Abstract. Tropical Tropopause Layer (TTL) clouds have a significant impact on the Earth’s radiative budget and regulate the amount of water vapor entering the stratosphere. During the Strateole-2 observation campaign, three microlidars were flown onboard stratospheric superpressure balloons from October 2021 to late January 2022, slowly drifting only a few kilometers above the TTL. These measurements have unprecedented sensitivity to thin cirrus and provide a fine-scale description of cloudy structures both in time and space. Case studies of collocated observations with the space-borne lidar Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) show a very good agreement between the instruments and highlight the unique ability of the microlidar to detect optically very thin clouds below CALIOP detection capacity (optical depth τ < 2 · 10−3). Statistics on cloud occurrence show that TTL cirrus appear in more than 50 % of the microlidar profiles and have a mean geometrical depth of 1 km. Ultrathin TTL cirrus (τ < 2 · 10−3) have a significant coverage (16 % of the profiles) and their mean geometrical depth is below 500 m.
Abstract. This study documents several processes of stratosphere-troposphere transport (STT) in the subtropical region. A case study of the interaction between a Rossby Wave breaking over the Canary Islands and a subtropical vortex core situated further south is analysed with ozone airborne measurements (in-situ and Lidar). The investigation is conducted using a Reverse Domain Filling technique to reconstruct high-resolution potential vorticity fields with a Lagrangian approach and with simulations of a mesoscale model. Results show irreversible STT associated with tropopause folding, Rossby Wave Breaking and the filamentation of the subtropical vortex core.
Abstract. Ozone data retrieved in the Arctic region from infrared radiance spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI) on board the MetOp-A European satellite are presented. They are compared with in situ and lidar observations obtained during a series of aircraft measurement campaigns as part of the International Polar Year POLARCAT activities in spring and summer 2008. Different air masses were sampled during the campaigns including clean air, polluted plumes originating from anthropogenic sources, forest fire plumes from the three northern continents, and stratospheric-influenced air masses. The comparison between IASI O3 [0–8 km], [0–12 km] partial columns and profiles with collocated aircraft observations is achieved by taking into account the different sensitivity and geometry of the sounding instruments. A detailed analysis is provided and the agreement is discussed in terms of vertical sensitivity and surface properties at the location of the observations. Overall, IASI O3 profiles are found to be in relatively good agreement with smoothed in situ and lidar profiles in the free troposphere with differences of less than 40% (25% over sea for both seasons) and 10%, respectively. The correlation between IASI O3 retrieved partial columns and the smoothed aircraft partial columns is good with DC-8 in situ data in spring over North America (r = 0.68), and over Greenland with ATR-42 lidar measurements in summer (r = 0.67). Correlations with other data are less significant highlighting the difficulty of IASI to capture precisely the O3 variability in the Arctic upper troposphere and lower stratosphere (UTLS). This is particularly noted in comparison with the [0–12 km] partial columns. The IASI [0–8 km] partial columns display a low negative bias (by less than 26% over snow) compared to columns derived from in situ measurements. Despite the relatively high biases of the IASI retrievals in the Arctic UTLS, our analysis shows that IASI can be used to identify, using O3 / CO ratios, stratospheric intrusions.
Abstract. Ozone pollution transported to the Arctic is a significant concern because of the rapid, enhanced warming in high northern latitudes, which is caused, in part, by short-lived climate forcers, such as ozone. Long-range transport of pollution contributes to background and episodic ozone levels in the Arctic. However, the extent to which plumes are photochemically active during transport, particularly during the summer, is still uncertain. In this study, regional chemical transport model simulations are used to examine photochemical production of ozone in air masses originating from boreal fire and anthropogenic emissions over North America and during their transport toward the Arctic during early July 2008. Model results are evaluated using POLARCAT aircraft data collected over boreal fire source regions in Canada (ARCTAS-B) and several days downwind over Greenland (POLARCAT-France and POLARCAT-GRACE). Model results are generally in good agreement with the observations, except for certain trace gas species over boreal fire regions, in some cases indicating that the fire emissions are too low. Anthropogenic and biomass burning pollution (BB) from North America was rapidly uplifted during transport east and north to Greenland where pollution plumes were observed in the mid- and upper troposphere during POLARCAT. A model sensitivity study shows that CO levels are in better agreement with POLARCAT measurements (fresh and aged fire plumes) upon doubling CO emissions from fires. Analysis of model results, using ΔO3/ΔCO enhancement ratios, shows that pollution plumes formed ozone during transport towards the Arctic. Fresh anthropogenic plumes have average ΔO3/ΔCO enhancement ratios of 0.63 increasing to 0.92 for aged anthropogenic plumes, indicating additional ozone production during aging. Fresh fire plumes are only slightly enhanced in ozone (ΔO3/ΔCO=0.08), but form ozone downwind with ΔO3/ΔCO of 0.49 for aged BB plumes (model-based run). We estimate that aged anthropogenic and BB pollution together made an important contribution to ozone levels with an average contribution for latitudes >55° N of up to 6.5 ppbv (18%) from anthropogenic pollution and 3 ppbv (5.2%) from fire pollution in the model domain in summer 2008.
