scholarly journals Long-path averaged mixing ratios of O<sub>3</sub> and NO<sub>2</sub> in the free troposphere from mountain MAX-DOAS

2014 ◽  
Vol 7 (10) ◽  
pp. 3373-3386 ◽  
Author(s):  
L. Gomez ◽  
M. Navarro-Comas ◽  
O. Puentedura ◽  
Y. Gonzalez ◽  
E. Cuevas ◽  
...  
Keyword(s):  
Optical Absorption Spectroscopy ◽  
High Mountain ◽  
Geometrical Approach ◽  
Free Troposphere ◽  
Simple Method ◽  
Air Masses ◽  
Mixing Ratios ◽  
Horizontal Path ◽  
Low Concentrations

Abstract. A new approximation is proposed to estimate O3 and NO2 mixing ratios in the northern subtropical free troposphere (FT). The proposed method uses O4 slant column densities (SCDs) at horizontal and near-zenith geometries to estimate a station-level differential path. The modified geometrical approach (MGA) is a simple method that takes advantage of a very long horizontal path to retrieve mixing ratios in the range of a few pptv. The methodology is presented, and the possible limitations are discussed. Multi-axis differential optical absorption spectroscopy (MAX-DOAS) high-mountain measurements recorded at the Izaña observatory (28° 18' N, 16° 29' W) are used in this study. The results show that under low aerosol loading, O3 and NO2 mixing ratios can be retrieved even at very low concentrations. The obtained mixing ratios are compared with those provided by in situ instrumentation at the observatory. The MGA reproduces the O3 mixing ratio measured by the in situ instrumentation with a difference of 28%. The different air masses scanned by each instrument are identified as a cause of the discrepancy between the O3 observed by MAX-DOAS and the in situ measurements. The NO2 is in the range of 20–40 ppt, which is below the detection limit of the in situ instrumentation, but it is in agreement with measurements from previous studies for similar conditions.

scholarly journals Long-path averaged mixing ratios of O<sub>3</sub> and NO<sub>2</sub> in the free troposphere from mountain MAX-DOAS

2013 ◽  
Vol 6 (5) ◽  
pp. 8235-8267
Author(s):  
L. Gomez ◽  
M. Navarro-Comas ◽  
O. Puentedura ◽  
Y. Gonzalez ◽  
E. Cuevas ◽  
...  
Keyword(s):  
Detection Limit ◽  
Optical Absorption ◽  
Radiative Transfer Model ◽  
Optical Absorption Spectroscopy ◽  
Transfer Model ◽  
High Mountain ◽  
Free Troposphere ◽  
Air Masses ◽  
Mixing Ratios

Abstract. A new approximation is proposed to estimate O3 and NO2 mixing ratios in the Northern Subtropics Free Troposphere (FT). Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) high mountain measurements, recorded at Izaña Observatory (28°18' N, 16°29' W), are used in this work. Proposed method uses horizontal and near-zenith geometries to estimate the station level differential path. Two different methods are described. First one uses retrieved Slant Column Densities (SCD) of O4. On second method, path is estimated from LIBRADTRAN radiative transfer model for the region and season. Results show that under low aerosol loading, O3 and NO2 mixing ratios concentrations can be retrieved with moderately low errors. Obtained concentrations have been compared with in situ instrumentation on the observatory. O3 concentration in FT is found to be in the range of 40–80 ppb, approximately. NO2 is in the range of 20–30 ppt, below the detection limit of in situ instrumentation. The different air masses scanned by each instrument have been identified as a cause of discrepancy between O3 observed by MAX-DOAS and in situ.

scholarly journals NO<sub>2</sub> seasonal evolution in the North Subtropical free troposphere

