ALBERT

Description: Three years of greenhouse gases measurements, obtained using a gas chromatograph (GC) system located at the Puy de Dôme station at 1465 m a.s.l. in Central France are presented. The GC system was installed in 2010 at Puy de Dôme and was designed for automatic and accurate semi-continuous measurements of atmospheric carbon dioxide, methane, nitrous oxide and sulfur hexafluoride mole fractions. We present in detail the instrumental set up and the calibration strategy, which together allow the GC to reach repeatabilities of 0.1 μmol mol−1, 1.2, 0.3 nmol mol−1 and 0.06 pmol mol−1 for CO2, CH4, N2O and SF6, respectively. Comparisons of the atmospheric time series with those obtained using other instruments shown that the GC system meets the World Meteorological Organization recommendations. The analysis of the three-year atmospheric time series revealed how the planetary boundary layer height drives the mole fractions observed at a mountain site such as Puy de Dôme where air masses alternate between the planetary boundary layer and the free troposphere. Accurate long-lived greenhouse gases measurements collocated with 222Rn measurements as an atmospheric tracer, allowed us to determine the CO2, CH4 and N2O emissions in the catchment area of the station. The derived CO2 surface flux revealed a clear seasonal cycle with net uptake by plant assimilation in the spring and net emission caused by the biosphere and burning of fossil fuel during the remainder of the year. We calculated a mean annual CO2 flux of 1150 t(CO2) km−2. The derived CH4 and N2O emissions in the station catchment area were 5.6 t(CH4) km−2 yr−1 and 1.5 t(N2O) km−2 yr−1, respectively. Our derived annual CH4 flux is in agreement with the national French inventory, whereas our derived N2O flux is five times larger than the same inventory.

Description: While atmospheric new particle formation (NPF) has been observed in various environments and was found to contribute significantly to the total aerosol particle concentration, the production of new particles over open seas is poorly documented in the literature. Nucleation events were detected and analysed over the Mediterranean Sea using two condensation particle counters and a Scanning Mobility Particle Sizer on-board the ATR-42 research aircraft during flights conducted between the 11 September and the 4 November 2012 in the framework of the HYMEX (HYdrological cycle in Mediterranean EXperiment) project. The main purpose of the present work was to characterize the spatial extent of the NPF process. Our findings show that nucleation is occurring over large areas above the Mediterranean Sea in all air mass types. Maximum concentrations of particles in the size range 5–10 nm (N5–10) do not systematically coincide with lower fetches (time spent by the air mass over the sea before sampling), and significant N5–10 values are found for fetches between 0 and 60 h depending on the air mass type. These observations suggest that nucleation events could be more influenced by processes occurring above the sea, rather than linked to synoptic history. The analysis of the vertical extent of nucleation demonstrates that the process is favoured at high altitude, above 1000 m, i.e. frequently in the free troposphere, and more especially between 2000 and 3000 m, where the nucleation frequency is close to 50%. This vertical distribution of nucleation is favoured by the gradients of several parameters, such as the condensation sink, the temperature and the relative humidity. The mixing of two air parcels could also explain the occurrence of nucleation at preferential altitudes. After they formed, particles slowly grow at high altitude to diameters of at least 30 nm while being poorly depleted by coagulation processes. Our analysis of the particle size distributions suggests that particle growth could decrease with increasing altitudes.

Description: Secondary pollutants such as ozone, secondary inorganic aerosol, and secondary organic aerosol formed in the plume of megacities can affect regional air quality. In the framework of the FP7/EU MEGAPOLI project, an intensive campaign was launched in the Greater Paris Region in July 2009. The major objective was to quantify different sources of organic aerosol (OA) within a megacity and in its plume. In this study, we use airborne measurements aboard the French ATR-42 aircraft to evaluate the regional chemistry-transport model CHIMERE within and downwind the Paris region. Slopes of the plume OA levels vs. Ox (= O3 + NO2) show secondary OA (SOA) formation normalized with respect to photochemical activity and are used for specific evaluation of the OA scheme in the model. Simulated and observed slopes are in good agreement, when the most realistic "high-NOx" yields are used in the Volatility-Basis-Set scheme implemented into the model. In addition, these slopes are relatively stable from one day to another, which suggest that they are characteristic for the given megacity plume environment. Since OA within the plume is mainly formed from anthropogenic precursors (VOC and primary OA, POA), this work allows a specific evaluation of anthropogenic SOA and SOA formed from primary semi-volatile and intermediate volatile VOCs (SI-SOA) formation scheme in a model. For specific plumes, this anthropogenic OA build-up can reach about 10 μg m−3. For the average of the month of July 2009, maximum increases occur close to the agglomeration for primary OA are noticed at several tens (for POA) to hundred (for SI-SOA) kilometers of distance from the Paris agglomeration.

