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On the radiative impact of aerosols on photolysis rates: comparison of simulations and observations in the Lampedusa island during the ChArMEx/ADRIMED campaign

The Mediterranean basin is characterized by large concentrations of aerosols from both natural and anthropogenic sources. These aerosols affect tropospheric photochemistry by modulating the photolytic rates. Three simulations of the atmospheric composition at basin scale have been performed with the CHIMERE chemistry-transport model for the period from 6 June to 15 July 2013 covered by the ADRIMED campaign, a campaign of intense measurements in the western Mediterranean basin. One simulation takes into account the radiative effect of the aerosols on photochemistry, the second one does not, and the third one is designed to quantify the model sensitivity to a bias in the ozone column. These simulations are compared to satellite and ground-based measurements, with a particular focus on the area of Lampedusa. Values of the aerosol optical depth (AOD) are obtained from the MODIS instrument on the AQUA and TERRA satellites as well as from stations in the AERONET network and from the MFRSR sun photometer deployed at Lampedusa. Additional measurements from instruments deployed at Lampedusa either permanently or exceptionally are used for other variables: MFRSR sun photometer for AOD, diode array spectrometer for actinic fluxes, LIDAR for the aerosol backscatter, sequential sampler for speciation of aerosol and Brewer spectrophotometer for the total ozone column. It is shown that CHIMERE has a significant ability to reproduce observed peaks in the AOD, which in Lampedusa are mainly due to dust outbreaks during the ADRIMED period, and that taking into account the radiative effect of the aerosols in CHIMERE considerably improves the ability of the model to reproduce the observed day-to-day variations of the photolysis rate of ozone to O2 and O(1D), J(O1D), and that of NO2 to NO and O(3P), J(NO2). While in the case of J(O1D) other variation factors such as the stratospheric ozone column are very important in representing correctly the day-to-day variations, the day-to-day variations of J(NO2) are captured almost completely by the model when the optical effects of the aerosols are taken into account. Finally, it is shown that the inclusion of the direct radiative effect of the aerosols in the CHIMERE model leads to reduced J(O1D) and J(NO2) values over all the simulation domain, which range from a few percents over continental Europe and the north-east Atlantic Ocean to about 20 % close to and downwind from Saharan dust sources. The effect on the modelled ozone concentration is 2-fold: the effect of aerosols leads to reduced ozone concentrations over the Mediterranean Sea and continental Europe, close to the sources of NOx, but it also leads to increased ozone concentrations over remote areas such as the Sahara and the tropical Atlantic Ocean.
Evaluation of VIIRS, GOCI, and MODIS Collection 6 AOD retrievals against ground sunphotometer observations over East Asia

Persistent high aerosol loadings together with extremely high population densities have raised serious air quality and public health concerns in many urban centers in East Asia. However, ground-based air quality monitoring is relatively limited in this area. Recently, satellite-retrieved Aerosol Optical Depth (AOD) at high resolution has become a powerful tool to characterize aerosol patterns in space and time. Using ground AOD observations from the Aerosol Robotic Network (AERONET) and the Distributed Regional Aerosol Gridded Observation Networks (DRAGON)-Asia Campaign, as well as from handheld sunphotometers, we evaluated emerging aerosol products from the Visible Infrared Imaging Radiometer Suite (VIIRS) aboard the Suomi National Polar-orbiting Partnership (S-NPP), the Geostationary Ocean Color Imager (GOCI) aboard the Communication, Ocean, and Meteorology Satellite (COMS), and Terra and Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) (Collection 6) in East Asia in 2012 and 2013. In the case study in Beijing, when compared with AOD observations from handheld sunphotometers, 51 % of VIIRS Environmental Data Record (EDR) AOD, 37 % of GOCI AOD, 33 % of VIIRS Intermediate Product (IP) AOD, 26 % of Terra MODIS C6 3 km AOD, and 16 % of Aqua MODIS C6 3 km AOD fell within the reference expected error (EE) envelope (±0.05 ± 0.15 AOD). Comparing against AERONET AOD over the Japan–South Korea region, 64 % of EDR, 37 % of IP, 61 % of GOCI, 39 % of Terra MODIS, and 56 % of Aqua MODIS C6 3 km AOD fell within the EE. In general, satellite aerosol products performed better in tracking the day-to-day variability than tracking the spatial variability at high resolutions. The VIIRS EDR and GOCI products provided the most accurate AOD retrievals, while VIIRS IP and MODIS C6 3 km products had positive biases.
Constraining condensed-phase formation kinetics of secondary organic aerosol components from isoprene epoxydiols

