NOx Background Mixing Ratios in Surface Air Over Europe and the Atlantic Ocean

Author(s):  
A. Broll ◽  
G. Helas ◽  
K.-J. Rumpel ◽  
P. Warneck
Keyword(s):  
2021 ◽  
Vol 21 (10) ◽  
pp. 8195-8211
Author(s):  
Ivan Tadic ◽  
Clara M. Nussbaumer ◽  
Birger Bohn ◽  
Hartwig Harder ◽  
Daniel Marno ◽  
...  

Abstract. Mechanisms of tropospheric ozone (O3) formation are generally well understood. However, studies reporting on net ozone production rates (NOPRs) directly derived from in situ observations are challenging and are sparse in number. To analyze the role of nitric oxide (NO) in net ozone production in the upper tropical troposphere above the Atlantic Ocean and western Africa, we present in situ trace gas observations obtained during the CAFE-Africa (Chemistry of the Atmosphere: Field Experiment in Africa) campaign in August and September 2018. The vertical profile of in situ measured NO along the flight tracks reveals lowest NO mixing ratios of less than 20 pptv between 2 and 8 km altitude and highest mixing ratios of 0.15–0.2 ppbv above 12 km altitude. Spatial distribution of tropospheric NO above 12 km altitude shows that the sporadically enhanced local mixing ratios (>0.4 ppbv) occur over western Africa, which we attribute to episodic lightning events. Measured O3 shows little variability in mixing ratios at 60–70 ppbv, with slightly decreasing and increasing tendencies towards the boundary layer and stratosphere, respectively. Concurrent measurements of CO, CH4, OH, HO2 and H2O enable calculations of NOPRs along the flight tracks and reveal net ozone destruction at −0.6 to −0.2 ppbv h−1 below 6 km altitude and balance of production and destruction around 7–8 km altitude. We report vertical average NOPRs of 0.2–0.4 ppbv h−1 above 12 km altitude with NOPRs occasionally larger than 0.5 ppbv h−1 over western Africa coincident with enhanced NO. We compare the observational results to simulated data retrieved from the general circulation model ECHAM/MESSy Atmospheric Chemistry (EMAC). Although the comparison of mean vertical profiles of NO and O3 indicates good agreement, local deviations between measured and modeled NO are substantial. The vertical tendencies in NOPRs calculated from simulated data largely reproduce those from in situ experimental data. However, the simulation results do not agree well with NOPRs over western Africa. Both measurements and simulations indicate that ozone formation in the upper tropical troposphere is NOx limited.


2011 ◽  
Vol 11 (14) ◽  
pp. 7375-7397 ◽  
Author(s):  
S.-H. Lee ◽  
S.-W. Kim ◽  
M. Trainer ◽  
G. J. Frost ◽  
S. A. McKeen ◽  
...  