2015 ◽  
Vol 15 (10) ◽  
pp. 14473-14504
Author(s):  
M. Gil-Ojeda ◽  
M. Navarro-Comas ◽  
L. Gómez-Martín ◽  
J. A. Adame ◽  
A. Saiz-Lopez ◽  
...  
Keyword(s):  
Optical Absorption Spectroscopy ◽  
High Mountain ◽  
Horizontal Line ◽  
Free Troposphere ◽  
Seasonal Evolution ◽  
The North ◽  
Measuring Period ◽  
The Impact ◽  
Pollution Events

Abstract. Three years of Multi-Axis Differential Optical Absorption Spectroscopy (MAXDOAS) measurements (2011–2013) have been used for estimating the NO2 mixing ratio along a horizontal line of sight from the high mountain Subtropical observatory of Izaña, at 2370 m a.s.l. (NDACC station, 28.3° N, 16.5° W). The method is based on horizontal path calculation from the O2–O2 collisional complex at the 477 nm absorption band which is measured simultaneously to the NO2, and is applicable under low aerosols loading conditions. The MAXDOAS technique, applied in horizontal mode in the free troposphere, minimizes the impact of the NO2 contamination resulting from the arrival of MBL airmasses from thermally forced upwelling breeze during central hours of the day. Comparisons with in-situ observations show that during most of measuring period the MAXDOAS is insensitive or very little sensitive to the upwelling breeze. Exceptions are found during pollution events under southern wind conditions. On these occasions, evidence of fast efficient and irreversible transport from the surface to the free troposphere is found. Background NO2 vmr, representative of the remote free troposphere, are in the range of 20–45 pptv. The observed seasonal evolution shows an annual wave where the peak is in phase with the solar radiation. Model simulations with the chemistry-climate CAM-Chem model are in good agreement with the NO2 measurements, and are used to further investigate the possible drivers of the NO2 seasonality observed at Izaña.

Aircraft measurements of nitrous acid in excess of model predictions in the boundary layer and free troposphere

2020 ◽  
Author(s):  
Benjamin Schreiner ◽  
Klaus Pfeilsticker ◽  
Flora Kluge ◽  
Meike Rotermund ◽  
Andreas Zahn ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Optical Absorption Spectroscopy ◽  
Free Troposphere ◽  
Aerosol Composition ◽  
Transport And Transformation ◽  
Air Masses ◽  
Airborne Measurements ◽  
Photolysis Frequencies ◽  
Model Predictions

&lt;p&gt;Middle and long-term &amp;#160;photo-chemical effects of local and regional pollution are not well quantified and are an area of active study. NO&lt;sub&gt;x&lt;/sub&gt; (here defined as NO, NO&lt;sub&gt;2&lt;/sub&gt;, and HONO) is a regional pollutant, which influences atmospheric oxidation capacity and ozone formation. Airborne measurements of atmospheric trace gases from the HALO (High Altitude Long Range) aircraft, particularly of NO, NO&lt;sub&gt;2&lt;/sub&gt;, and HONO were performed as part of the EMeRGe (Effect of Megacities on the Transport and Transformation of Pollutants on the Regional to Global Scales) campaign over continental Europe and southeast Asia in July 2017 and April 2018, respectively. NO (and NO&lt;sub&gt;Y&lt;/sub&gt;), O&lt;sub&gt;3&lt;/sub&gt;, and the photolysis frequencies of NO&lt;sub&gt;2&lt;/sub&gt; and HONO were measured in-situ. NO&lt;sub&gt;2&lt;/sub&gt; and HONO were inferred from Limb measurements of the mini-DOAS (Differential Optical Absorption Spectroscopy) instrument, using the novel scaling method (H&amp;#252;neke et al., 2017). These measurements were compared with simulations of the MECO/EMAC models. In relatively polluted air-masses in the boundary layer and free troposphere, HONO measured in excess of model predictions (and previous measurements) suggests an in-situ formation and a significant source of OH as well as a pathway for re-noxification. Aerosol composition simultaneously measured &amp;#160;by the C-Tof-AMS instrument may reveal potential reaction mechanisms to explain the discrepancy.&amp;#160;&lt;/p&gt;

scholarly journals Origins and characterization of CO and O<sub>3</sub> in the African upper troposphere