Isomeric epoxydiols from isoprene photooxidation (IEPOX) have been shown to produce substantial amounts of secondary organic aerosol (SOA) mass and are therefore considered a major isoprene-derived SOA precursor. Heterogeneous reactions of IEPOX on atmospheric aerosols form various aerosol-phase components or "tracers" that contribute to the SOA mass burden. A limited number of the reaction rate constants for these acid-catalyzed aqueous-phase tracer formation reactions have been constrained through bulk laboratory measurements. We have designed a chemical box model with multiple experimental constraints to explicitly simulate gas- and aqueous-phase reactions during chamber experiments of SOA growth from IEPOX uptake onto acidic sulfate aerosol. The model is constrained by measurements of the IEPOX reactive uptake coefficient, IEPOX and aerosol chamber wall losses, chamber-measured aerosol mass and surface area concentrations, aerosol thermodynamic model calculations, and offline filter-based measurements of SOA tracers. By requiring the model output to match the SOA growth and offline filter measurements collected during the chamber experiments, we derive estimates of the tracer formation reaction rate constants that have not yet been measured or estimated for bulk solutions.
Aerosol size distribution seasonal characteristics measured in Tiksi, Russian Arctic

Four years of continuous aerosol number size distribution measurements from the Arctic Climate Observatory in Tiksi, Russia, are analyzed. Tiksi is located in a region where in situ information on aerosol particle properties has not been previously available. Particle size distributions were measured with a differential mobility particle sizer (in the diameter range of 7–500 nm) and with an aerodynamic particle sizer (in the diameter range of 0.5–10 μm). Source region effects on particle modal features and number, and mass concentrations are presented for different seasons. The monthly median total aerosol number concentration in Tiksi ranges from 184 cm−3 in November to 724 cm−3 in July, with a local maximum in March of 481 cm−3. The total mass concentration has a distinct maximum in February–March of 1.72–2.38 μg m−3 and two minimums in June (0.42 μg m−3) and in September–October (0.36–0.57 μg m−3). These seasonal cycles in number and mass concentrations are related to isolated processes and phenomena such as Arctic haze in early spring, which increases accumulation and coarse-mode numbers, and secondary particle formation in spring and summer, which affects the nucleation and Aitken mode particle concentrations. Secondary particle formation was frequently observed in Tiksi and was shown to be slightly more common in marine, in comparison to continental, air flows. Particle formation rates were the highest in spring, while the particle growth rates peaked in summer. These results suggest two different origins for secondary particles, anthropogenic pollution being the important source in spring and biogenic emissions being significant in summer. The impact of temperature-dependent natural emissions on aerosol and cloud condensation nuclei numbers was significant: the increase in both the particle mass and the CCN (cloud condensation nuclei) number with temperature was found to be higher than in any previous study done over the boreal forest region. In addition to the precursor emissions of biogenic volatile organic compounds, the frequent Siberian forest fires, although far away, are suggested to play a role in Arctic aerosol composition during the warmest months. Five fire events were isolated based on clustering analysis, and the particle mass and cloud condensation nuclei number were shown to be somewhat affected by these events. In addition, during calm and cold months, aerosol concentrations were occasionally increased by local aerosol sources in trapping inversions. These results provide valuable information on interannual cycles and sources of Arctic aerosols.
Estimates of European uptake of CO2 inferred from GOSAT XCO2 retrievals: sensitivity to measurement bias inside and outside Europe