Abstract. Transport and chemical transformation of well-defined New York City (NYC) urban plumes over the North Atlantic Ocean were studied using aircraft measurements collected on 20–21 July 2004 during the ICARTT (International Consortium for Atmospheric Research on Transport and Transformation) field campaign and WRF-Chem (Weather Research and Forecasting-Chemistry) model simulations. The strong NYC urban plumes were characterized by carbon monoxide (CO) mixing ratios of 350–400 parts per billion by volume (ppbv) and ozone (O3) levels of about 100 ppbv near New York City on 20 July in the WP-3D in-situ and DC-3 lidar aircraft measurements. On 21 July, the two aircraft captured strong urban plumes with about 350 ppbv CO and over 150 ppbv O3 (~160 ppbv maximum) about 600 km downwind of NYC over the North Atlantic Ocean. The measured urban plumes extended vertically up to about 2 km near New York City, but shrank to 1–1.5 km over the stable marine boundary layer (MBL) over the North Atlantic Ocean. The WRF-Chem model reproduced ozone formation processes, chemical characteristics, and meteorology of the measured urban plumes near New York City (20 July) and in the far downwind region over the North Atlantic Ocean (21 July). The quasi-Lagrangian analysis of transport and chemical transformation of the simulated NYC urban plumes using WRF-Chem results showed that the pollutants can be efficiently transported in (isentropic) layers in the lower atmosphere (<2–3 km) over the North Atlantic Ocean while maintaining a dynamic vertical decoupling by cessation of turbulence in the stable MBL. The O3 mixing ratio in the NYC urban plumes remained at 80–90 ppbv during nocturnal transport over the stable MBL, then grew to over 100 ppbv by daytime oxidation of nitrogen oxides (NOx = NO + NO2) with mixing ratios on the order of 1 ppbv. Efficient transport of reactive nitrogen species (NOy), specifically nitric acid (HNO3), was confirmed through the comparison of the CO/NOy ratio in photochemically fresh and aged NYC plumes, implying the possibility of long-range transport of O3 over the stable MBL over the North Atlantic Ocean in association with NOx regeneration mechanism. The impact of chemical initial and boundary conditions (IC/BCs) on modelled O3 urban plumes was investigated in terms of the background O3 level and the vertical structure of the urban plumes. Simulations with dynamic ("time-variant") chemical IC/BCs enhanced the O3 level by 2–12 ppbv on average in the atmospheric layer below 3 km, showing better agreement with the observed NYC plumes and biomass-burning plumes than the simulation with prescribed static IC/BCs. The simulation including MOZART-4 chemical IC/BCs and Alaskan/Canadian wildfire emissions compared better to the observed O3 profiles in the upper atmospheric layer (>~3 km) than models that only accounted for North American anthropogenic/biogenic and wildfire contributions to background ozone. The comparison between models and observations show that chemical IC/BCs must be properly specified to achieve accurate model results.


2006 ◽  
Vol 6 (12) ◽  
pp. 5435-5444 ◽  
Author(s):  
A. Pozzer ◽  
P. Jöckel ◽  
R. Sander ◽  
J. Williams ◽  
L. Ganzeveld ◽  
...  

Abstract. The new submodel AIRSEA for the Modular Earth Submodel System (MESSy) is presented. It calculates the exchange of chemical species between the ocean and the atmosphere with a focus on organic compounds. The submodel can be easily extended to a large number of tracers, including highly soluble ones. It is demonstrated that the application of explicitly calculated air-sea exchanges with AIRSEA can induce substantial changes in the simulated tracer distributions in the troposphere in comparison to a model setup in which this process is neglected. For example, the simulations of acetone, constrained with measured oceanic concentrations, shows relative changes in the atmospheric surface layer mixing ratios over the Atlantic Ocean of up to 300%.


2010 ◽  
Vol 10 (8) ◽  
pp. 3723-3741 ◽  
Author(s):  
J. Hegarty ◽  
H. Mao ◽  
R. Talbot

