This paper investigates the impact of biogenic isoprene and terpene emissions on photochemical species levels in the French Ile‐de‐France region during several photooxidant pollution episodes in ...summer 1998 and 1999 during the Atmospheric Pollution Over the Paris Area (ESQUIF) project. The effect of biogenic emissions on both ozone produced on a continental scale and advected in Ile‐de‐France and on ozone locally formed are assessed. For this purpose, simulations with and without biogenic emissions are performed with a nested version of the CHIMERE model. This chemistry transport model includes both a continental (western European) domain with 0.5° horizontal resolution and a regional domain (Ile‐de‐France) of 150 × 150 km extension with a horizontal resolution of 6 km. An emissions database for biogenic isoprene and terpene emissions from forests has been set up. These emissions are estimated using emission factors for different tree species recently revised by Simpson et al. 1999 and for different land use data sets, including highly resolved (1 km) satellite measurements for Ile‐de‐France. Good agreement has been found between modeled and measured (by aircraft) isoprene levels (overall bias <10%), which lends confidence to the use of the emissions database for subsequent simulations. The comparison between runs with and without biogenic volatile organic compound (VOC) emissions indicates a significant difference in ozone in Ile‐de‐France, up to 40 ppb for one extreme day. Biogenic VOC emissions from Ile‐de‐France along with those from outside the Ile‐de‐France region have an approximately equal responsibility for the additional ozone buildup. The main reason for this increased ozone formation is the enhancement of radicals due to larger concentrations of carbonyl species and ozone and their subsequent photolysis. Biogenic emissions lead to a shift in the sensitivity to emissions (toward more “NOx‐limited”). However, generally, either with or without biogenic emissions, a “VOC‐limited” regime is simulated over the Ile‐de‐France region.
Due to its impact on environment, tropospheric ozone received particular attention since several decades. Ground‐based networks associated with regional chemical transport models are used to monitor ...and forecast surface ozone concentrations, but coverage, representativeness, and accuracy issues remain important. Recent satellite observations have demonstrated the capacity to probe tropospheric ozone, but there has been no explicit attempt to quantify their ability to measure ozone pollution near ground. We propose here to assess the ability of ozone sounders to detect a photochemical ozone pollution event that is supposed to be a favorable situation for satellite detection. We have chosen ozone pollution event over Europe associated with a warm conveyor belt that efficiently transports photochemically produced ozone upward. Ozone satellite products from Global Ozone Monitoring Experiment‐2, Infrared Atmospheric Sounding Interferometer (IASI), and Ozone Monitoring Instrument are analyzed here for their capacity to capture such an event. Also, in situ observations and regional chemical‐transport models show increasing ozone concentrations in the continental and Mediterranean boundary layer and further transport to central Europe and Scandinavia associated with upward transport. Satellite observations do not detect high ozone concentrations within the boundary layer due the weak sensitivity near the surface. Nevertheless, we have shown that the IR sounder IASI was able to detect, qualitatively and quantitatively, the ozone plume transported upward by the warm conveyor belt, suggesting that a quantification of upward transport of ozone pollution could be possible using current satellite observations. This should encourage us to further explore approaches more sensitive to surface ozone (such as the multispectral approach) and to prepare the next generation of still more sensitive spaceborne instruments.
Key Point
Ability of satellite to detect ozone pollution is evaluated
The content and evolution of brown carbon (BrC) in smokes from Siberian forest fires were analyzed using measurements of the aerosol absorption optical depth (AAOD) at three Russian AERONET stations ...located in Tomsk, Zvenigorod, and Yekaterinburg. Estimates are obtained of the relative contribution of BrC in fine aerosol particles to the absorption of solar radiation at a wavelength of 440 nm (η
BrC
) and, in particular, for an anomalous episode of long-range transport of smokes from Siberia to the European part of Russia in summer 2016. A considerable BrC content is found in smokes in Tomsk and Zvenigorod (where η
BrC
is estimated to be 15 and 18% on average). It is noteworthy that no significant η
BrC
values were revealed during passage of smokes from Siberian fires over Yekaterinburg. The η
BrC
values were found to decrease with aerosol aging under sunlit conditions on the characteristic timescale of about 30 h. At the same time, the measurements in Zvenigorod indicate that the absorption properties of the organic component of smoke aerosol increase during a much longer evolution.
In this paper, we examine the extent to which an ensemble generated from a single air quality model correctly represents the global uncertainty of ozone simulations with a regional scale ...chemistry-transport model and whether it is suitable for ozone data assimilation. An ensemble of 30 members is constructed from a reference simulation in which the model parameters that are the most uncertain for determining ozone concentrations are randomly perturbed. Comparisons of the simulated ensemble using the model CHIMERE with observations are examined over the summer season both at the surface and higher in the troposphere. Although the ensemble overestimates vertical and horizontal correlation between errors, the average model error is well represented both at the surface and in the vertical dimension (after an adjustment for the latter). A variability of about 7–8
ppb is found. The results found in this study with respect to tropospheric ozone model errors and error correlation lengths both from ensemble simulations and model to observation comparisons are of particular interest for data assimilation when constructing model error covariance matrices.