Description: Three years of greenhouse gas measurements, obtained using a gas chromatograph (GC) system located at the Puy de Dôme station at 1465 m a.s.l. in central France, are presented. The GC system was installed in 2010 at Puy de Dôme and was designed for automatic and accurate semicontinuous measurements of atmospheric carbon dioxide, methane, nitrous oxide and sulfur hexafluoride mole fractions. We present in detail the instrumental setup and the calibration strategy, which together allow the GC to reach repeatabilities of 0.1 μmol mol−1, 1.2 nmol mol−1, 0.3 nmol mol−1 and 0.06 pmol mol−1 for CO2, CH4, N2O and SF6, respectively. The analysis of the 3-year atmospheric time series revealed how the planetary boundary layer height drives the mole fractions observed at a mountain site such as Puy de Dôme where air masses alternate between the planetary boundary layer and the free troposphere. Accurate long-lived greenhouse gas measurements collocated with 222Rn measurements as an atmospheric tracer allowed us to determine the CO2, CH4 and N2O emissions in the catchment area of the station. The derived CO2 surface flux revealed a clear seasonal cycle, with net uptake by plant assimilation in the spring and net emission caused by the biosphere and burning of fossil fuel during the remainder of the year. We calculated a mean annual CO2 flux of 1310 ± 680 t CO2 km−2. The derived CH4 and N2O emissions in the station catchment area were 7.0 ± 4.0 t CH4 km−2 yr−1 and 1.8 ± 1.0 t N2O km−2 yr−1, respectively. Our derived annual CH4 flux is in agreement with the national French inventory, whereas our derived N2O flux is 5 times larger than the same inventory.

Description: Secondary pollutants such as ozone, secondary inorganic aerosol, and secondary organic aerosol formed in the plumes of megacities can affect regional air quality. In the framework of the FP7/EU MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) project, an intensive campaign was launched in the greater Paris region in July 2009. The major objective was to quantify different sources of organic aerosol (OA) within a megacity and in its plume. In this study, we use airborne measurements aboard the French ATR-42 aircraft to evaluate the regional chemistry-transport model CHIMERE within and downwind of the Paris region. Two mechanisms of secondary OA (SOA) formation are used, both including SOA formation from oxidation and chemical aging of primary semivolatile and intermediate volatility organic compounds (SI-SOA) in the volatility basis set (VBS) framework. As for SOA formed from traditional VOC (volatile organic compound) precursors (traditional SOA), one applies chemical aging in the VBS framework adopting different SOA yields for high- and low-NOx environments, while another applies a single-step oxidation scheme without chemical aging. Two emission inventories are used for discussion of emission uncertainties. The slopes of the airborne OA levels versus Ox (i.e., O3 + NO2) show SOA formation normalized with respect to photochemical activity and are used for specific evaluation of the OA scheme in the model. The simulated slopes were overestimated slightly by factors of 1.1, 1.7 and 1.3 with respect to those observed for the three airborne measurements, when the most realistic "high-NOx" yields for traditional SOA formation in the VBS scheme are used in the model. In addition, these slopes are relatively stable from one day to another, which suggests that they are characteristic for the given megacity plume environment. The configuration with increased primary organic aerosol (POA) emissions and with a single-step oxidation scheme of traditional SOA also agrees with the OA / Ox slopes (about ± 50 % with respect to the observed ones); however, it underestimates the background. Both configurations are coherent with observed OA plume buildup, but they show very different SI-SOA and traditional anthropogenic SOA (ASOA) contributions. It is hence concluded that available theoretical knowledge and available data in this study are not sufficient to discern the relative contributions of different types of anthropogenic SOA in the Paris pollution plume, while its sum is correctly simulated. Based on these simulations, for specific plumes, the anthropogenic OA buildup can reach between 8 and 10μg m−3. For the average of the month of July 2009, maximum OA increases due to emissions from the Paris agglomeration are noticed close to the agglomeration at various length scales: several tens (for primary OA) to hundreds (for SI-SOA and ASOA) of kilometers from the Paris agglomeration. In addition, BSOA (SOA formed from biogenic VOC precursors) is an important contributor to regional OA levels (inside and outside the Paris plume).

Description: While atmospheric new particle formation (NPF) has been observed in various environments and was found to contribute significantly to the total aerosol particle concentration, the production of new particles over open seas is poorly documented in the literature. Nucleation events were detected and analysed over the Mediterranean Sea using two condensation particle counters and a scanning mobility particle sizer on board the ATR-42 research aircraft during flights conducted between 11 September and 4 November 2012 in the framework of the HYMEX (HYdrological cycle in Mediterranean EXperiment) project. The main purpose of the present work was to characterize the spatial extent of the NPF process, both horizontally and vertically. Our findings show that nucleation is occurring over large areas above the Mediterranean Sea in all air mass types. Maximum concentrations of particles in the size range 5–10 nm (N5–10) do not systematically coincide with lower fetches (time spent by the air mass over the sea before sampling), and significant N5–10 values are found for fetches between 0 and 60 h depending on the air mass type. These observations suggest that nucleation events could be more influenced by local precursors originating from emission processes occurring above the sea, rather than linked to synoptic history. Vertical soundings were performed, giving the opportunity to examine profiles of the N5–10 concentration and to analyse the vertical extent of NPF. Our observations demonstrate that the process could be favoured above 1000 m, i.e. frequently in the free troposphere, and more especially between 2000 and 3000 m, where the NPF frequency is close to 50 %. This vertical distribution of NPF might be favoured by the gradients of several atmospheric parameters, together with the mixing of two air parcels, which could also explain the occurrence of the process at preferential altitudes. In addition, increased condensation sinks collocated with high concentrations of small particles suggest the occurrence of NPF events promoted by inputs from the boundary layer, most probably associated with convective clouds and their outflow. After their formation, particles slowly grow at higher altitudes to diameters of at least 30 nm while not being greatly depleted or affected by coagulation. Our analysis of the particle size distributions suggests that particle growth could decrease with increasing altitude.