2021 ◽  
Author(s):  
Victor Lannuque ◽  
Bastien Sauvage ◽  
Brice Barret ◽  
Hannah Clark ◽  
Gilles Athier ◽  
...  
Keyword(s):  
Wind Shear ◽  
Asian Monsoon ◽  
Shear Zones ◽  
Hadley Cell ◽  
Trade Winds ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
Hadley Cells

Abstract. Between December 2005 and 2013, the In-service Aircraft for a Global Observing System (IAGOS) program produced almost daily in situ measurements of CO and O3 between Europe and southern Africa. IAGOS data combined with measurements from the IASI instrument onboard the Metop-A satellite (2008–2013) are used to characterize meridional distributions and seasonality of CO and O3 in the African upper troposphere (UT). The FLEXPART particle dispersion model and the SOFT-IO model which combines the FLEXPART model with CO emission inventories are used to explore the sources and origins of the observed transects of CO and O3. We focus our analysis on two main seasons: December to March (DJFM) and June to October (JJASO). These seasons have been defined according to the position of Intertropical Convergence Zone (ITCZ), determined using in situ measurements from IAGOS. During both seasons, the UT CO meridional transects are characterized by maximum mixing ratios located 10° from the position of the ITCZ above the dry regions inside the hemisphere of the strongest Hadley cell (132 to 165 ppb at 0–5° N in DJFM and 128 to 149 ppb at 3–7° S in JJASO), and decreasing values south- and north-ward. The O3 meridional transects are characterized by mixing ratio minima of ~ 42–54 ppb at the ITCZ (10–16° S in DJFM and 5–8° N in JJASO) framed by local maxima (~ 53–71 ppb) coincident with the wind shear zones North and South of the ITCZ. O3 gradients are strongest in the hemisphere of the strongest Hadley cell. IASI UT O3 distributions in DJFM have revealed that the maxima are a part of a crescent-shaped O3 plume above the Atlantic Ocean around the Gulf of Guinea. CO emitted at the surface is transported towards the ITCZ by the trade winds and then convectively uplifted. Once in the upper troposphere, CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maximum CO mixing ratios are found. Anthropogenic and fires both contribute, by the same order of magnitude, to the CO budget of the African upper troposphere. Local fires have the highest contribution, drive the location of the observed UT CO maxima, and are related to the following transport pathway: CO emitted at the surface is transported towards the ITCZ by the trade winds and further convectively uplifted. Then UT CO enriched air masses are transported away from the ITCZ by the upper branches of the Hadley cells and accumulate within the zonal wind shear zones where the maxima are located. Anthropogenic CO contribution is mostly from Africa during the entire year, with a low seasonal variability, and is related to similar transport circulation than fire air masses. There is also a large contribution from Asia in JJASO related to the fast convective uplift of polluted air masses in the Asian monsoon region which are further westward transported by the tropical easterly jet (TEJ) and the Asian monsoon anticyclone (AMA). O3 minima correspond to air masses that were recently uplifted from the surface where mixing ratios are low at the ITCZ. The O3 maxima correspond to old high altitude air masses uplifted from either local or long distance area of high O3 precursor emissions (Africa and South America during all the year, South Asia mainly in JJASO), and must be created during transport by photochemistry. This analysis of meridional transects contribute to a better understanding of distributions of CO and O3 in the intertropical African upper troposphere and the processes which drive these distributions. Therefore, it provides a solid basis for comparison and improvement of models and satellite products in order to get the good O3 for the good reasons.

scholarly journals Vertical profiles of NO<sub>2</sub>, SO<sub>2</sub>, HONO, HCHO, CHOCHO, and aerosols derived from MAX-DOAS measurements at a rural site in the central-western North China Plain and their relation to emission sources and effects of regional transport