Abstract The characterization and the precise measurements of atmospheric pollutant’s concentration are essential to improve the understanding and modeling of urban air pollution processes. The QualAir platform at the Université Pierre et Marie Curie (UPMC) is an experimental research platform dedicated to urban air quality and pollution studies. As one of the major instruments, the ground-based QualAir Fourier transform spectrometer (FTS) provides information on the air composition of a megacity like Paris, France. Operating in solar infrared absorption, it enables the monitoring of several important pollutants involved in tropospheric chemistry and atmospheric transport around the Ile de France region. Results on nitrous oxide (N2O), methane (CH4), and carbon monoxide (CO) will be presented in this paper, as well as the CO measurements comparison with satellite and in situ measurements showing the capabilities and strengths of this ground-based FTS with the other instruments of the QualAir platform.
Abstract. Most of the global fossil fuel CO2 emissions arise from urbanized and industrialized areas. Bottom-up inventories quantify them but with large uncertainties. In 2010–2011, the first atmospheric in situ CO2 measurement network for Paris, the capital of France, began operating with the aim of monitoring the regional atmospheric impact of the emissions coming from this megacity. Five stations sampled air along a northeast–southwest axis that corresponds to the direction of the dominant winds. Two stations are classified as rural (Traînou – TRN; Montgé-en-Goële – MON), two are peri-urban (Gonesse – GON; Gif-sur-Yvette – GIF) and one is urban (EIF, located on top of the Eiffel Tower). In this study, we analyze the diurnal, synoptic and seasonal variability of the in situ CO2 measurements over nearly 1 year (8 August 2010–13 July 2011). We compare these datasets with remote CO2 measurements made at Mace Head (MHD) on the Atlantic coast of Ireland and support our analysis with atmospheric boundary layer height (ABLH) observations made in the center of Paris and with both modeled and observed meteorological fields. The average hourly CO2 diurnal cycles observed at the regional stations are mostly driven by the CO2 biospheric cycle, the ABLH cycle and the proximity to urban CO2 emissions. Differences of several µmol mol−1 (ppm) can be observed from one regional site to the other. The more the site is surrounded by urban sources (mostly residential and commercial heating, and traffic), the more the CO2 concentration is elevated, as is the associated variability which reflects the variability of the urban sources. Furthermore, two sites with inlets high above ground level (EIF and TRN) show a phase shift of the CO2 diurnal cycle of a few hours compared to lower sites due to a strong coupling with the boundary layer diurnal cycle. As a consequence, the existence of a CO2 vertical gradient above Paris can be inferred, whose amplitude depends on the time of the day and on the season, ranging from a few tenths of ppm during daytime to several ppm during nighttime. The CO2 seasonal cycle inferred from monthly means at our regional sites is driven by the biospheric and anthropogenic CO2 flux seasonal cycles, the ABLH seasonal cycle and also synoptic variations. Enhancements of several ppm are observed at peri-urban stations compared to rural ones, mostly from the influence of urban emissions that are in the footprint of the peri-urban station. The seasonal cycle observed at the urban station (EIF) is specific and very sensitive to the ABLH cycle. At both the diurnal and the seasonal scales, noticeable differences of several ppm are observed between the measurements made at regional rural stations and the remote measurements made at MHD, that are shown not to define background concentrations appropriately for quantifying the regional (∼ 100 km) atmospheric impact of urban CO2 emissions. For wind speeds less than 3 m s−1, the accumulation of local CO2 emissions in the urban atmosphere forms a dome of several tens of ppm at the peri-urban stations, mostly under the influence of relatively local emissions including those from the Charles de Gaulle (CDG) Airport facility and from aircraft in flight. When wind speed increases, ventilation transforms the CO2 dome into a plume. Higher CO2 background concentrations of several ppm are advected from the remote Benelux–Ruhr and London regions, impacting concentrations at the five stations of the network even at wind speeds higher than 9 m s−1. For wind speeds ranging between 3 and 8 m s−1, the impact of Paris emissions can be detected in the peri-urban stations when they are downwind of the city, while the rural stations often seem disconnected from the city emission plume. As a conclusion, our study highlights a high sensitivity of the stations to wind speed and direction, to their distance from the city, but also to the ABLH cycle depending on their elevation. We learn some lessons regarding the design of an urban CO2 network: (1) careful attention should be paid to properly setting regional (∼ 100 km) background sites that will be representative of the different wind sectors; (2) the downwind stations should be positioned as symmetrically as possible in relation to the city center, at the peri-urban/rural border; (3) the stations should be installed at ventilated sites (away from strong local sources) and the air inlet set up above the building or biospheric canopy layer, whichever is the highest; and (4) high-resolution wind information should be available with the CO2 measurements.