We present here the development and first field deployment of a novel Aircraft-based Laser ABlation Aerosol MAss spectrometer (ALABAMA), which is capable of measuring the chemical composition and ...size of individual ambient aerosol particles in the size range between 150 and 900 nm. The instrument uses a continuous wave 532 nm laser to size and detect the particles, a pulsed 266 nm laser to ablate and ionize the particles, and a bipolar, Z-shaped time-of-flight mass spectrometer to detect positive and negative ions. The ALABAMA fits into a 19"-aircraft rack of 150 cm height and has a total weight of 140 kg, thus currently being one of the smallest and lightest-weight instruments of its type. We present a detailed characterization of ALABAMA with respect to particle beam width, detection and ablation efficiency, and example mass spectra of different particle types. The first aircraft-based field mission was performed within the MEGAPOLI summer campaign in July 2009 around Paris, France, onboard an ATR42 aircraft. During 11 research flights, corresponding to a total measuring time of approximately 44 hours, ALABAMA measured 6502 single particle mass spectra. The mass spectra were classified into eight particle classes using distinctive markers for each particle type. The most abundant particle types contained organic and secondary inorganic compounds. The results further show that differences in the abundance of observed particle types between different air masses are very pronounced when comparing air masses arriving from the greater Paris area with air masses arriving from other directions.
For the investigation of megacity emission development and the impact outside the source region, mobile aerosol and trace gas measurements were carried out in the Paris metropolitan area between 1 ...July and 31 July 2009 (summer conditions) and 15 January and 15 February 2010 (winter conditions) in the framework of the European Union FP7 MEGAPOLI project. Two mobile laboratories, MoLa and MOSQUITA, were deployed, and here an overview of these measurements and an investigation of the applicability of such measurements for the analysis of megacity emissions are presented. Both laboratories measured physical and chemical properties of fine and ultrafine aerosol particles as well as gas phase constituents of relevance for urban pollution scenarios. The applied measurement strategies include cross-section measurements for the investigation of plume structure and quasi-Lagrangian measurements axially along the flow of the city's pollution plume to study plume aging processes. Results of intercomparison measurements between the two mobile laboratories represent the adopted data quality assurance procedures. Most of the compared measurement devices show sufficient agreement for combined data analysis. For the removal of data contaminated by local pollution emissions a video tape analysis method was applied. Analysis tools like positive matrix factorization and peak integration by key analysis applied to high-resolution time-of-flight aerosol mass spectrometer data are used for in-depth data analysis of the organic particulate matter. Several examples, including a combination of MoLa and MOSQUITA measurements on a cross section through the Paris emission plume, are provided to demonstrate how such mobile measurements can be used to investigate the emissions of a megacity. A critical discussion of advantages and limitations of mobile measurements for the investigation of megacity emissions completes this work.
It has been shown by numerical simulation that the rate of formation of secondary organic aerosols (SOAs) in smoke plumes caused by vegetation and peat fires under real conditions can significantly ...depend on the aerosol optical thickness (AOT). The AOT determines the photodissociation rate and hydroxyl radical concentration, which in turn determines the rate of SOA generation as a result of oxidation of semivolatile organic compounds. Quantitative analysis has been carried out for the situation that took place in European Russia during the 2010 Russian wildfires. The state-of-the-art 3D chemical transport model is used in this study; the simulations are optimized and validated using the data of monitoring of the particulate matter in the Moscow region and Finland. The findings indicate that it is important to allow for this effect in studies focused on the analysis and prediction of air pollution due to wildfires, as well as climate and weather studies, whose results may depend on the assumptions about the content and properties of atmospheric carbon-containing aerosol.
To evaluate the added value brought by the next generation of IASI (Infrared Atmospheric Sounder Interferometer) instruments to monitor lower tropospheric (LT) ozone, we developed a ...pseudo-observation simulator, including a direct simulator of thermal infrared spectra and a full inversion scheme to retrieve ozone concentration profiles. We based our simulations on the instrumental configuration of IASI and of an IASI-like instrument, with a factor 2 improvement in terms of spectral resolution and radiometric noise. This scenario, that will be referred to as IASI/2, is one possible configuration of the IASI-NG (New Generation) instrument (the configuration called IASI-NG/IRS2) currently designed by CNES (Centre National d'Études Spatiales). IASI-NG is expected to be launched in the 2020 timeframe as part of the EPS-SG (EUMETSAT Polar System-Second Generation, formerly post-EPS) mission. We produced one month (August 2009) of tropospheric ozone pseudo-observations based on these two instrumental configurations. We compared the pseudo-observations and we found a clear improvement of LT ozone (up to 6 km altitude) pseudo-observations quality for IASI/2. The estimated total error is expected to be more than 35% smaller at 5 km, and 20% smaller for the LT ozone column. The total error on the LT ozone column is, on average, lower than 10% for IASI/2. IASI/2 is expected to have a significantly better vertical sensitivity (monthly average degrees of freedom surface-6 km of 0.70) and to be sensitive at lower altitudes (more than 0.5 km lower than IASI, reaching nearly 3 km). Vertical ozone layers of 4 to 5 km thickness are expected to be resolved by IASI/2, while IASI has a vertical resolution of 6-8 km. According to our analyses, IASI/2 is expected to have the possibility of effectively separate lower from upper tropospheric ozone information even for low sensitivity scenarios. In addition, IASI/2 is expected to be able to better monitor LT ozone patterns at local spatial scale and to monitor abrupt temporal evolutions occurring at timescales of a few days, thus bringing an expected added value with respect to IASI for the monitoring of air quality.
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