Atmospheric concentration measurements are used to adjust the daily to monthly budget of fossil fuel CO2 emissions of the Paris urban area from the prior estimates established by the Airparif local ...air quality agency. Five atmospheric monitoring sites are available, including one at the top of the Eiffel Tower. The atmospheric inversion is based on a Bayesian approach, and relies on an atmospheric transport model with a spatial resolution of 2 km with boundary conditions from a global coarse grid transport model. The inversion adjusts prior knowledge about the anthropogenic and biogenic CO2 fluxes from the Airparif inventory and an ecosystem model, respectively, with corrections at a temporal resolution of 6 h, while keeping the spatial distribution from the emission inventory. These corrections are based on assumptions regarding the temporal autocorrelation of prior emissions uncertainties within the daily cycle, and from day to day. The comparison of the measurements against the atmospheric transport simulation driven by the a priori CO2 surface fluxes shows significant differences upwind of the Paris urban area, which suggests a large and uncertain contribution from distant sources and sinks to the CO2 concentration variability. This contribution advocates that the inversion should aim at minimising model-data misfits in upwind-downwind gradients rather than misfits in mole fractions at individual sites. Another conclusion of the direct model-measurement comparison is that the CO2 variability at the top of the Eiffel Tower is large and poorly represented by the model for most wind speeds and directions. The model's inability to reproduce the CO2 variability at the heart of the city makes such measurements ill-suited for the inversion. This and the need to constrain the budgets for the whole city suggests the assimilation of upwind-downwind mole fraction gradients between sites at the edge of the urban area only. The inversion significantly improves the agreement between measured and modelled concentration gradients. Realistic emissions are retrieved for two 30-day periods and suggest a significant overestimate by the AirParif inventory. Similar inversions over longer periods are necessary for a proper evaluation of the optimised CO2 emissions against independent data.
Within the framework of a French nationally funded project (CO2-MEGAPARIS) for quantifying the CO2 emissions of the Paris area, a lidar-based experimental investigation of the variability of the ...atmospheric boundary layer (ABL) depths was performed over four days in March 2011 under clear sky conditions. The prevailing synoptic settings were mainly characterized by anti-cyclonic situations with low wind. The key aim of this paper is to assess the impact of the urban heat island intensity (UHII) on the spatio-temporal variability of the ABL depths over the Paris megacity. A network of fixed aerosol lidars was deployed inside the city and in the vicinity of sub-urban and rural areas. Additionally, the spatial heterogeneity of the nocturnal boundary layer (NBL) depths over greater Paris area is addressed, thanks in particular, to the deployment of a 355-nm elastic lidar in a mobile van to measure the aerosol distributions. Radiosonde-derived profiles (twice a day) of thermodynamic variables over the sub-urban site helped investigate the temperature inversion above ground and hence to compare the lidar-derived ABL depths. Comparing these two results, an excellent concordance was found with a correlation coefficient of 0.994.
Five important factors closely related to the ABL circulation, namely, spatio-temporal variability of the ABL depths, growth rate of the ABL depths, entrainment zone thickness, and near-surface temperature fields including resultant UHII were considered to infer the urban–rural contrasts. The mean NBL depth over the urban area was on average 63 m (45%) higher than its adjacent sub-urban area which was, on occasion, as much as (74 m) 58% higher mainly due to the effect of UHII. Daytime well-mixed convective boundary layer and associated strong turbulent mixing near its top over the urban area showed higher entrainment zone thickness (326 m) than over sub-urban (234 m) and rural (200 m) areas. Temperature growth rates during sunrise increased up to more than 3 °C h−1 over the sub-urban area while over the urban region it was 2.5 °C h−1 or even less. The ABL depths over the urban site decayed more slowly (500 m h−1) than over the sub-urban area (600 m h−1) during the late afternoon transition period suggesting an impact of the UHII on the ABL dynamics over the urban area.
► Multi-lidar investigation of spatio-temporal variability of the ABL depth around Paris. ► First mobile lidar-based study of the spatial variability of NBL depth around a megacity. ► Assessment of impact of urban heat island (UHI) intensity and urban–rural contrast on ABL depth evolution. ► Higher entrainment zone thickness over urban area than over rural and sub-urban areas.
