stratosphere (LS) in agreement with expectations for Brtot in the middle stratosphere (Engel and Rigby et al. (2018)). The data reflects the expected variability in Brtot in the LS due to variable influx of shorter-lived brominated source and product gases from different regions of entry. A closer look into Brorg and Bryinorg, as well as simultaneously measured transport tracers (CO and N2O) and an air mass lag-time tracer (SF6), suggests that bromine-rich air masses persistently protruded into the lowermost stratosphere (LMS) in boreal summer, creating a high bromine region (HBrR). A subsection, HBrR*, has a weighted average of [Brtot] = 20.9 ± 0.8 ppt. The most probable source region is former air from the tropical upper troposphere and tropopause layer (UT/TTL) with a weighted mean [Brtot] = 21.6 ± 0.7 ppt. CLaMS Lagrangian transport modelling shows that the HBrR air mass consists of 51.2 % from the tropical troposphere, 27.1 % from the stratospheric background, and 6.4 % from the mid-latitude troposphere (as well as contributions from other domains). The majority of the surface air reaching the HBrR is from the Asian monsoon and its adjacent tropical regions, which greatly influences trace gas transport into the LMS in boreal summer and fall. Tropical cyclones from Central America in addition to air associated with the Asian monsoon region contribute to the elevated Brtot observed in the UT/TTL. TOMCAT global 3–D model simulations of a concurrent increase of Brtot show an associated O3 change of −2.6 ± 0.7 % in the LS and −3.1 ± 0.7 % near the tropopause. Our study of varying Brtot in the LS also emphasizes the need for more extensive monitoring of stratospheric Brtot globally and seasonally to fully understand its impact on LMS O3 and its radiative forcing of climate, as well as in aged air in the middle stratosphere to elucidate the stratospheric trend in bromine.

scholarly journals Organic and inorganic bromine measurements around the extratropical tropopause and lowermost stratosphere: insights into the transport pathways and total bromine

2021 ◽  
Vol 21 (20) ◽  
pp. 15375-15407
Author(s):  
Meike K. Rotermund ◽  
Vera Bense ◽  
Martyn P. Chipperfield ◽  
Andreas Engel ◽  
Jens-Uwe Grooß ◽  
...  
Keyword(s):  
Radiative Forcing ◽  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Source Region ◽  
Weighted Average ◽  
Boreal Summer ◽  
Weighted Mean ◽  
Air Mass ◽  
Upper Troposphere ◽  
Middle Stratosphere

Abstract. We report on measurements of total bromine (Brtot) in the upper troposphere and lower stratosphere taken during 15 flights with the German High Altitude and LOng range research aircraft (HALO). The research campaign WISE (Wave-driven ISentropic Exchange) included regions over the North Atlantic, Norwegian Sea, and northwestern Europe in fall 2017. Brtot is calculated from measured total organic bromine (Brorg) added to inorganic bromine (Bryinorg), evaluated from measured BrO and photochemical modeling. Combining these data, the weighted mean [Brtot] is 19.2±1.2 ppt in the northern hemispheric lower stratosphere (LS), in agreement with expectations for Brtot in the middle stratosphere (Engel and Rigby et al., 2018). The data reflect the expected variability in Brtot in the LS due to variable influx of shorter lived brominated source and product gases from different regions of entry. A closer look into Brorg and Bryinorg, as well as simultaneously measured transport tracers (CO and N2O) and an air mass lag time tracer (SF6), suggests that bromine-rich air masses persistently protruded into the lowermost stratosphere (LMS) in boreal summer, creating a high bromine region (HBrR). A subsection, HBrR∗, has a weighted average of [Brtot] = 20.9±0.8 ppt. The most probable source region is air recently transported from the tropical upper troposphere and tropopause layer (UT/TTL) with a weighted mean of [Brtot] = 21.6±0.7 ppt. CLaMS Lagrangian transport modeling shows that the HBrR air mass consists of 51.2 % from the tropical troposphere, 27.1 % from the stratospheric background, and 6.4 % from the midlatitude troposphere (as well as contributions from other domains). The majority of the surface air reaching the HBrR is from the Asian monsoon and its adjacent tropical regions, which greatly influences trace gas transport into the LMS in boreal summer and fall. Tropical cyclones from Central America in addition to air associated with the Asian monsoon region contribute to the elevated Brtot observed in the UT/TTL. TOMCAT global 3-D model simulations of a concurrent increase of Brtot show an associated O3 change of -2.6±0.7 % in the LS and -3.1±0.7 % near the tropopause. Our study of varying Brtot in the LS also emphasizes the need for more extensive monitoring of stratospheric Brtot globally and seasonally to fully understand its impact on LMS O3 and its radiative forcing of climate, as well as in aged air in the middle stratosphere to elucidate the stratospheric trend in bromine.