2018 ◽  
Author(s):  
Yang Wang ◽  
Steffen Dörner ◽  
Sebastian Donner ◽  
Sebastian Böhnke ◽  
Isabelle De Smedt ◽  
...  
Keyword(s):  
Trace Gases ◽  
Rural Site ◽  
Optical Absorption Spectroscopy ◽  
Vertical Profiles ◽  
Regional Transport ◽  
Near Surface ◽  
North West ◽  
Mixing Ratios ◽  
Chemistry Research

Abstract. A Multi Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument was deployed in May and June 2016 at a monitoring station (37.18° N, 114.36° E) in the suburban area of Xingtai (one of the most polluted cities in China) during the Atmosphere-Aerosol-Boundary Layer-Cloud (A2BC) and Air chemistry Research In Asia (ARIAs) joint experiments to derive tropospheric vertical profiles of NO2, SO2, HONO, HCHO, CHOCHO and aerosols. Aerosol optical depths derived from MAX-DOAS were found to be consistent with collocated sun-photometer measurements. Also the derived near-surface aerosol extinction and HCHO mixing ratio agree well with coincident visibility meter and in situ HCHO measurements, with mean HCHO near-surface mixing ratios of ~ 3.5 ppb. Underestimates of MAX-DOAS results compared to in situ measurements of NO2 (~ 60 %), SO2 (~ 20 %) are found expectedly due to vertical and horizontal inhomogeneity of trace gases. Vertical profiles of aerosols and NO2, SO2 are reasonably consistent with those measured by a collocated Raman Lidar and aircraft spirals over the station. The deviations can be attributed to differences in sensitivity as a function of altitude and substantial horizontal gradients of pollutants. Aerosols, HCHO, and CHOCHO profiles typically extended to higher altitudes (with 75 % integrated column located below ~ 1.4 km) than did NO2, SO2, and HONO (with 75 % integrated column below ~ 0.5 km) under polluted condition. Lifted layers were systematically observed for all species, (except HONO), indicating accumulation, secondary formation, or long-range transport of the pollutants at higher altitudes. Maximum values routinely occurred in the morning for NO2, SO2, and HONO, but around noon for aerosols, HCHO, and CHOCHO, mainly dominated by photochemistry, characteristic upslope/downslope circulation and PBL dynamics. Significant day-to-day variations are found for all species due to the effect of regional transport and changes in synoptic pattern analysed with HYSPLIT trajectories. Low pollution was often observed for air masses from the north-west (behind cold fronts), and high pollution from the southern areas such as industrialized Wuan. The contribution of regional transport for the pollutants measured at the site during the observation period was estimated to be about 20 % to 30 % for trace gases, and about 50 % for aerosols. In addition, agricultural burning events impacted the day-to-day variations of HCHO, CHOCHO and aerosols.

scholarly journals Middle atmospheric water vapour and dynamics in the vicinity of the polar vortex during the Hygrosonde-2 campaign

2009 ◽  
Vol 9 (13) ◽  
pp. 4407-4417 ◽  
Author(s):  
S. Lossow ◽  
M. Khaplanov ◽  
J. Gumbel ◽  
J. Stegman ◽  
G. Witt ◽  
...  
Keyword(s):  
Water Vapour ◽  
Middle Atmosphere ◽  
Polar Vortex ◽  
The Arctic ◽  
Small Scale ◽  
Air Masses ◽  
Mixing Ratios ◽  
Water Vapour Concentration ◽  
Wind Shears

