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Ozone and fine particle in the western Yangtze River Delta: an overview of 1 yr data at the SORPES station

This work presents an overview of 1 yr measurements of ozone (O3) and fine particular matter (PM2.5) and related trace gases at a recently developed regional background site, the Station for Observing Regional Processes of the Earth System (SORPES), in the western part of the Yangtze River Delta (YRD) in eastern China. Ozone and PM2.5 showed strong seasonal cycles but with contrast patterns: O3 reached a maximum in warm seasons but PM2.5 in cold seasons. Correlation analysis suggests a VOC-sensitive regime for O3 chemistry and a formation of secondary aerosols under conditions of high O3 in summer. Compared with the National Ambient Air Quality Standards in China, our measurements report 15 days of O3 exceedance and 148 days of PM2.5 exceedance during the 1 yr period, suggesting a severe air pollution situation in this region. Case studies for typical O3 and PM2.5 episodes demonstrated that these episodes were generally associated with an air mass transport pathway over the mid-YRD, i.e., along the Nanjing–Shanghai axis with its city clusters, and showed that synoptic weather played an important role in air pollution, especially for O3. Agricultural burning activities caused high PM2.5 and O3 pollution during harvest seasons, especially in June. A calculation of potential source contributions based on Lagrangian dispersion simulations suggests that emissions from the YRD contributed to over 70% of the O3 precursor CO, with a majority from the mid-YRD. North-YRD and the North China Plain are the main contributors to PM2.5 pollution in this region. This work shows an important environmental impact from industrialization and urbanization in the YRD region, and suggests an urgent need for improving air quality in these areas through collaborative control measures among different administrative regions.
Validation of MIPAS-ENVISAT H2O operational data collected between July 2002 and March 2004

Water vapour (H2O) is one of the operationally retrieved key species of the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument aboard the Environmental Satellite (ENVISAT) which was launched into its sun-synchronous orbit on 1 March 2002 and operated until April 2012. Within the MIPAS validation activities, independent observations from balloons, aircraft, satellites, and ground-based stations have been compared to European Space Agency (ESA) version 4.61 operational H2O data comprising the time period from July 2002 until March 2004 where MIPAS measured with full spectral resolution. No significant bias in the MIPAS H2O data is seen in the lower stratosphere (above the hygropause) between about 15 and 30 km. Differences of H2O quantities observed by MIPAS and the validation instruments are mostly well within the combined total errors in this altitude region. In the upper stratosphere (above about 30 km), a tendency towards a small positive bias (up to about 10%) is present in the MIPAS data when compared to its balloon-borne counterpart MIPAS-B, to the satellite instruments HALOE (Halogen Occultation Experiment) and ACE-FTS (Atmospheric Chemistry Experiment, Fourier Transform Spectrometer), and to the millimeter-wave airborne sensor AMSOS (Airborne Microwave Stratospheric Observing System). In the mesosphere the situation is unclear due to the occurrence of different biases when comparing HALOE and ACE-FTS data. Pronounced deviations between MIPAS and the correlative instruments occur in the lowermost stratosphere and upper troposphere, a region where retrievals of H2O are most challenging. Altogether it can be concluded that MIPAS H2O profiles yield valuable information on the vertical distribution of H2O in the stratosphere with an overall accuracy of about 10 to 30% and a precision of typically 5 to 15% – well within the predicted error budget, showing that these global and continuous data are very valuable for scientific studies. However, in the region around the tropopause retrieved MIPAS H2O profiles are less reliable, suffering from a number of obstacles such as retrieval boundary and cloud effects, sharp vertical discontinuities, and frequent horizontal gradients in both temperature and H2O volume mixing ratio (VMR). Some profiles are characterized by retrieval instabilities.
Black carbon physical properties and mixing state in the European megacity Paris