Abstract. The distributions of tropospheric ozone (O3) and carbon monoxide (CO), and the synoptic factors regulating these distributions over the western North Atlantic Ocean during winter and summer were investigated using profile retrievals from the Tropospheric Emission Spectrometer (TES) for 2004–2006. Seasonal composites of TES retrievals, reprocessed to remove the influence of the a priori on geographical and seasonal structure, exhibited strong seasonal differences. At the 681 hPa level during winter months of December, January and February (DJF) the composite O3 mixing ratios were uniformly low (~45 ppbv), but continental export was evident in a channel of enhanced CO (100–110 ppbv) flowing eastward from the US coast. In summer months June, July, and August (JJA) O3 mixing ratios were variable (45–65 ppbv) and generally higher due to increased photochemical production. The summer distribution also featured a channel of enhanced CO (95–105 ppbv) flowing northeastward around an anticyclone and exiting the continent over the Canadian Maritimes around 50° N. Offshore O3-CO slopes were generally 0.15–0.20 mol mol−1 in JJA, indicative of photochemical O3 production. Composites for 4 predominant synoptic patterns or map types in DJF suggested that export to the lower free troposphere (681 hPa level) was enhanced by the warm conveyor belt airstream of mid-latitude cyclones while stratospheric intrusions increased TES O3 levels at 316 hPa. A major finding in the DJF data was that offshore 681 hPa CO mixing ratios behind cold fronts could be enhanced up to >150 ppbv likely by lofting from the surface via shallow convection resulting from rapid destabilization of cold air flowing over much warmer ocean waters. In JJA composites for 3 map types showed that the general export pattern of the seasonal composites was associated with a synoptic pattern featuring the Bermuda High. However, weak cyclones and frontal troughs could enhance offshore 681 hPa CO mixing ratios to >110 ppbv with O3-CO slopes >0.50 mol mol−1 south of 45° N. Intense cyclones, which were not as common in the summer, enhanced export by lofting of boundary layer pollutants from over the US and also provided a possible mechanism for transporting pollutants from boreal fire outflow southward to the US east coast. Overall, for winter and summer the TES retrievals showed substantial evidence of air pollution export to the western North Atlantic Ocean with the most distinct differences in distribution patterns related to strong influences of mid-latitude cyclones in winter and the Bermuda High anticyclone in summer.


2003 ◽  
Vol 3 (2) ◽  
pp. 459-468 ◽  
Author(s):  
M. Traub ◽  
H. Fischer ◽  
M. de Reus ◽  
R. Kormann ◽  
H. Heland ◽  
...  

Abstract. During the Mediterranean Intensive Oxidant Study (MINOS) in August 2001 a total of 14 measurement flights were performed with the DLR Falcon jet aircraft from Heraklion, Crete. One objective of this campaign was to investigate the role of long-range transport of pollutants into the Mediterranean area. An analysis of 5-day back trajectories indicates that in the lower troposphere (0-4 km) air masses originated from eastern and western Europe, in the mid-troposphere (4-8 km) from the North Atlantic Ocean region and in the upper troposphere (8-14 km) from North Atlantic Ocean/North America (NANA) as well as South Asia. We allocated all back trajectories to clusters based on their ending height and source region. The mixing ratios of ozone, nitrogen oxide, total reactive oxidized nitrogen (NOy), formaldehyde, methanol, acetonitrile, acetone, peroxyacetyl nitrate (PAN), carbon dioxide, carbon monoxide and methane measured along the flight tracks are examined in relation to the different cluster trajectories. In the lower troposphere the mean trace gas mixing ratios of the eastern Europe cluster trajectories were significantly higher than those from western Europe. In the upper troposphere air from the NANA region seems to be influenced by the stratosphere, in addition, air masses were transported from South Asia, being influenced by strong convection in the Indian monsoon.


2021 ◽  
Vol 21 (22) ◽  
pp. 16689-16707
Author(s):  
Ju-Mee Ryoo ◽  
Leonhard Pfister ◽  
Rei Ueyama ◽  
Paquita Zuidema ◽  
Robert Wood ◽  
...  