Abstract. The Hygrosonde-2 campaign took place on 16 December 2001 at Esrange/Sweden (68° N, 21° E) with the aim to investigate the small scale distribution of water vapour in the middle atmosphere in the vicinity of the Arctic polar vortex. In situ balloon and rocket-borne measurements of water vapour were performed by means of OH fluorescence hygrometry. The combined measurements yielded a high resolution water vapour profile up to an altitude of 75 km. Using the characteristic of water vapour being a dynamical tracer it was possible to directly relate the water vapour data to the location of the polar vortex edge, which separates air masses of different character inside and outside the polar vortex. The measurements probed extra-vortex air in the altitude range between 45 km and 60 km and vortex air elsewhere. Transitions between vortex and extra-vortex usually coincided with wind shears caused by gravity waves which advect air masses with different water vapour volume mixing ratios. From the combination of the results from the Hygrosonde-2 campaign and the first flight of the optical hygrometer in 1994 (Hygrosonde-1) a clear picture of the characteristic water vapour distribution inside and outside the polar vortex can be drawn. Systematic differences in the water vapour concentration between the inside and outside of the polar vortex can be observed all the way up into the mesosphere. It is also evident that in situ measurements with high spatial resolution are needed to fully account for the small-scale exchange processes in the polar winter middle atmosphere.

The Airyx 2D SkySpec instrument: MAX-DOAS measurements of tropospheric NO2 and HCHO in Munich and the comparison to satellite observations

2020 ◽  
Author(s):  
Johannes Lampel ◽  
Ka Lok Chan ◽  
Denis Pöhler ◽  
Matthias Wiegner ◽  
Carlos Alberti ◽  
...  
Keyword(s):  
Pearson Correlation ◽  
Satellite Observations ◽  
Optical Absorption Spectroscopy ◽  
Aerosol Extinction ◽  
Aerosol Formation ◽  
Mixing Ratios ◽  
Monitor Data ◽  
Sun Light ◽  
Good Agreement

&lt;p&gt;We present the Airyx 2D SkySpec Instrument: A commercially available two-dimensionally scanning Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) setup for the observations of trace gases using spectral measurements of scattered sun light and optionally also direct sun light. The waterproof design of the scanner unit is designed for long-term outdoor deployment. Temperature stabilisation of the spectrometers and automatic calibration spectra measurement are used to ensure high-quality measurement data over months and years of observations.&lt;/p&gt;&lt;p&gt;We show 2.5 years of measurements in Munich. Vertical columns and vertical distribution profiles of aerosol extinction coefficient, NO&lt;sub&gt;2&lt;/sub&gt; and HCHO are retrieved from the 2D MAX-DOAS observations. The measured surface aerosol extinction coefficients and NO&lt;sub&gt;2&lt;/sub&gt; mixing ratios are compared to in-situ monitor data. The retrieved surface NO&lt;sub&gt;2&lt;/sub&gt; mixing ratios show good agreement with in-situ monitor data with a Pearson correlation coefficient (R) of 0.91. Good agreement (R= 0.80) is also found for AOD when compared to sun-photometer measurements. Tropospheric vertical column densities (VCDs) of NO2 and HCHO derived from the MAX-DOAS measurements are also used to validate OMI and TROPOMI satellite observations. Monthly averaged data show good correlation, however, satellite observations are on average 30% lower than the MAX-DOAS measurements. Furthermore, the 2D MAX-DOAS observations are used to investigate the spatio-temporal characteristic of NO2 and HCHO in Munich. Analysis of the relations among aerosol, NO&lt;sub&gt;2&lt;/sub&gt; and HCHO show higher aerosol to HCHO ratios in winter indicating a longer atmospheric lifetime of aerosol and HCHO. The analysis also suggests that secondary aerosol formation is the major source of aerosols in Munich.&lt;/p&gt;

scholarly journals Airborne observations and modeling of springtime stratosphere-to-troposphere transport over California

2013 ◽  
Vol 13 (4) ◽  
pp. 10157-10192 ◽  
Author(s):  
E. L. Yates ◽  
L. T. Iraci ◽  
M. C. Roby ◽  
R. B. Pierce ◽  
M. S. Johnson ◽  
...  
Keyword(s):  
Air Quality ◽  
Free Troposphere ◽  
Air Mass ◽  
Air Masses ◽  
Airborne Measurements ◽  
Mixing Ratios ◽  
Stratospheric Intrusion ◽  
Tropospheric O3 ◽  
Carbon Dioxide Co2 ◽  
The Impact