Aerosol hygroscopicity and refractory black carbon (rBC) properties were characterised during wintertime at a suburban site in Paris, one of the biggest European cities. Hygroscopic growth factor (GF) frequency distributions, characterised by distinct modes of more-hygroscopic background aerosol and non- or slightly hygroscopic aerosol of local (or regional) origin, revealed an increase of the relative contribution of the local sources compared to the background aerosol with decreasing particle size. BC-containing particles in Paris were mainly originating from fresh traffic emissions, whereas biomass burning only gave a minor contribution. The mass size distribution of the rBC cores peaked on average at an rBC core mass equivalent diameter of DMEV ~ 150 nm. The BC-containing particles were moderately coated (coating thickness Δcoat ~ 33 nm on average for rBC cores with DMEV = 180–280 nm) and an average mass absorption coefficient (MAC) of ~ 8.6 m2 g−1 at the wavelength λ = 880 nm was observed. Different time periods were selected to investigate the properties of BC-containing particles as a function of source and air mass type. The traffic emissions were found to be non-hygroscopic (GF ≈ 1.0), and essentially all particles with a dry mobility diameter (D0) larger than D0 = 110 nm contained an rBC core. rBC from traffic emissions was further observed to be uncoated within experimental uncertainty (Δcoat ~ 2 nm ± 10 nm), to have the smallest BC core sizes (maximum of the rBC core mass size distribution at DMEV ~ 100 nm) and to have the smallest MAC (~ 7.3 m2g−1 at λ = 880 nm). The biomass burning aerosol was slightly more hygroscopic than the traffic emissions (with a distinct slightly-hygroscopic mode peaking at GF ≈ 1.1–1.2). Furthermore, only a minor fraction (&leq; 10%) of the slightly-hygroscopic particles with 1.1 &leq; GF &leq; 1.2 (and D0 = 265 nm) contained a detectable rBC core. The BC-containing particles from biomass burning were found to have a medium coating thickness as well as slightly larger mean rBC core sizes and MAC values compared to traffic emissions. The aerosol observed under the influence of aged air masses and air masses from Eastern Continental Europe was dominated by a~more-hygroscopic mode peaking at GF ≈ 1.6. Most particles (95%), in the more-hygroscopic mode at D0 = 265 nm, did not contain a detectable rBC core. A significant fraction of the BC-containing particles had a substantial coating with non-refractory aerosol components. MAC values of ~ 8.8 m2g−1 and ~ 8.3 m2g−1 at λ = 880 nm and mass mean rBC core diameters of 150 nm and 200 nm were observed for the aged and continental air mass types, respectively. The reason for the larger rBC core sizes compared to the fresh emissions – transport effects or a different rBC source – remains unclear. The dominant fraction of the BC-containing particles was found to have no or very little coating with non-refractory matter. The lack of coatings is consistent with the observation that the BC-containing particles are non- or slightly-hygroscopic, which makes them poor cloud condensation nuclei. It can therefore be expected that wet removal through nucleation scavenging is inefficient for fresh BC-containing particles in urban plumes. The mixing-state-specific cloud droplet activation behaviour of BC-containing particles including the effects of atmospheric aging processes should be considered in global simulations of atmospheric BC, as the wet removal efficiency remains a major source of uncertainty in its life-cycle.
Modeling air pollution in Lebanon: evaluation at a suburban site in Beirut during summer

Beirut, the capital of Lebanon, which is located on the eastern shore of the Mediterranean basin, experiences high air pollution episodes. Annual average concentrations of coarse and fine particulate matter (PM2.5) as well as nitrogen oxides (NOx) often exceed the World Health Organization (WHO) guidelines. Therefore, improving air quality in this region is essential. The Polyphemus/Polair3D modeling system is used here to investigate air pollution episodes in Beirut during 2 to 18 July 2011. The modeling domain covers two nested grids of 1 and 5 km horizontal resolution over greater Beirut and Lebanon, respectively. The anthropogenic emission inventory was developed earlier (Waked et al., 2012). The Weather and Research Forecasting (WRF) model is used to generate the meteorological fields and the Model of Emissions of Gases and Aerosols from Nature (MEGAN) is used for biogenic emissions. The results of the study are compared to measurements from a field campaign conducted in the suburb of Beirut during 2–18 July 2011. The model reproduces satisfactorily the concentrations of most gaseous pollutants, the total mass of PM2.5 as well as PM2.5 elemental carbon (EC), organic carbon (OC), and sulfate. Ozone concentrations are overestimated and it appears that this overestimation results mainly from the boundary conditions.
Estimation of volatile organic compound emissions for Europe using data assimilation