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

2017 ◽  
Vol 17 (11) ◽  
pp. 7055-7066 ◽  
Author(s):  
Felix Ploeger ◽  
Paul Konopka ◽  
Kaley Walker ◽  
Martin Riese
Keyword(s):  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Monsoon Circulation ◽  
Pollution Transport ◽  
Chemistry Transport Model ◽  
Transport Pathways ◽  
Air Mass ◽  
Mass Fractions ◽  
The Tropics

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.

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
Keyword(s):  
Asian Monsoon ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Monsoon Circulation ◽  
Pollution Transport ◽  
Chemistry Transport Model ◽  
Transport Pathways ◽  
Air Mass ◽  
Mass Fractions ◽  
The Tropics

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.

scholarly journals Transport analysis and source attribution of seasonal and interannual variability of CO in the tropical upper troposphere and lower stratosphere

2013 ◽  
Vol 13 (1) ◽  
pp. 129-146 ◽  
Author(s):  
J. Liu ◽  
J. A. Logan ◽  
L. T. Murray ◽  
H. C. Pumphrey ◽  
M. J. Schwartz ◽  
...  
Keyword(s):  
Annual Cycle ◽  
Annual Variation ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Boreal Summer ◽  
Lower Altitude ◽  
Model Simulations ◽  
Upper Troposphere ◽  
Annual Variations ◽  
Upward Transport

Abstract. We used the GEOS-Chem chemistry-transport model to investigate impacts of surface emissions and dynamical processes on the spatial and temporal patterns of CO observed by the Microwave Limb Sounder (MLS) in the upper troposphere (UT) and lower stratosphere (LS). Model simulations driven by GEOS-4 and GEOS-5 assimilated fields present many features of the seasonal and inter-annual variation of CO in the upper troposphere and lower stratosphere. Both model simulations and the MLS data show a transition from semi-annual variations in the UT to annual variations in the LS. Tagged CO simulations indicate that the semi-annual variation of CO in the UT is determined mainly by the temporal overlapping of surface biomass burning from different continents as well as the north-south shifts of deep convection. Both GEOS-4 and GEOS-5 have maximum upward transport in April and May with a minimum in July to September. The CO peaks from the Northern Hemisphere (NH) fires propagate faster to the LS than do those from the Southern Hemisphere (SH) fires. Thus the transition from a semi-annual to an annual cycle around 80 hPa is induced by a combination of the CO signal at the tropopause and the annual cycle of the Brewer-Dobson circulation. In GEOS-5, the shift to an annual cycle occurs at a lower altitude than in MLS CO, a result of inadequate upward transport. We deduce vertical velocities from MLS CO, and use them to evaluate the velocities derived from the archived GEOS meteorological fields. We find that GEOS-4 velocities are similar to those from MLS CO between 215 hPa and 125 hPa, while the velocities in GEOS-5 are too low in spring and summer. The mean tropical vertical velocities from both models are lower than those inferred from MLS CO above 100 hPa, particularly in GEOS-5, with mean downward, rather than upward motion in boreal summer. Thus the models' CO maxima from SH burning are transported less effectively than those in MLS CO above 147 hPa and almost disappear by 100 hPa. The strongest peaks in the CO tape-recorder are in late 2004, 2006, and 2010, with the first two resulting from major fires in Indonesia and the last from severe burning in South America, all associated with intense droughts.