Abstract. Stratosphere-to-troposphere transport (STT) results in air masses of stratospheric origin intruding into the free troposphere. Once in the free troposphere, O3-rich stratospheric air can be transported and mixed with tropospheric air masses, contributing to the tropospheric O3 budget. Evidence of STT can be identified based on the differences in the trace gas composition of the two regions. Because ozone (O3) is present in such large quantities in the stratosphere compared to the troposphere, it is frequently used as a tracer for STT events. This work reports on airborne in situ measurements of O3 and other trace gases during two STT events observed over California, USA. The first, on 14 May 2012, was associated with a cut-off low, and the second, on 5 June 2012, occurred during a post-trough, building ridge event. In each STT event, airborne measurements identified high O3 within a stratospheric intrusion which was observed as low as 3 km above sea level. During both events the stratospheric air mass was characterized by elevated O3 mixing ratios and reduced carbon dioxide (CO2) and water vapor. The reproducible observation of reduced CO2 within the stratospheric air mass supports the use of non-conventional tracers as an additional method for detecting STT. A detailed meteorological analysis of each STT event is presented and observations are interpreted with the Realtime Air Quality Modeling System (RAQMS). The implications of the two STT events are discussed in terms of the impact on the total tropospheric O3 budget and the impact on air quality and policy-making.

scholarly journals In situ measurements of molecular iodine in the marine boundary layer: the link to macroalgae and the implications for O<sub>3</sub>, IO, OIO and NO<sub>x</sub>

2010 ◽  
Vol 10 (1) ◽  
pp. 361-390
Author(s):  
R.-J. Huang ◽  
K. Seitz ◽  
J. Buxmann ◽  
D. Poehler ◽  
K. E. Hornsby ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Marine Boundary Layer ◽  
Single Point ◽  
Molecular Iodine ◽  
In Situ Measurements ◽  
Gas Chromatography Mass Spectrometry ◽  
Optical Absorption Spectroscopy ◽  
Mixing Ratios ◽  
Concentration Levels

Abstract. "Single-point" in situ measurements of molecular iodine (I2) were carried out in the coastal marine boundary layer (MBL) using diffusion denuders in combination with a gas chromatography-mass spectrometry (GC-MS) method. Comparison measurements were taken at Mace Head and Mweenish Bay, on the West Coast of Ireland. The observed mixing ratios of I2 at Mweenish Bay are much higher than that at Mace Head, indicating the emissions of I2 are correlated with the local algal biomass density and algae species. The concentration levels of I2 were found to correlate inversely with tidal height and correlate positively with the concentration levels of O3 in the surrounding air. However, the released I2 can also lead to O3 destruction via the reaction of O3 with iodine atoms that are formed by the photolysis of I2 during the day and via the reaction of I2 with NOx at night. IO and OIO were measured by long-path differential optical absorption spectroscopy (LP-DOAS). The results show that the concentrations of both daytime and nighttime IO are correlated with the mixing ratios of I2. OIO was observed not only during the day but also, for the first time at both Mace Head and Mweenish Bay, at night. In addition, I2 was measured simultaneously by the LP-DOAS technique and compared with the "single-point" in situ measurement. The results suggest that the local algae sources dominate the inorganic iodine chemistry at Mace Head and Mweenish Bay.

scholarly journals Variability and budget of CO<sub>2</sub> in Europe: analysis of the CAATER airborne campaigns – Part 1: Observed variability

