scholarly journals Pollution trace gases C<sub>2</sub>H<sub>6</sub>, C<sub>2</sub>H<sub>2</sub>, HCOOH, and PAN in the North Atlantic UTLS: observations and simulations

2021 ◽  
Vol 21 (10) ◽  
pp. 8213-8232
Author(s):  
Gerald Wetzel ◽  
Felix Friedl-Vallon ◽  
Norbert Glatthor ◽  
Jens-Uwe Grooß ◽  
Thomas Gulde ◽  
...  

Abstract. Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave-driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMRs) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Elevated quantities of PAN were measured even in the lowermost stratosphere (locally up to 14 km), likely reflecting the fact that this molecule has the longest lifetime of the four species discussed herein. Backward trajectory calculations as well as global three-dimensional Chemical Lagrangian Model of the Stratosphere (CLaMS) simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South Asia and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models.

2020 ◽  
Author(s):  
Gerald Wetzel ◽  
Felix Friedl-Vallon ◽  
Norbert Glatthor ◽  
Jens-Uwe Grooß ◽  
Thomas Gulde ◽  
...  

Abstract. Measurements of the pollution trace gases ethane (C2H6), ethyne (C2H2), formic acid (HCOOH), and peroxyacetyl nitrate (PAN) were performed in the North Atlantic upper troposphere and lowermost stratosphere (UTLS) region with the airborne limb imager GLORIA (Gimballed Limb Observer for Radiance Imaging of the Atmosphere) with high spatial resolution down to cloud top. Observations were made during flights with the German research aircraft HALO (High Altitude and LOng Range Research Aircraft) in the frame of the WISE (Wave-driven ISentropic Exchange) campaign, which was carried out in autumn 2017 from Shannon (Ireland) and Oberpfaffenhofen (Germany). Enhanced volume mixing ratios (VMR) of up to 2.2 ppbv C2H6, 0.2 ppbv C2H2, 0.9 ppbv HCOOH, and 0.4 ppbv PAN were detected during the flight on 13 September 2017 in the upper troposphere and around the tropopause above the British Isles. Since PAN has the longest lifetime of this foursome, elevated quantities of this molecule could be measured even in the lowermost stratosphere (locally up to 14 km). Backward trajectory calculations as well as global three-dimensional CLaMS simulations with artificial tracers of air mass origin have shown that the main sources of the observed pollutant species are forest fires in North America and anthropogenic pollution in South and Southeast Asia uplifted and moved within the Asian monsoon anticyclone (AMA) circulation system. After release from the AMA, these species or their precursor substances are transported by strong tropospheric winds over large distances, depending on their particular atmospheric lifetime of up to months. Observations are compared to simulations with the atmospheric models EMAC (ECHAM5/MESSy Atmospheric Chemistry) and CAMS (Copernicus Atmosphere Monitoring Service). These models are qualitatively able to reproduce the measured VMR enhancements but underestimate the absolute amount of the increase. Increasing the emissions in EMAC by a factor of 2 reduces the disagreement between simulated and measured results and illustrates the importance of the quality of emission databases used in chemical models.


2008 ◽  
Vol 8 (2) ◽  
pp. 7509-7554
Author(s):  
E. Real ◽  
K. Law ◽  
H. Schlager ◽  
A. Roiger ◽  
H. Huntrieser ◽  
...  

Abstract. The photochemical evolution of an anthropogenic plume from the New-York/Boston region during its transport at low altitudes over the North Atlantic to the European west coast has been studied using a Lagrangian framework. This plume, originally strongly polluted, was sampled by research aircraft just off the North American east coast on 3 successive days, and 3 days downwind off the west coast of Ireland where another aircraft re-sampled a weakly polluted plume. Changes in trace gas concentrations during transport were reproduced using a photochemical trajectory model including deposition and mixing effects. Chemical and wet deposition processing dominated the evolution of all pollutants in the plume. The mean net O3 production was evaluated to be -5 ppbv/day leading to low values of O3 by the time the plume reached Europe. Wet deposition of nitric acid was responsible for an 80% reduction in this O3 production. If the plume had not encountered precipitation, it would have reached the Europe with O3 levels up to 80-90 ppbv, and CO levels between 120 and 140 ppbv. Photochemical destruction also played a more important role than mixing in the evolution of plume CO due to high levels of both O3 and water vapour showing that CO cannot always be used as a tracer for polluted air masses, especially for plumes transported at low altitudes. The results also show that, in this case, an important increase in the O3/CO slope can be attributed to chemical destruction of CO and not to photochemical O3 production as is often assumed.


