Airborne Measurements of Trace Organic Species in the Upper Troposphere Over Europe: the Impact of Deep Convection

2006 ◽  
Vol 3 (4) ◽  
pp. 244 ◽  
Author(s):  
Aurélie Colomb ◽  
Jonathan Williams ◽  
John Crowley ◽  
Valérie Gros ◽  
Rolf Hofmann ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Deep Convection ◽  
Trace Gases ◽  
Upper Troposphere ◽  
Airborne Measurements ◽  
Organic Species ◽  
Mixing Ratios ◽  
Benzene Toluene ◽  
The Impact ◽  
Organic Trace

Environmental Context. In the upper troposphere, sources of HOx such as acetone, peroxides, and aldehydes can play an important role in governing the production and destruction of ozone. Convection (over both land and sea) carries gases that can contribute to increased levels of HOx to the upper troposphere. The chemical impact of convection on the continental upper troposphere over Europe is studied by sampling the upper troposphere. Mass spectrometry techniques are used to analyze the collected samples. Such a study should aid in understanding the impact meteorological events have on atmospheric chemistry. Abstract. The volume mixing ratios of several organic trace gases and ozone (O3) were measured in the upper troposphere over Europe during the UTOPIHAN-ACT aircraft campaign in July 2003. The organic trace gases included alkanes, isoprene, aromatics, iodomethane, and trichloroethylene, oxygenates such as acetone, methanol, formaldehyde, carbon monoxide, and longer-lived tracer species such as chlorofluorocarbons and halochloroflurocarbons. The aim of the UTOPIHAN-ACT project was to study the chemical impact of deep convection on the continental upper troposphere. A Lear Jet aircraft, based in Germany, was flown at heights between 6 and 13 km in the region 59°N–42°N to 7°W–13°E during July 2003. Overall, the convectively influenced measurements presented here show a weaker variability lifetime dependence of trace gases than similar measurements collected over the Mediterranean region under more stable high-pressure conditions. Several cases of convective outflow are identified by the elevated mixing ratios of organic species relative to quiescent background conditions, with both biogenic and anthropogenic influences detectable in the upper troposphere. Enhancement at higher altitudes, notably of species with relatively short chemical lifetimes such as benzene, toluene, and even isoprene indicates deep convection over short timescales during summertime. The impact of deep convection on the local upper tropospheric formaldehyde and HOx budgets is assessed.

scholarly journals Uncertainties in atmospheric chemistry modelling due to convection parameterisations and subsequent scavenging

2010 ◽  
Vol 10 (4) ◽  
pp. 1931-1951 ◽  
Author(s):  
H. Tost ◽  
M. G. Lawrence ◽  
C. Brühl ◽  
P. Jöckel ◽  
◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Model Simulation ◽  
Chemical Reactivity ◽  
Deep Convection ◽  
Trace Gases ◽  
Convective Transport ◽  
Moist Convection ◽  
Tracer Transport ◽  
Convection Schemes ◽  
The Impact

Abstract. Moist convection in global modelling contributes significantly to the transport of energy, momentum, water and trace gases and aerosols within the troposphere. Since convective clouds are on a scale too small to be resolved in a global model their effects have to be parameterised. However, the whole process of moist convection and especially its parameterisations are associated with uncertainties. In contrast to previous studies on the impact of convection on trace gases, which had commonly neglected the convective transport for some or all compounds, we investigate this issue by examining simulations with five different convection schemes. This permits an uncertainty analysis due to the process formulation, without the inconsistencies inherent in entirely neglecting deep convection or convective tracer transport for one or more tracers. Both the simulated mass fluxes and tracer distributions are analysed. Investigating the distributions of compounds with different characteristics, e.g., lifetime, chemical reactivity, solubility and source distributions, some differences can be attributed directly to the transport of these compounds, whereas others are more related to indirect effects, such as the transport of precursors, chemical reactivity in certain regions, and sink processes. The model simulation data are compared with the average regional profiles of several measurement campaigns, and in detail with two campaigns in fall and winter 2005 in Suriname and Australia, respectively. The shorter-lived a compound is, the larger the differences and consequently the uncertainty due to the convection parameterisation are, as long as it is not completely controlled by local production that is independent of convection and its impacts (e.g. water vapour changes). Whereas for long-lived compounds like CO or O3 the mean differences between the simulations are less than 25%), differences for short-lived compounds reach up to ±100% with different convection schemes. A rating of an overall "best" performing scheme is difficult, since the optimal performance depends on the region and compound.

scholarly journals HO<sub>x</sub> measurements in the summertime upper troposphere over Europe: a comparison of observations to a box model and a 3-D model