Abstract. In 2016–2018, the ObseRvations of Aerosols above CLouds and their intEractionS (ORACLES) project undertook 3-month-long deployments to the southeastern (SE) Atlantic Ocean using research aircraft to better understand the impact of biomass burning (BB) aerosol transport to the SE Atlantic Ocean on climate. In this (part 1 of the meteorological overview) paper, the climatological features at monthly timescales are investigated. The southern African easterly jet (AEJ-S), defined as the zonal easterlies over 600–700 hPa exceeding 6 m s−1 around 5–15∘ S, is a characteristic feature of the mid-level circulation over southern Africa that was also during the deployment months of August 2017, September 2016, and October 2018. Climatologically, the AEJ-S develops at lower altitudes (∼ 3 km; 700 hPa) between 5–10∘ S in August, while it develops at around 4 km (∼ 600 hPa) and further south (5–15∘ S) in September and October, largely driven by the strong sensible heating over the African plateau. Notable meteorological anomalous characteristics during the 3 deployment months, compared to climatology (2000–2018), include the following: (1) during August 2017, the AEJ-S was weaker than the climatological mean, with an additional anomalous upper-level jet aloft (∼ 6 km) around 10∘ S. August 2017 was also drier over the SE Atlantic at 600–700 hPa than climatology, with a stronger Benguela low-level jet (LLJ) at 925–950 hPa along the Namibian coast of the SE Atlantic. Consistent with this, the southern Atlantic anticyclone was also stronger and closer to the coast than the August climatological mean. (2) During September 2016, the AEJ-S intensity was similar to the climatological mean, although the heat low and vertical motion over the land was slightly stronger compared to the September climatology. The LLJ and the large-scale southern Atlantic anticyclone were stronger than the climatological mean. (3) During October 2018, the AEJ-S was slightly weaker compared to the climatological mean, as was the LLJ and the southern Atlantic anticyclone. October 2018 was wetter over the Benguela coastal region at 600 hPa than the climatological mean. During all the deployment months, the sea surface temperatures (SST) over the SE Atlantic were warmer than the climatological means, but the monthly mean low cloud fraction was only noticeably reduced in August 2017. A weak August 2017 AEJ-S can explain low offshore black carbon (BC) mixing ratios within the European Centre for Medium-Range Weather Forecasts (ECMWF) Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, although the BC peak altitude, at 2–3 km, is below that of the AEJ-S. The upper-level wave disturbance and the associated anomalous circulation also explain the weakening of AEJ-S through the reduction of the strength of the heat low over the land during August 2017.


2006 ◽  
Vol 6 (4) ◽  
pp. 8189-8214
Author(s):  
A. Pozzer ◽  
P. Jöckel ◽  
R. Sander ◽  
L. Ganzeveld ◽  
J. Lelieveld

Abstract. The new submodel AIRSEA for the Modular Earth Submodel System (MESSy) is presented. It calculates the exchange of chemical species between the ocean and the atmosphere with a focus on organic compounds. The submodel can be easily extended to a large number of tracers, including highly soluble ones. It is demonstrated that application of explicitly calculated air-sea exchanges with AIRSEA can induce substantial changes in the simulated tracer distributions in the troposphere in comparison to a model version in which this process is neglected. For example, the simulations of acetone, constrained with measured oceanic concentrations, shows relative changes in the atmospheric surface layer mixing ratios over the Atlantic Ocean up to 300%.


2011 ◽  
Vol 11 (5) ◽  
pp. 14031-14089
Author(s):  
S.-H. Lee ◽  
S.-W. Kim ◽  
M. Trainer ◽  
G. J. Frost ◽  
S. A. McKeen ◽  
...  