2019 ◽  
Vol 19 (10) ◽  
pp. 6621-6636 ◽  
Author(s):  
Thorsten Kaluza ◽  
Daniel Kunkel ◽  
Peter Hoor

Abstract. The evolution of the tropopause inversion layer (TIL) during cyclogenesis in the North Atlantic storm track is investigated using operational meteorological analysis data (Integrated Forecast System from the European Centre for Medium-Range Weather Forecasts). For this a total of 130 cyclones have been analysed during the months August through October between 2010 and 2014 over the North Atlantic. Their paths of migration along with associated flow features in the upper troposphere and lower stratosphere (UTLS) have been tracked based on the mean sea level pressure field. Subsets of the 130 cyclones have been used for composite analysis using minimum sea level pressure to filter the cyclones based on their strength. The composite structure of the TIL strength distribution in connection with the overall UTLS flow strongly resembles the structure of the individual cyclones. Key results are that a strong dipole in TIL strength forms in regions of cyclonic wrap-up of UTLS air masses of different origin and isentropic potential vorticity. These air masses are associated with the cyclonic rotation of the underlying cyclones. The maximum values of enhanced static stability above the tropopause occur north and northeast of the cyclone centre, vertically aligned with outflow regions of strong updraft and cloud formation up to the tropopause, which are situated in anticyclonic flow patterns in the upper troposphere. These regions are co-located with a maximum of vertical shear of the horizontal wind. The strong wind shear within the TIL results in a local minimum of Richardson numbers, representing the possibility for turbulent instability and potential mixing (or air mass exchange) within regions of enhanced static stability in the lowermost stratosphere.


2020 ◽  
Author(s):  
Gerald Wetzel ◽  
Felix Friedl-Vallon ◽  
Norbert Glatthor ◽  
Jens-Uwe Grooß ◽  
Thomas Gulde ◽  
...  

&lt;p&gt;The Gimballed Limb Observer for Radiance Imaging of the Atmosphere (GLORIA) is an imaging Fourier transform spectrometer (iFTS) using a 2-dimensional detector array to record emission spectra in the mid-infrared region with high spatial resolution. GLORIA is operated on high altitude research aircraft, mainly in the limb observational geometry to measure vertical profiles of temperature and atmospheric trace species with high vertical resolution.&lt;/p&gt;&lt;p&gt;In autumn 2017, the Wave-driven ISentropic Exchange (WISE) aircraft campaign took place from Shannon (Ireland). Sixteen flights with the High Altitude and Long Range Research Aircraft (HALO) were performed between 31 August and 21 October 2017 over the eastern North Atlantic region.&lt;/p&gt;&lt;p&gt;GLORIA observations were analysed with regard to pollutant species like C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;6&lt;/sub&gt;, C&lt;sub&gt;2&lt;/sub&gt;H&lt;sub&gt;2&lt;/sub&gt;, HCOOH, and PAN, which are produced at distinct source regions near the ground and transported to remote regions due to their atmospheric lifetime of several weeks. Enhanced volume mixing ratios of these molecules were detected along some parts of the flight track in the upper troposphere and lowermost stratosphere (UTLS).&lt;/p&gt;&lt;p&gt;Measured profiles of these species are compared to simulations from the ECHAM/MESSy Atmospheric Chemistry (EMAC) model and reanalysis data from the Copernicus Atmosphere Monitoring Service (CAMS). Furthermore, emission tracers and back-trajectories from the Chemical Lagrangian Model of the Stratosphere (CLaMS) are used to analyse the source regions of these pollution events.&lt;/p&gt;


2000 ◽  
Vol 105 (D15) ◽  
pp. 19795-19809 ◽  
Author(s):  
J. Crawford ◽  
D. Davis ◽  
J. Olson ◽  
G. Chen ◽  
S. Liu ◽  
...  

2008 ◽  
Vol 8 (7) ◽  
pp. 1989-2005 ◽  
Author(s):  
S. Y. Kim ◽  
R. Talbot ◽  
H. Mao ◽  
D. Blake ◽  
S. Vay ◽  
...  