2012 ◽  
Vol 12 (11) ◽  
pp. 30619-30660 ◽  
Author(s):  
E. Regelin ◽  
H. Harder ◽  
M. Martinez ◽  
D. Kubistin ◽  
C. Tatum Ernest ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Circulation Model ◽  
Box Model ◽  
Measurement Unit ◽  
Data Set ◽  
Upper Troposphere ◽  
Sources And Sinks ◽  
Airborne Measurements ◽  
Mixing Ratios

Abstract. In-situ airborne measurements of OH and HO2 with the HORUS (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy) instrument were performed in the summertime upper troposphere across Europe during the HOOVER 2 (HOx OVer EuRope) campaign in July 2007. Complementary measurements of trace gas species and photolysis frequencies were conducted to obtain a broad data set, which has been used to quantify the significant HOx sources and sinks. In this study we compare the in-situ measurement of OH and HO2 with simulated mixing ratios from the constrained box model CAABA/MECCA (Chemistry As A Box Model Application/Module Efficiently Calculating the Chemistry of the Atmosphere), and the global circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry Model). The constrained box model reproduces the observed OH and HO2 mixing ratios with better agreement (obs/mod median 98% OH, 96% HO2) than the global model (median 76% OH, 59% HO2). The observations and the computed HOx sources and sinks are used to identify deviations between the models and their impacts on the calculated HOx budget.

scholarly journals HOx measurements in the summertime upper troposphere over Europe: a comparison of observations to a box model and a 3-D model

2013 ◽  
Vol 13 (21) ◽  
pp. 10703-10720 ◽  
Author(s):  
E. Regelin ◽  
H. Harder ◽  
M. Martinez ◽  
D. Kubistin ◽  
C. Tatum Ernest ◽  
...  
Keyword(s):  
Atmospheric Chemistry ◽  
Circulation Model ◽  
Box Model ◽  
Measurement Unit ◽  
Data Set ◽  
Upper Troposphere ◽  
Sources And Sinks ◽  
Airborne Measurements ◽  
Mixing Ratios

Abstract. In situ airborne measurements of OH and HO2 with the HORUS (HydrOxyl Radical measurement Unit based on fluorescence Spectroscopy) instrument were performed in the summertime upper troposphere across Europe during the HOOVER 2 (HOx OVer EuRope) campaign in July 2007. Complementary measurements of trace gas species and photolysis frequencies were conducted to obtain a broad data set, which has been used to quantify the significant HOx sources and sinks. In this study we compare the in situ measurement of OH and HO2 with simulated mixing ratios from the constrained box model CAABA/MECCA (Chemistry As A Box Model Application/Module Efficiently Calculating the Chemistry of the Atmosphere), and the global circulation model EMAC (ECHAM5/MESSy Atmospheric Chemistry Model). The constrained box model reproduces the observed OH and HO2 mixing ratios with better agreement (obs/mod median 98% OH, 96% HO2) than the global model (median 76% OH, 59% HO2). The observations and the computed HOx sources and sinks are used to identify deviations between the models and their impacts on the calculated HOx budget.

scholarly journals The impact of biomass burning on upper tropospheric carbon monoxide: A study using MOCAGE global model and IAGOS airborne data

2020 ◽  
Author(s):  
Martin Cussac ◽  
Virginie Marécal ◽  
Valérie Thouret ◽  
Béatrice Josse ◽  
Bastien Sauvage
Keyword(s):  
Carbon Monoxide ◽  
Biomass Burning ◽  
Boreal Forests ◽  
Transport Model ◽  
Deep Convection ◽  
High Latitudes ◽  
Upper Troposphere ◽  
Airborne Measurements ◽  
Fire Plumes ◽  
The Impact

Abstract. In this paper the fate of biomass burning emissions of carbon monoxide is studied with the global chemistry transport model MOCAGE and IAGOS airborne measurements for the year of 2013. The objectives are firstly to improve their representation within the model and secondly to analyse their contribution to carbon monoxide concentrations in the upper troposphere. At first, a new implementation of biomass burning injection is developed for MOCAGE, using the latest products available in GFAS biomass burning inventory on plume altitude and injection height. This method is validated against IAGOS observations of CO made in fire plumes, identified thanks to the SOFT-IO source attribution data. The use of these GFAS products lead to improved MOCAGE skill to simulate fire plumes originating from boreal forests wildfires. It was also shown that this new biomass burning injection method did not change upper tropospheric carbon monoxide concentrations elsewhere on the globe as the previous one was already satisfying. Then, MOCAGE performances were evaluated in general in the upper troposphere in comparison to the IAGOS database, and were shown to be very good, with very little bias and good correlations between the model and the observations. Finally, we analyse the contribution of biomass burning to upper tropospheric carbon monoxide concentrations. This was done by comparing simulations were biomass were toggled on and off in different source regions of the world to assess their individual influence. The two regions contributing the most to upper tropospheric CO were found to be the boreal forests and equatorial Africa, in accordance with the quantities of CO they emit each year and the fact that they undergo fast vertical transport: deep convection in the tropics and pyroconvection at high latitudes. It was found that biomass burning contributes for more than 11 % on average on the CO concentrations in the upper troposphere, and up to 50 % at high latitudes during the wildfire season.