Abstract. Transport and chemical transformation of well-defined New York City (NYC) urban plumes over the North Atlantic Ocean were studied using aircraft measurements collected on 20–21 July 2004 during the ICARTT (International Consortium for Atmospheric Research on Transport and Transformation) field campaign and WRF-Chem (Weather Research and Forecasting-Chemistry) model simulations. The strong NYC urban plumes were characterized by carbon monoxide (CO) mixing ratios of 350–400 parts per billion by volume (ppbv) and ozone (O3) levels of about 100 ppbv near New York City on 20 July in the WP-3D in-situ and DC-3 lidar aircraft measurements. On 21 July, the two aircraft captured strong urban plumes with about 350 ppbv CO and over 150 ppbv O3 (~160 ppbv maximum) about 600 km downwind of NYC over the North Atlantic Ocean. The measured urban plumes extended vertically up to about 2 km near New York City, but shrank to 1–1.5 km over the stable marine boundary layer (MBL) over the North Atlantic Ocean. The WRF-Chem model reproduced ozone formation processes, chemical characteristics, and meteorology of the measured urban plumes near New York City (20 July) and in the far downwind region over the North Atlantic Ocean (21 July). The quasi-Lagrangian analysis of transport and chemical transformation of the simulated NYC urban plumes using WRF-Chem results showed that the pollutants can be efficiently transported in (isentropic) layers in the lower atmosphere (<2–3 km) over the North Atlantic Ocean while maintaining a dynamic vertical decoupling by cessation of turbulence in the stable MBL. The O3 mixing ratio in the NYC urban plumes remained at 80–90 ppbv during nocturnal transport over the stable MBL, then grew to over 100 ppbv by daytime oxidation of nitrogen oxides (NOx = NO + NO2) with mixing ratios on the order of 1 ppbv. Efficient transport of reactive nitrogen species (NOy), specifically nitric acid (HNO3), was confirmed through the comparison of the CO/NOy ratio in photochemically fresh and aged NYC plumes, implying the possibility of long-range transport of O3 over the stable MBL over the North Atlantic Ocean in association with NOx regeneration mechanism. The impact of chemical initial and boundary conditions (IC/BCs) on modelled O3 urban plumes was investigated in terms of the background O3 level and the vertical structure of the urban plumes. Simulations with dynamic chemical IC/BCs enhanced the O3 level by 2–12 ppbv on average in the atmospheric layer below 3 km, showing better agreement with the observed NYC plumes and biomass-burning plumes than the simulation with prescribed static IC/BCs. The simulation including MOZART-4 chemical IC/BCs and Alaskan/Canadian wildfire emissions compared better to the observed O3 profiles in the upper atmospheric layer (>~3 km) than models that only accounted for North American anthropogenic/biogenic and wildfire contributions to background ozone. The comparison between models and observations show that chemical IC/BCs must be properly specified to achieve accurate model results.


2013 ◽  
Vol 13 (13) ◽  
pp. 6345-6357 ◽  
Author(s):  
S. Fuhlbrügge ◽  
K. Krüger ◽  
B. Quack ◽  
E. Atlas ◽  
H. Hepach ◽  
...  

Abstract. During the DRIVE~(Diurnal and Regional Variability of Halogen Emissions) ship campaign we investigated the variability of the halogenated very short-lived substances (VSLS) bromoform (CHBr3), dibromomethane (CH2Br2) and methyl iodide (CH3I) in the marine atmospheric boundary layer in the eastern tropical and subtropical North Atlantic Ocean during May/June 2010. The highest VSLS mixing ratios were found near the Mauritanian coast and close to Lisbon (Portugal). With backward trajectories we identified predominantly air masses from the open North Atlantic with some coastal influence in the Mauritanian upwelling area, due to the prevailing NW winds. The maximum VSLS mixing ratios above the Mauritanian upwelling were 8.92 ppt for bromoform, 3.14 ppt for dibromomethane and 3.29 ppt for methyl iodide, with an observed maximum range of the daily mean up to 50% for bromoform, 26% for dibromomethane and 56% for methyl iodide. The influence of various meteorological parameters – such as wind, surface air pressure, surface air and surface water temperature, humidity and marine atmospheric boundary layer (MABL) height – on VSLS concentrations and fluxes was investigated. The strongest relationship was found between the MABL height and bromoform, dibromomethane and methyl iodide abundances. Lowest MABL heights above the Mauritanian upwelling area coincide with highest VSLS mixing ratios and vice versa above the open ocean. Significant high anti-correlations confirm this relationship for the whole cruise. We conclude that especially above oceanic upwelling systems, in addition to sea–air fluxes, MABL height variations can influence atmospheric VSLS mixing ratios, occasionally leading to elevated atmospheric abundances. This may add to the postulated missing VSLS sources in the Mauritanian upwelling region (Quack et al., 2007).


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