The determination of the depth of daytime and nighttime mixing layers must be known very accurately to relate boundary-layer concentrations of gases or particles to upstream fluxes. The mixing-height ...is parametrized in numerical weather prediction models, so improving the determination of the mixing height will improve the quality of the estimated gas and particle budgets. Datasets of mixing-height diurnal cycles with high temporal and spatial resolutions are sought by various end users. Lidars and ceilometers provide vertical profiles of backscatter from aerosol particles. As aerosols are predominantly concentrated in the mixing layer, lidar backscatter profiles can be used to trace the depth of the mixing layer. Large numbers of automatic profiling lidars and ceilometers are deployed by meteorological services and other agencies in several European countries providing systems to monitor the mixing height on temporal and spatial scales of unprecedented density. We investigate limitations and capabilities of existing mixing height retrieval algorithms by applying five different retrieval techniques to three different lidars and ceilometers deployed during two 1-month campaigns. We studied three important steps in the mixing height retrieval process, namely the lidar/ceilometer pre-processing to reach sufficient signal-to-noise ratio, gradient detection techniques to find the significant aerosol gradients, and finally quality control and layer attribution to identify the actual mixing height from multiple possible layer detections. We found that layer attribution is by far the most uncertain step. We tested different gradient detection techniques, and found no evidence that the first derivative, wavelet transform, and two-dimensional derivative techniques have different skills to detect one or multiple significant aerosol gradients from lidar and ceilometer attenuated backscatter. However, our study shows that, when mixing height retrievals from a ultraviolet lidar and a near-infrared ceilometer agreed, they were 25–40% more likely to agree with an independent radiosonde mixing height retrieval than when each lidar or ceilometer was used alone. Furthermore, we point to directions that may assist the layer attribution step, for instance using commonly available surface measurements of radiation and temperature to derive surface sensible heat fluxes as a proxy for the intensity of convective mixing. It is a worthwhile effort to pursue such studies so that within a few years automatic profiling lidar and ceilometer networks can be utilized efficiently to monitor mixing heights at the European scale.
The Total Carbon Column Observing Network (TCCON) is a ground-based network of Fourier Transform Spectrometer (FTS) sites around the globe, where the column abundances of CO2 , CH4 , N2 O, CO and O2 ...are measured. CO2 is constrained with a precision better than 0.25% (1-σ). To achieve a similarly high accuracy, calibration to World Meteorological Organization (WMO) standards is required. This paper introduces the first aircraft calibration campaign of five European TCCON sites and a mobile FTS instrument. A series of WMO standards in-situ profiles were obtained over European TCCON sites via aircraft and compared with retrievals of CO2 column amounts from the TCCON instruments. The results of the campaign show that the FTS measurements are consistently biased 1.1% ± 0.2% low with respect to WMO standards, in agreement with previous TCCON calibration campaigns. The standard a priori profile for the TCCON FTS retrievals is shown to not add a bias. The same calibration factor is generated using aircraft profiles as a priori and with the TCCON standard a priori. With a calibration to WMO standards, the highly precise TCCON CO2 measurements of total column concentrations provide a suitable database for the calibration and validation of nadir-viewing satellites.
During the extended activity of Mount Etna volcano in February–April 2021, three distinct paroxysmal events took place from February 21 to 26, which were associated with a very uncommon transport of ...the injected upper‐tropospheric plumes toward the north. Using a synergy of observations and modeling, we characterized the emissions and three‐dimensional dispersion for these three plumes, monitored their downwind distribution and optical properties, and estimated their radiative impacts at selected locations. With a satellite‐based source inversion, we estimate the emitted sulfur dioxide (SO2) mass at an integrated value of 55 kt and plumes injections at up to 12 km altitudes, which qualifies this series as an extreme event for Mount Etna. Then, we combine Lagrangian dispersion modeling, initialized with measured temporally resolved SO2 emission fluxes and altitudes, with satellite observations to track the dispersion of the three individual plumes. The transport toward the north allowed the height‐resolved downwind monitoring of the plumes at selected observatories in France, Italy, and Israel, using LiDARs and photometric aerosol observations. Volcanic‐specific aerosol optical depths (AODs) in the visible spectral range ranging from about 0.004 to 0.03 and local daily average shortwave radiative forcing (RF) ranging from about −0.2 to −1.2 W m−2 (at the top of atmosphere) and from about −0.2 to −3.0 W m−2 (at the surface) are found. The composition (possible presence of ash), AOD, and RF of the plume have a large inter‐plume and intra‐plume variability and thus depend strongly on the position of the sampled section of the plumes.