scholarly journals Transport analysis and source attribution of seasonal and interannual variability of CO in the tropical upper troposphere and lower stratosphere

2012 ◽  
Vol 12 (7) ◽  
pp. 17397-17442 ◽  
Author(s):  
Junhua Liu ◽  
J. A. Logan ◽  
L. T. Murray ◽  
H. C. Pumphrey ◽  
M. J. Schwartz ◽  
...  
Keyword(s):  
Annual Cycle ◽  
Annual Variation ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Boreal Summer ◽  
Lower Altitude ◽  
Model Simulations ◽  
Upper Troposphere ◽  
Annual Variations ◽  
Upward Transport

Abstract. We used the GEOS-Chem chemistry-transport model to investigate impacts of surface emissions and dynamical processes on the spatial and temporal patterns of CO observed by the Microwave Limb Sounder (MLS) in the upper troposphere and lower stratosphere (UTLS). Model simulations driven by GEOS-4 and GEOS-5 assimilated fields present many features of the seasonal and inter-annual variation of CO in the UTLS. Both model simulations and the MLS data show a transition from semi-annual variations in the UT to annual variations in the LS. Tagged CO simulations indicate that the semi-annual variation of CO in the UT is determined mainly by the temporal overlapping of surface biomass burning from different continents as well as the north-south shifts of deep convection. Both GEOS-4 and GEOS-5 have maximum upward transport in April and May with a minimum in July to September. The CO peaks from NH fires propagate faster to the LS than do those from SH fires. Thus the transition from a semi-annual to an annual cycle around 80 hPa is induced by a combination of the CO signal at the tropopause and the annual cycle of the Brewer-Dobson circulation. In GEOS-5, the shift to an annual cycle occurs at a lower altitude than in MLS CO, a result of inadequate upward transport. We deduce vertical velocities from MLS CO, and find that those in GEOS-4 agree well with them between 215 hPa and 125 hPa in boreal summer, fall and winter, while the velocities in GEOS-5 are too low in all seasons. The mean tropical vertical velocities from both models are lower than those inferred from MLS CO above 100 hPa in June to November, particularly in GEOS-5, with mean downward, rather than upward motion in boreal summer. Thus the models' CO maxima from SH burning are transported less effectively than those in MLS CO above 147 hPa and almost disappear by 100 hPa. The strongest peaks in the CO tape-recorder are in late 2004, 2006, and 2010, with the first two resulting from major fires in Indonesia and the last from severe burning in South America, all associated with intense droughts.

scholarly journals The efficiency of transport into the stratosphere via the Asian and North American summer monsoon circulations

2019 ◽  
Vol 19 (24) ◽  
pp. 15629-15649 ◽  
Author(s):  
Xiaolu Yan ◽  
Paul Konopka ◽  
Felix Ploeger ◽  
Aurélien Podglajen ◽  
Jonathon S. Wright ◽  
...  
Keyword(s):  
Summer Monsoon ◽  
North American ◽  
Lower Stratosphere ◽  
Atmospheric Composition ◽  
Transport Pathways ◽  
Air Mass ◽  
Transport Efficiency ◽  
Upper Troposphere ◽  
Horizontal Transport ◽  
The Tropics

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.

scholarly journals Dispersion of the Nabro volcanic plume and its relation to the Asian summer monsoon

2013 ◽  
Vol 13 (12) ◽  
pp. 33177-33205 ◽  
Author(s):  
T. D. Fairlie ◽  
J.-P. Vernier ◽  
M. Natarajan ◽  
K. M. Bedka
Keyword(s):  
East Asia ◽  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Asian Summer Monsoon ◽  
Stratospheric Aerosol ◽  
Boreal Summer ◽  
Volcanic Plume ◽  
Direct Role ◽  
Volcanic Material ◽  
The Impact