scholarly journals Cloud-scale modelling of the impact of deep convection on the fate of oceanic bromoform in the troposphere: a case study over the west coast of Borneo

2020 ◽  
Author(s):  
Paul D. Hamer ◽  
Virginie Marécal ◽  
Ryan Hossaini ◽  
Michel Pirre ◽  
Gisèle Krysztofiak ◽  
...  
Keyword(s):  
Boundary Layer ◽  
West Coast ◽  
Deep Convection ◽  
Convective System ◽  
The West ◽  
Upper Troposphere ◽  
Convective Systems ◽  
Mixing Ratios ◽  
The Impact

Abstract. Coastal oceans emit bromoform (CHBr3) that can be transported rapidly to the upper troposphere by deep convection. In the troposphere, the spatial and vertical distribution of CHBr3 and its product gases (PGs) depend on emissions, chemical processing, transport by large scale flow, convection, and associated washout. This paper presents a modelling study on the fate of CHBr3 and its PGs in the troposphere. A case study at cloud scale was conducted along the west coast of Borneo, when several deep convective systems triggered in the afternoon and early evening of November 19th 2011. These systems were sampled by the Falcon aircraft during the field campaign of the SHIVA project. We analyse these systems using a simulation with the cloud-resolving meteorological model C-CATT-BRAMS at 2 × 2 km resolution that describes transport, photochemistry, and washout of CHBr3. We find that simulated CHBr3 mixing ratios and the observed values in the boundary layer and the outflow of the convective systems agree. However, the model underestimates the background CHBr3 mixing ratios in the upper troposphere, which suggests a missing source. An analysis of the simulated chemical speciation of bromine within and around each simulated convective system during the mature convective stage reveals that > 85 % of the bromine derived from CHBr3 and its PGs is transported vertically to the point of convective detrainment in the form of CHBr3 and that the remaining small fraction is in the form of organic PGs, principally insoluble brominated carbonyls produced from the photo-oxidation of CHBr3. The model simulates that within the boundary layer and free troposphere, the inorganic PGs are only present in soluble forms, i.e., HBr, HOBr, and BrONO2, and consequently, within the convective clouds, the inorganic PGs are almost entirely removed by wet scavenging. For the conditions of the simulated case study Br2 plays no significant role in the vertical transport of bromine. This likely results from the small simulated quantities of inorganic bromine involved, the presence of HBr in large excess compared to HOBr and the less soluble BrO, and the relatively quick removal of soluble compounds within the convective column. This prevalence of HBr is a result of the wider simulated regional atmospheric composition whereby background tropospheric ozone levels are exceptionally low.

scholarly journals Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere

2011 ◽  
Vol 11 (1) ◽  
pp. 121-162 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini
Keyword(s):  
Lower Stratosphere ◽  
Transport Model ◽  
Deep Convection ◽  
Three Dimensional ◽  
Convective Activity ◽  
Chemical Transport Model ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Entire Amount ◽  
The Impact

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.

scholarly journals Impact of deep convection and dehydration on bromine loading in the upper troposphere and lower stratosphere

2011 ◽  
Vol 11 (6) ◽  
pp. 2671-2687 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini
Keyword(s):  
Lower Stratosphere ◽  
Transport Model ◽  
Deep Convection ◽  
Three Dimensional ◽  
Convective Activity ◽  
Chemical Transport Model ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Entire Amount ◽  
The Impact

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform convective detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.

scholarly journals The impact of biomass burning on upper tropospheric carbon monoxide: a study using MOCAGE global model and IAGOS airborne data

2020 ◽  
Vol 20 (15) ◽  
pp. 9393-9417
Author(s):  
Martin Cussac ◽  
Virginie Marécal ◽  
Valérie Thouret ◽  
Béatrice Josse ◽  
Bastien Sauvage
Keyword(s):  
Carbon Monoxide ◽  
Biomass Burning ◽  
Boreal Forests ◽  
Transport Model ◽  
Deep Convection ◽  
High Latitudes ◽  
Upper Troposphere ◽  
Airborne Measurements ◽  
Fire Plumes ◽  
The Impact