The emissions of non-methane volatile organic compounds (VOCs) over western Europe for the year 2005 are estimated via inverse modelling by assimilation of in situ observations of concentration and then subsequently compared to a standard emission inventory. The study focuses on 15 VOC species: five aromatics, six alkanes, two alkenes, one alkyne and one biogenic diene. The inversion relies on a validated fast adjoint of the chemical transport model used to simulate the fate and transport of these VOCs. The assimilated ground-based measurements over Europe are provided by the European Monitoring and Evaluation Programme (EMEP) network. The background emission errors and the prior observational errors are estimated by maximum-likelihood approaches. The positivity assumption on the VOC emission fluxes is pivotal for a successful inversion, and this maximum-likelihood approach consistently accounts for the positivity of the fluxes. For most species, the retrieved emissions lead to a significant reduction of the bias, which underlines the misfit between the standard inventories and the observed concentrations. The results are validated through a forecast test and a cross-validation test. An estimation of the posterior uncertainty is also provided. It is shown that the statistically consistent non-Gaussian approach based on a reliable estimation of the errors offers the best performance. The efficiency in correcting the inventory depends on the lifetime of the VOCs and the accuracy of the boundary conditions. In particular, it is shown that the use of in situ observations using a sparse monitoring network to estimate emissions of isoprene is inadequate because its short chemical lifetime significantly limits the spatial radius of influence of the monitoring data. For species with a longer lifetime (a few days), successful, albeit partial, emission corrections can reach regions hundreds of kilometres away from the stations. Domain-wide corrections of the emission inventories of some VOCs are significant, with underestimations of the order of a factor of 2 for propane, ethane, ethylene and acetylene.
A functional group oxidation model (FGOM) for SOA formation and aging

Secondary organic aerosol (SOA) formation from a volatile organic compound (VOC) involves multiple generations of oxidation that include functionalization and fragmentation of the parent carbon backbone and likely particle-phase oxidation and/or accretion reactions. Despite the typical complexity of the detailed molecular mechanism of SOA formation and aging, a relatively small number of functional groups characterize the oxidized molecules that constitute SOA. Given the carbon number and set of functional groups, the volatility of the molecule can be estimated. We present here a functional group oxidation model (FGOM) that represents the process of SOA formation and aging. The FGOM contains a set of parameters that are to be determined by fitting of the model to laboratory chamber data: total organic aerosol concentration, and O : C and H : C atomic ratios. The sensitivity of the model prediction to variation of the adjustable parameters allows one to assess the relative importance of various pathways involved in SOA formation. An analysis of SOA formation from the high- and low-NOx photooxidation of four C12 alkanes (n-dodecane, 2-methylundecane, hexylcyclohexane, and cyclododecane) using the FGOM is presented, and comparison with the statistical oxidation model (SOM) of Cappa et al. (2013) is discussed.
Constraints on aerosol processes in climate models from vertically-resolved aircraft observations of black carbon