Abstract. A case of continental outflow from the United States (US) was examined using airborne measurements from NASA DC-8 flight 13 during the Intercontinental Chemical Transport Experiment – North America (INTEX-NA). Mixing ratios of methane (CH4) and carbon monoxide (CO) at 8–11 km altitude over the North Atlantic were elevated to 1843 ppbv and 134 ppbv respectively, while those of carbon dioxide (CO2) and carbonyl sulfide (COS) were reduced to 372.4 ppmv and 411 pptv respectively. In this region, urban and industrial influences were evidenced by elevated mixing ratios and good linear relationships between urban and industrial tracers compared to North Atlantic background air. Moreover, low mixing ratios and a good correlation between COS and CO2 showed a fingerprint of terrestrial uptake and minimal dilution during rapid transport over a 1–2 day time period. Analysis of synoptic conditions, backward trajectories, and photochemical aging estimates based on C3H8/C2H6 strongly suggested that elevated anthropogenic tracers in the upper troposphere of the flight region were the result of transport via convection and warm conveyor belt (WCB) uplifting of boundary layer air over the southeastern US. This mechanism is supported by the similar slope values of linear correlations between long-lived (months) anthropogenic tracers (e.g., C2Cl4 and CHCl3) from the flight region and the planetary boundary layer in the southeastern US. In addition, the aircraft measurements suggest that outflow from the US augmented the entire tropospheric column at mid-latitudes over the North Atlantic. Overall, the flight 13 data demonstrate a pervasive impact of US anthropogenic emissions on the troposphere over the North Atlantic.


2017 ◽  
Vol 30 (17) ◽  
pp. 6629-6643 ◽  
Author(s):  
Dachao Jin ◽  
Zhaoyong Guan

Using the NCEP–NCAR reanalysis and other observational datasets, the authors have investigated the relationship of summer rainfall variations between the Hetao region of northern China and the middle and lower reaches of Yangtze River (MLRYR). The results have demonstrated that rainfall in Hetao varies out of phase with that in MLRYR on the interannual time scales. This phenomenon is referred to as the Hetao–Yangtze rainfall seesaw (HYRS). An HYRS index is defined to reveal both spatial and temporal features of HYRS. It is found that the North Atlantic Oscillation (NAO) affects the HYRS. In years when the NAO is in its positive phase, anomalous divergences in the lower troposphere and anomalous convergences in the upper troposphere are observed in regions of the Mediterranean and eastern Europe. The anomalous convergences in the upper troposphere occur as the positive Rossby wave source excites a circumglobal teleconnection (CGT) in the midlatitudes, exhibiting the eastward propagation of Rossby wave energy along the Asian jet. Meanwhile, the Eurasian–Pacific (EUP) teleconnection also affects the HYRS. Influenced mainly by the CGT pattern, the circulations over Hetao and MLRYR are consequently perturbed. The atmosphere over Hetao converges anomalously in the lower troposphere and diverges anomalously in the upper troposphere, facilitating more than normal rainfall there. At the same time, the atmosphere over MLRYR diverges anomalously in the lower troposphere and converges anomalously in the upper troposphere, resulting in more than normal summer rainfall in MLRYR. In this way, the north–south rainfall seesaw is formed. This NAO-induced rainfall seesaw is potentially useful for summer rainfall predictions in both MLRYR and the Hetao region of northern China.


2018 ◽  
Author(s):  
Thorsten Kaluza ◽  
Daniel Kunkel ◽  
Peter Hoor

Abstract. The variability and similarities in the evolution of the tropopause inversion (TIL) layer during cyclongenesis in the North Atlantic storm track are investigated using operational meteorological analysis data (Integrated Forecast System from the European Centre for Medium-Range Weather Forecasts). For this a total amount of 130 cyclones have been analysed which evolved during the months August through October between 2010–2014 over the North Atlantic. Their paths of migration along with associated flow features in the upper troposphere/lower stratosphere (UTLS) have been tracked using the mean sea level pressure. Subsets of the 130 cyclones have been used for composite analysis using minimum sea level pressure to filter the cyclones based on their strength. The composite structure of the TIL strength distribution in connection with the overall UTLS flow strongly resembles the structure of the individual cyclones. Key results are that a strong dipole in tropopause inversion layer strength forms in regions of cyclonic wrap-up of UTLS air masses of different origin and isentropic potential vorticity. These air masses are associated with the cyclonic rotation of the underlaying cyclones. The maximum values of enhanced static stability above the tropopause occur north and northeast of the cyclone centre, vertically aligned with outflow regions of strong updraft and cloud formation up to the tropopause, which are situated in anticyclonic flow patterns in the upper troposphere. These regions are colocated with a maximum of vertical shear of the horizontal wind. The strong wind shear within the TIL results in a local minimum of Richardson numbers, representing the possibility for turbulent instability and potential mixing (or air mass exchange) within regions of enhanced static stability in the lowermost stratosphere.


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