Abstract. We use nighttime measurements from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite, together with a Lagrangian trajectory model, to study the initial dispersion of volcanic aerosol from the eruption of Mt. Nabro (Ethiopia/Eritrea) in June 2011. The Nabro eruption reached the lower stratosphere directly, and dispersal of the plume in the upper troposphere and lower stratosphere (UTLS) was constrained initially by the Asian anticyclone, which prevails in the UTLS from the Mediterranean Sea to East Asia during boreal summer. CALIPSO detected aerosol layers, with optical properties consistent with sulfate, in the lower stratosphere above the monsoon convective region in South and South-East Asia within 10 days of the eruption. We show that quasi-isentropic differential advection in the vertically sheared flow surrounding the Asian anticyclone explains many of these stratospheric aerosol layers. We use Meteosat-7 data to examine the possible role of deep convection in the Asian monsoon in transporting volcanic material to the lower stratosphere during this time, but find no evidence that convection played a direct role, in contrast with claims made in earlier studies. On longer time scales, we use CALIPSO data to illustrate diabatic ascent of the Nabro aerosol in the lower stratosphere, at rates of ~10 K per month for the first two months after the eruption, falling to ~3 K per month after the Asian anticyclone dissipates. We attribute ~15% of this to self-lofting. We show that aerosol optical depth associated with the Nabro plume peaks in July; we find the associated radiative forcing is relatively small; top of atmosphere (TOA) radiative forcing peaks at ~1.6 W m−2 locally in July, ~10% of that reported for the impact of Pinatubo in 1991 and within observed interannual variability.

scholarly journals The outflow of Asian biomass burning carbonaceous aerosol into the upper troposphere and lower stratosphere in spring: radiative effects seen in a global model

2021 ◽  
Vol 21 (18) ◽  
pp. 14371-14384
Author(s):  
Prashant Chavan ◽  
Suvarna Fadnavis ◽  
Tanusri Chakroborty ◽  
Christopher E. Sioris ◽  
Sabine Griessbach ◽  
...  
Keyword(s):  
Water Vapor ◽  
Biomass Burning ◽  
Radiative Forcing ◽  
Lower Stratosphere ◽  
Carbonaceous Aerosol ◽  
The Arctic ◽  
Carbonaceous Aerosols ◽  
Maximum Enhancement ◽  
Model Simulations ◽  
Upper Troposphere

Abstract. Biomass burning (BB) over Asia is a strong source of carbonaceous aerosols during spring. From ECHAM6–HAMMOZ model simulations and satellite observations, we show that there is an outflow of Asian BB carbonaceous aerosols into the upper troposphere and lower stratosphere (UTLS) (black carbon: 0.1 to 6 ng m−3 and organic carbon: 0.2 to 10 ng m−3) during the spring season. The model simulations show that the greatest transport of BB carbonaceous aerosols into the UTLS occurs from the Indochina and East Asia region by deep convection over the Malay Peninsula and Indonesia. The increase in BB carbonaceous aerosols enhances atmospheric heating by 0.001 to 0.02 K d−1 in the UTLS. The aerosol-induced heating and circulation changes increase the water vapor mixing ratios in the upper troposphere (by 20–80 ppmv) and in the lowermost stratosphere (by 0.02–0.3 ppmv) over the tropics. Once in the lower stratosphere, water vapor is further transported to the South Pole by the lowermost branch of the Brewer–Dobson circulation. These aerosols enhance the in-atmosphere radiative forcing (0.68±0.25 to 5.30±0.37 W m−2), exacerbating atmospheric warming, but produce a cooling effect on climate (top of the atmosphere – TOA: -2.38±0.12 to -7.08±0.72 W m−2). The model simulations also show that Asian carbonaceous aerosols are transported to the Arctic in the troposphere. The maximum enhancement in aerosol extinction is seen at 400 hPa (by 0.0093 km−1) and associated heating rates at 300 hPa (by 0.032 K d−1) in the Arctic.

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