Abstract. In this paper, the fate of biomass burning emissions of carbon monoxide is studied with the global chemistry–transport model MOCAGE (MOdélisation de Chimie Atmosphérique à Grande Échelle) and IAGOS (In-Service Aircraft for a Global Observing System) airborne measurements for the year 2013. The objectives are firstly to improve their representation within the model and secondly to analyse their contribution to carbon monoxide concentrations in the upper troposphere. At first, a new implementation of biomass burning injection is developed for MOCAGE, using the latest products available in Global Fire Assimilation System (GFAS) biomass burning inventory on plume altitude and injection height. This method is validated against IAGOS observations of CO made in fire plumes, identified thanks to the SOFT-IO source attribution data. The use of these GFAS products leads to improved MOCAGE skill to simulate fire plumes originating from boreal forest wildfires. It is also shown that this new biomass burning injection method modifies the distribution of carbon monoxide in the free and upper troposphere, mostly at northern boreal latitudes. Then, MOCAGE performance is evaluated in general in the upper troposphere and lower stratosphere in comparison to the IAGOS observations and is shown to be very good, with very low bias and good correlations between the model and the observations. Finally, we analyse the contribution of biomass burning to upper tropospheric carbon monoxide concentrations. This is done by comparing simulations where biomass are toggled on and off in different source regions of the world to assess their individual influence. The two regions contributing the most to upper tropospheric CO are found to be the boreal forests and equatorial Africa, in accordance with the quantities of CO they emit each year and the fact that they undergo fast vertical transport: deep convection in the tropics and pyroconvection at high latitudes. It is also found that biomass burning contributes more than 11 % on average to the CO concentrations in the upper troposphere and up to 50 % at high latitudes during the wildfire season.

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 Modelling marine emissions and atmospheric distributions of halocarbons and DMS: the influence of prescribed water concentration vs. prescribed emissions

2015 ◽  
Vol 15 (12) ◽  
pp. 17553-17598
Author(s):  
S. T. Lennartz ◽  
G. Krysztofiak-Tong ◽  
C. A. Marandino ◽  
B.-M. Sinnhuber ◽  
S. Tegtmeier ◽  
...  
Keyword(s):  
Wind Speed ◽  
Atmospheric Chemistry ◽  
Climate Model ◽  
Trace Gases ◽  
Surface Wind ◽  
Water Concentration ◽  
Absolute Magnitude ◽  
Actual State ◽  
Transfer Velocity ◽  
Mixing Ratios

Abstract. Marine produced short-lived trace gases such as dibromomethane (CH2Br2), bromoform (CHBr3), methyliodide (CH3I) and dimethylsulfide (DMS) significantly impact tropospheric and stratospheric chemistry. Describing their marine emissions in atmospheric chemistry models as accurately as possible is necessary to quantify their impact on ozone depletion and the Earth's radiative budget. So far, marine emissions of trace gases have mainly been prescribed from emission climatologies, thus lacking the interaction between the actual state of the atmosphere and the ocean. Here we present simulations with the chemistry climate model EMAC with online calculation of emissions based on surface water concentrations, in contrast to directly prescribed emissions. Considering the actual state of the model atmosphere results in a concentration gradient consistent with model real-time conditions at ocean surface and atmosphere, which determine the direction and magnitude of the computed flux. This method has a number of conceptual and practical benefits, as the modelled emission can respond consistently to changes in sea surface temperature, surface wind speed, sea ice cover and especially atmospheric mixing ratio. This online calculation could enhance, dampen or even invert the fluxes (i.e. deposition instead of emissions) of VSLS. We show that differences between prescribing emissions and prescribing concentrations (−28 % for CH2Br2 to +11 % for CHBr3) result mainly from consideration of the actual, time-varying state of the atmosphere. The absolute magnitude of the differences depends mainly on the surface ocean saturation of each particular gas. Comparison to observations from aircraft, ships and ground stations reveals that computing the air–sea flux interactively leads in most of the cases to more accurate atmospheric mixing ratios in the model compared to the computation from prescribed emissions. Calculating emissions online also enables effective testing of different air–sea transfer velocity parameterizations k, which was performed here for eight different parameterizations. The testing of these different k values is of special interest for DMS, as recently published parameterizations derived by direct flux measurements using eddy covariance measurements suggest decreasing k values at high wind speeds or a linear relationship with wind speed. Implementing these parameterizations reduces discrepancies in modelled DMS atmospheric mixing ratios and observations by a factor of 1.5 compared to parameterizations with a quadratic or cubic relationship to wind speed.

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