2011 ◽  
Vol 11 (12) ◽  
pp. 5655-5672 ◽  
Author(s):  
I. Xueref-Remy ◽  
C. Messager ◽  
D. Filippi ◽  
M. Pastel ◽  
P. Nedelec ◽  
...  
Keyword(s):  
Standard Deviation ◽  
Fossil Fuel ◽  
Back Trajectory ◽  
Free Troposphere ◽  
The West ◽  
Back Trajectories ◽  
Air Masses ◽  
Airborne Measurements ◽  
Fossil Fuel Emissions

Abstract. Atmospheric airborne measurements of CO2 are very well suited for estimating the time-varying distribution of carbon sources and sinks at the regional scale due to the large geographical area covered over a short time. We present here an analysis of two cross-European airborne campaigns carried out on 23–26 May 2001 (CAATER-1) and 2–3 October 2002 (CAATER-2) over Western Europe. The area covered during CAATER-1 and CAATER-2 was 4° W to 14° E long; 44° N to 52° N lat and 1° E to 17° E long; 46° N to 52° N lat respectively. High precision in situ CO2, CO and Radon 222 measurements were recorded. Flask samples were collected during both campaigns to cross-validate the in situ data. During CAATER-1 and CAATER-2, the mean CO2 concentration was 370.1 ± 4.0 (1-σ standard deviation) ppm and 371.7 ± 5.0 (1-σ) ppm respectively. A HYSPLIT back-trajectories analysis shows that during CAATER 1, northwesterly winds prevailed. In the planetary boundary layer (PBL) air masses became contaminated over Benelux and Western Germany by emissions from these highly urbanized areas, reaching about 380 ppm. Air masses passing over rural areas were depleted in CO2 because of the photosynthesis activity of the vegetation, with observations as low as 355 ppm. During CAATER-2, the back-trajectory analysis showed that air masses were distributed among the 4 sectors. Air masses were enriched in CO2 and CO over anthropogenic emission spots in Germany but also in Poland, as these countries have part of the most CO2-emitting coal-based plants in Europe. Simultaneous measurements of in situ CO2 and CO combined with back-trajectories helped us to distinguish between fossil fuel emissions and other CO2 sources. The ΔCO/ΔCO2 ratios (R2 = 0.33 to 0.88, slopes = 2.42 to 10.37), calculated for anthropogenic-influenced air masses over different countries/regions matched national inventories quite well, showing that airborne measurements can help to identify the origin of fossil fuel emissions in the PBL even when distanced by several days/hundreds of kms from their sources. We have compared airborne CO2 observations to nearby ground station measurements and thereby, confirmed that measurements taken in the lower few meters of the PBL (low-level ground stations) are representative of the local scale, while those located in the free troposphere (FT) (moutain stations) are representative of atmospheric CO2 regionally on a scale of a few hundred kilometers. Stations located several 100 km away from each other differ from a few ppm in their measurements indicating the existence of a gradient within the free troposphere. Observations at stations located on top of small mountains may match the airborne data if the sampled air comes from the FT rather than coming up from the valley. Finally, the analysis of the CO2 vertical variability conducted on the 14 profiles recorded in each campaign shows a variability at least 5 to 8 times higher in the PBL (the 1-σ standard deviation associated to the CO2 mean of all profiles within the PBL is 4.0 ppm and 5.7 ppm for CAATER-1 and CAATER-2, respectively) than in the FT (within the FT, 1-σ is 0.5 ppm and 1.1 ppm for CAATER-1 and CAATER-2, respectively). The CO2 jump between the PBL and the FT equals 3.7 ppm for the first campaign and −0.3 ppm for the second campaign. A very striking zonal CO2 gradient of about 11 ppm was observed in the mid-PBL during CAATER-2, with higher concentrations in the west than in the east. This gradient may originate from differences in atmospheric mixing, ground emission rates or Autumn's earlier start in the west. More airborne campaigns are currently under analysis in the framework of the CARBOEUROPE-IP project to better assess the likelihood of these different hypotheses. In a companion paper (Xueref-Remy et al., 2011, Part 2), a comparison of vertical profiles from observations and several modeling frameworks was conducted for both campaigns.

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