Plain Language Summary
The volcanic plumes from Mount Etna's eruptions disperse usually toward the east, to the Central‐Eastern Mediterranean, where ground stations are not available to monitor and characterize them. During the extended intense volcanic activity of Mount Etna in February–April 2021, some of the plumes dispersed toward the north, in an area where many and well‐equipped ground observatories are available. This was a unique opportunity to study the emissions, dispersion dynamics, shape/composition, and impacts of Mount Etna's aerosol plumes. We analyzed these rare events using many information layers: satellite observations, numerical simulation of the plume's dispersion, and downwind ground‐based observatories. By coupling these information pieces, we could reconstruct these events and untangle their impacts from those of a major Saharan dust outbreak that occurred simultaneously. These events were found quite extreme for Mount Etna (extreme emissions and high altitude—around 12 km). We found that this type of extreme Etna's eruptions has a relevant (and not yet studied) impact on the atmospheric composition and regional climate in the Mediterranean area. The plumes, after continental dispersion, exhibit a complex filamentary shape and a complex aerosol composition and properties, due to the presence of both sulfur‐containing particles and ash.
Key Points
Three distinct paroxysmal events took place at Mount Etna from February 21 to 26, 2021 and the plumes were transported toward the north
Plumes dispersion is characterized with Lagrangian modeling initialized with measured SO2 emissions and with satellite observations
A series of LiDARs detected and characterized the plumes downwind and their observations are used to estimate the plumes radiative forcing
To develop an accurate measurement network of greenhouse gases, instruments in the field need to be stable and precise and thus require infrequent calibrations and a low consumption of consumables. ...For about 10 years, cavity ring-down spectroscopy (CRDS) analyzers have been available that meet these stringent requirements for precision and stability. Here, we present the results of tests of CRDS instruments in the laboratory (47 instruments) and in the field (15 instruments). The precision and stability of the measurements are studied. We demonstrate that, thanks to rigorous testing, newer models generally perform better than older models, especially in terms of reproducibility between instruments. In the field, we see the importance of individual diagnostics during the installation phase, and we show the value of calibration and target gases that assess the quality of the data. Finally, we formulate recommendations for use of these analyzers in the field.
Measurements of CO2, CO, NOx and selected Volatile Organic Compounds (VOCs) mole fractions were performed continuously during a 10-day period in the Guy Môquet tunnel in Thiais, a peri-urban area ...about 15 km south of the centre of Paris, between 28 September and 8 October 2012. This data set is used here to identify the characteristics of traffic-emitted CO2 by evaluating its ratios to co-emitted species for the first time in the Paris region. High coefficients of determination (r2 > 0.7) are observed between CO2 and certain compounds that are characteristic of the traffic source (CO, NOx, benzene, xylenes and acetylene). Weak correlations (r2 < 0.2) are found with species such as propane, n-butane and i-butane that are associated with fuel evaporation, an insignificant source for CO2. To better characterise the traffic signal we focus only on species that are well-correlated with CO2 and on rush-hour periods characterised by the highest traffic-related mole fractions. From those mole fractions we remove the nighttime-average weekday mole fraction obtained for each species that we infer to be the most appropriate background signal for our study. Then we calculate observed Δspecies / ΔCO2 ratios, which we compare with the ones provided by the 2010 bottom–up high-resolved regional emission inventory from Airparif (the association in charge of monitoring the air quality in Île-de-France), focusing on local emission data for the specific road of the tunnel. We find an excellent agreement (2%) between the local inventory emission CO / CO2 ratio and our observed ΔCO / ΔCO2 ratio. Former tunnel experiments carried out elsewhere in the world provided observed ΔCO / ΔCO2 ratios that differ from 49 to 592% to ours. This variability can be related to technological improvement of vehicles, differences in driving conditions, and fleet composition. We also find a satisfactory agreement with the Airparif inventory for n-propylbenzene, n-pentane and xylenes to CO2 ratios. For most of the other species, the ratios obtained from the local emission inventory overestimate the observed ratios to CO2 by 34 to more than 300%. However, the emission ratios of NOx, o-xylene and i-pentane are underestimated by 30 to 79%. One main cause of such high differences between the inventory and our observations is likely the obsolete feature of the VOCs speciation matrix of the inventory that has not been updated since 1998, although law regulations on some VOCs have occurred since that time. Our study bears important consequences, discussed in the conclusion, for the characterisation of the urban CO2 plume and for atmospheric inverse modelling of urban CO2 emissions.