Evaluation of the aerosol schemes in current climate models is dependent upon the available observational data. In-situ observations from flight campaigns can provide valuable data about the vertical distribution of aerosol that is difficult to obtain from satellite or ground-based platforms, although they are localised in space and time. Using single-particle soot-photometer (SP2) measurements from the HIAPER Pole-to-Pole Observations (HIPPO) campaign, which consists of many vertical profiles over a large region of the Pacific, we evaluate the meridional and vertical distribution of black carbon (BC) aerosol simulated by the HadGEM3–UKCA and ECHAM5–HAM2 models. Both models show a similar pattern of overestimating the BC column burden compared to that derived from the observations, in many areas by an order of magnitude. However, by sampling the simulated BC mass mixing ratio along the flight track and comparing to the observations, we show that this discrepancy has a rather different vertical structure in the two models: in HadGEM3–UKCA the discrepancy is dominated by excess aerosol in the tropical upper troposphere, while in ECHAM5–HAM2 areas of discrepancy are spread across many different latitudes and altitudes. Using this methodology, we conduct sensitivity tests on two specific elements of the models: biomass-burning emissions and scavenging by convective precipitation. We show that, by coupling the convective scavenging more tightly with convective transport, both the column burden and vertical distribution of BC in HadGEM3–UKCA are much improved with respect to the observations, with a substantial and statistically significant increase in correlation – this demonstrates the importance of a realistic representation of this process. In contrast, updating from GFED2 to GFED3.1 biomass-burning emissions makes a more modest improvement in both models, which is not statistically significant. By comparing our results with a more traditional approach using regional- and monthly-mean vertical profile curves, we show that the point-by-point analysis allows the model improvements to be demonstrated more clearly. We also demonstrate the important role that nudged simulations (where the large-scale model dynamics are continuously relaxed towards a reanalysis) can play in this type of evaluation, allowing statistically significant differences between configurations of the aerosol scheme to be seen where the differences between the corresponding free-running simulations would not be significant.
Volcanic SO2 fluxes derived from satellite data: a survey using OMI, GOME-2, IASI and MODIS

Sulphur dioxide (SO2) fluxes of active degassing volcanoes are routinely measured with ground-based equipment to characterize and monitor volcanic activity. SO2 of unmonitored volcanoes or from explosive volcanic eruptions, can be measured with satellites. However, remote-sensing methods based on absorption spectroscopy generally provide integrated amounts of already dispersed plumes of SO2 and satellite derived flux estimates are rarely reported. Here we review a number of different techniques to derive volcanic SO2 fluxes using satellite measurements of plumes of SO2 and investigate the temporal evolution of the total emissions of SO2 for three very different volcanic events in 2011: Puyehue-Cordón Caulle (Chile), Nyamulagira (DR Congo) and Nabro (Eritrea). High spectral resolution satellite instruments operating both in the ultraviolet-visible (OMI/Aura and GOME-2/MetOp-A) and thermal infrared (IASI/MetOp-A) spectral ranges, and multispectral satellite instruments operating in the thermal infrared (MODIS/Terra-Aqua) are used. We show that satellite data can provide fluxes with a sampling of a day or less (few hours in the best case). Generally the flux results from the different methods are consistent, and we discuss the advantages and weaknesses of each technique. Although the primary objective of this study is the calculation of SO2 fluxes, it also enables us to assess the consistency of the SO2 products from the different sensors used.
Corrigendum to "Net radiative forcing and air quality responses to regional CO emission reductions" published in Atmos. Chem. Phys., 13, 5381–5399, 2013
Impact of the vertical emission profiles on background gas-phase pollution simulated from the EMEP emissions over Europe

Five one-year air quality simulations over a domain covering Europe have been performed using the CHIMERE chemistry transport model and the EMEP emission dataset for Europe. These five simulations differ only by the representation of the effective emission heights for anthropogenic emissions: one has been run using the EMEP standard recommendations, three others with vertical injection profiles derived from the EMEP recommendations but multiplying the injection height by 0.75, 0.50 and 0.25, respectively, while the last one uses vertical profiles derived from the recent literature. It is shown that using injection heights lower than the EMEP recommendations leads to significantly improved simulation of background SO2, NO2 and O3 concentrations when compared to the Airbase station measurements.