Abstract. The goal of the paper are to: (1) present tropospheric ozone (O3) climatologies in summer 2008 based on a large amount of measurements, during the International Polar Year when the Polar Study using Aircraft, Remote Sensing, Surface Measurements, and Models of Climate Chemistry, Aerosols, and Transport (POLARCAT) campaigns were conducted (2) investigate the processes that determine O3 concentrations in two different regions (Canada and Greenland) that were thoroughly studied using measurements from 3 aircraft and 7 ozonesonde stations. This paper provides an integrated analysis of these observations and the discussion of the latitudinal and vertical variability of tropospheric ozone north of 55° N during this period is performed using a regional model (WFR-Chem). Ozone, CO and potential vorticity (PV) distributions are extracted from the simulation at the measurement locations. The model is able to reproduce the O3 latitudinal and vertical variability but a negative O3 bias of 6–15 ppbv is found in the free troposphere over 4 km, especially over Canada. Ozone average concentrations are of the order of 65 ppbv at altitudes above 4 km both over Canada and Greenland, while they are less than 50 ppbv in the lower troposphere. The relative influence of stratosphere-troposphere exchange (STE) and of ozone production related to the local biomass burning (BB) emissions is discussed using differences between average values of O3, CO and PV for Southern and Northern Canada or Greenland and two vertical ranges in the troposphere: 0–4 km and 4–8 km. For Canada, the model CO distribution and the weak correlation (< 30 %) of O3 and PV suggests that stratosphere-troposphere exchange (STE) is not the major contribution to average tropospheric ozone at latitudes less than 70° N, due to the fact that local biomass burning (BB) emissions were significant during the 2008 summer period. Conversely over Greenland, significant STE is found according to the better O3 versus PV correlation (> 40 %) and the higher 75th PV percentile. A weak negative latitudinal summer ozone gradient −6 to −8 ppbv is found over Canada in the mid troposphere between 4 and 8 km. This is attributed to an efficient O3 photochemical production due to the BB emissions at latitudes less than 65° N, while STE contribution is more homogeneous in the latitude range 55° N to 70° N. A positive ozone latitudinal gradient of 12 ppbv is observed in the same altitude range over Greenland not because of an increasing latitudinal influence of STE, but because of different long range transport from multiple mid-latitude sources (North America, Europe and even Asia for latitudes higher than 77° N).
Two ground‐based ozone lidars have been operated at Observatoire de Haute Provence (OHP) for 11 days during the Intercontinental Transport of Ozone and Precursors (ITOP‐2004) measurement campaign. Ozone and scattering ratio vertical profiles have been measured from the boundary layer up to the tropopause. At first order, tropospheric ozone temporal variability is due to local pollution within the planetary boundary layer and to stratosphere‐troposphere exchange. Remaining ozone rich layers within the free troposphere are related to long‐range transport processes. Transport pathways are discussed combining Lagrangian particle dispersion modeling analysis and upstream airborne in situ measurements of the chemical composition of these air masses. High ozone and CO mixing ratios measured within polluted plumes aboard the aircraft correspond to ozone and aerosol layers seen by the lidar. Most of these layers have their origin in North America where they are uplifted either by forest fires or by warm conveyor belts in the vicinity of frontal regions. During the campaign, these polluted and thin (<1 km) layers remain coherent and are transported in a Lagrangian manner over the Atlantic Ocean. The layers observed above OHP in the lower free troposphere exhibit ozone mixing ratio 50% larger than background values. With an ozone content of 3 to 6 Dobson Units, these layers increase by 5 to 10% the background tropospheric ozone column.