Accurate simulation of the spatial and temporal variability of tracer mixing ratios over urban areas is a challenging and interesting task needed to be performed in order to utilise CO2 measurements ...in an atmospheric inverse framework and to better estimate regional CO2 fluxes. This study investigates the ability of a high-resolution model to simulate meteorological and CO2 fields around Paris agglomeration during the March field campaign of the CO2-MEGAPARIS project. The mesoscale atmospheric model Meso-NH, running at 2 km horizontal resolution, is coupled with the Town Energy Balance (TEB) urban canopy scheme and with the Interactions between Soil, Biosphere and Atmosphere CO2-reactive (ISBA-A-gs) surface scheme, allowing a full interaction of CO2 modelling between the surface and the atmosphere. Statistical scores show a good representation of the urban heat island (UHI) with stronger urban–rural contrasts on temperature at night than during the day by up to 7 °C. Boundary layer heights (BLH) have been evaluated on urban, suburban and rural sites during the campaign, and also on a suburban site over 1 yr. The diurnal cycles of the BLH are well captured, especially the onset time of the BLH increase and its growth rate in the morning, which are essential for tall tower CO2 observatories. The main discrepancy is a small negative bias over urban and suburban sites during nighttime (respectively 45 m and 5 m), leading to a few overestimations of nocturnal CO2 mixing ratios at suburban sites and a bias of +5 ppm. The diurnal CO2 cycle is generally well captured for all the sites. At the Eiffel tower, the observed spikes of CO2 maxima occur every morning exactly at the time at which the atmospheric boundary layer (ABL) growth reaches the measurement height. At suburban ground stations, CO2 measurements exhibit maxima at the beginning and at the end of each night, when the ABL is fully contracted, with a strong spatio-temporal variability. A sensitivity test without urban parameterisation removes the UHI and underpredicts nighttime BLH over urban and suburban sites, leading to large overestimation of nocturnal CO2 mixing ratio at the suburban sites (bias of +17 ppm). The agreement between observation and prediction for BLH and CO2 concentrations and urban–rural increments, both day and night, demonstrates the potential of using the urban mesoscale system in the context of inverse modelling
Our ability to predict future climate change relies on our understanding of current and future CO2 fluxes, particularly on a regional scale (100-1000 km). CO2 regional sources and sinks are still ...poorly understood. Inverse transport modeling, a method often used to quantify these fluxes, relies on atmospheric CO2 measurements. One of the main challenges for the transport models used in the inversions is to properly reproduce CO2 vertical gradients between the boundary layer and the free troposphere, as these gradients impact on the partitioning of the calculated fluxes between the different model regions. Vertical CO2 profiles are very well suited to assess the performances of the models. In this paper, we conduct a comparison between observed and modeled CO2 profiles recorded during two CAATER campaigns that occurred in May 2001 and October 2002 over Western Europe, as described in a companion paper. We test different combinations between a global transport model (LMDZt), a mesoscale transport model (CHIMERE), and different sets of biospheric fluxes, all chosen with a diurnal cycle (CASA, SiB2 and ORCHIDEE). The vertical profile comparison shows that: 1) in most cases the influence of the biospheric flux is small but sometimes not negligible, ORCHIDEE giving the best results in the present study; 2) LMDZt is most of the time too diffuse, as it simulates a too high boundary layer height; 3) CHIMERE better reproduces the observed gradients between the boundary layer and the free troposphere, but is sometimes too variable and gives rise to incoherent structures. We conclude there is a need for more vertical profiles to conduct further studies to improve the parameterization of vertical transport in the models used for CO2 flux inversions. Furthermore, we use a modeling method to quantify CO2 fluxes at the regional scale from a chosen observing point, coupling influence functions from the transport model LMDZt (that works quite well at the synoptic scale) with information on the space-time distribution of fluxes. This modeling method is compared to a dual tracer method (the so-called Radon method) for a case study on 25 May 2001 during which simultaneous well-correlated in situ CO2 and Radon 222 measurements have been collected. Both methods give a similar result: a flux within the Radon 222 method uncertainty (35%), that is an atmospheric CO2 sink of -4.2 to -4.4 gC m-2 day-1 . We have estimated the uncertainty of the modeling method to be at least 33% on average, and even more for specific individual events. This method allows the determination of the area that contributed to the CO2 observed concentration. In our case, the observation point located at 1700 m a.s.l. in the north of France, is influenced by an area of 1500×700 km2 that covers the Benelux region, part of Germany and western Poland. Furthermore, this method allows deconvolution between the different contributing fluxes. In this case study, the biospheric sink contributes 73% of the total flux, fossil fuel emissions for 27%, the oceanic flux being negligible. However, the uncertainties of the influence function method need to be better assessed. This could be possible by applying it to other cases where the calculated fluxes can be checked independently, for example at tall towers where simultaneous CO2 and Radon 222 measurements can be conducted. The use of optimized fluxes (from atmospheric inversions) and of mesoscale models for atmospheric transport may also significantly reduce the uncertainties.
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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