Estimates of the natural CO2 flux over Europe inferred from in situ measurements of atmospheric CO2 mole fraction have been used previously to check top-down flux estimates inferred from space-borne dry-air CO2 column (XCO2) retrievals. Several recent studies have shown that CO2 fluxes inferred from XCO2 data from the Japanese Greenhouse gases Observing SATellite (GOSAT) and the Scanning Imaging Absorption Spectrometer for Atmospheric CHartographY (SCIAMACHY) have larger seasonal amplitudes and a more negative annual net CO2 balance than those inferred from the in situ data. The cause of this elevated European uptake of CO2 is still unclear, but some recent studies have suggested that this is a genuine scientific phenomenon. Here, we put forward an alternative hypothesis and show that realistic levels of bias in GOSAT data can result in an erroneous estimate of elevated uptake over Europe. We use a global flux inversion system to examine the relationship between measurement biases and estimates of CO2 uptake from Europe. We establish a reference in situ inversion that uses an Ensemble Kalman Filter (EnKF) to assimilate conventional surface mole fraction observations and XCO2 retrievals from the surface-based Total Carbon Column Observing Network (TCCON). We use the same EnKF system to assimilate two independent versions of GOSAT XCO2 data. We find that the GOSAT-inferred European terrestrial biosphere uptake peaks during the summer, similar to the reference inversion, but the net annual flux is 1.40 ± 0.19 GtC a−1 compared to a value of 0.58 ± 0.14 GtC a−1 for our control inversion that uses only in situ data. To reconcile these two estimates, we perform a series of numerical experiments that assimilate observations with added biases or assimilate synthetic observations for which part or all of the GOSAT XCO2 data are replaced with model data. We find that for our global flux inversions, a large portion (60–90 %) of the elevated European uptake inferred from GOSAT data in 2010 is due to retrievals outside the immediate European region, while the remainder can largely be explained by a sub-ppm retrieval bias over Europe. We use a data assimilation approach to estimate monthly GOSAT XCO2 biases from the joint assimilation of in situ observations and GOSAT XCO2 retrievals. The inferred biases represent an estimate of systematic differences between GOSAT XCO2 retrievals and the inversion system at regional or sub-regional scales. We find that a monthly varying bias of up to 0.5 ppm can explain an overestimate of the annual sink of up to 0.20 GtC a−1. Our results highlight the sensitivity of CO2 flux estimates to regional observation biases, which have not been fully characterized by the current observation network. Without further dedicated measurements we cannot prove or disprove that European ecosystems are taking up a larger-than-expected amount of CO2. More robust inversion systems are also needed to infer consistent fluxes from multiple observation types.
Seasonal variations of ultra-fine and submicron aerosols in Taipei, Taiwan: implications for particle formation processes in a subtropical urban area

The aim of this study is to investigate the seasonal variations in the physicochemical properties of atmospheric ultra-fine particles (UFPs, d ≤ 100 nm) and submicron particles (PM1, d ≤ 1 µm) in an east Asian urban area, which are hypothesized to be affected by the interchange of summer and winter monsoons. An observation experiment was conducted at TARO (Taipei Aerosol and Radiation Observatory), an urban aerosol station in Taipei, Taiwan, from October 2012 to August 2013. The measurements included the mass concentration and chemical composition of UFPs and PM1, as well as the particle number concentration (PNC) and the particle number size distribution (PSD) with size range of 4–736 nm. The results indicated that the mass concentration of PM1 was elevated during cold seasons with a peak level of 18.5 µg m−3 in spring, whereas the highest concentration of UFPs was measured in summertime with a mean of 1.64 µg m−3. Moreover, chemical analysis revealed that the UFPs and PM1 were characterized by distinct composition; UFPs were composed mostly of organics, whereas ammonium and sulfate were the major constituents of PM1. The seasonal median of total PNCs ranged from 13.9  ×  103 cm−3 in autumn to 19.4  ×  103 cm−3 in spring. Median concentrations for respective size distribution modes peaked in different seasons. The nucleation-mode PNC (N4 − 25) peaked at 11.6  ×  103 cm−3 in winter, whereas the Aitken-mode (N25 − 100) and accumulation-mode (N100 − 736) PNC exhibited summer maxima at 6.0  ×  103 and 3.1  ×  103 cm−3, respectively. The change in PSD during summertime was attributed to the enhancement in the photochemical production of condensable organic matter that, in turn, contributed to the growth of aerosol particles in the atmosphere. In addition, clear photochemical production of particles was observed, mostly in the summer season, which was characterized by average particle growth and formation rates of 4.0 ± 1.1 nm h−1 and 1.4 ± 0.8 cm−3 s−1, respectively. The prevalence of new particle formation (NPF) in summer was suggested as a result of seasonally enhanced photochemical oxidation of SO2 that contributed to the production of H2SO4, and a low level of PM10 (d ≤ 10 µm) that served as the condensation sink. Regarding the sources of aerosol particles, correlation analysis of the PNCs against NOx revealed that the local vehicular exhaust was the dominant contributor of the UFPs throughout the year. Conversely, the Asian pollution outbreaks had significant influence in the PNC of accumulation-mode particles during the seasons of winter monsoons. The results of this study implied the significance of secondary organic aerosols in the seasonal variations of UFPs and the influences of continental pollution outbreaks in the downwind areas of Asian outflows.
Observed high-altitude warming and snow cover retreat over Tibet and the Himalayas enhanced by black carbon aerosols

Himalayan mountain glaciers and the snowpack over the Tibetan Plateau provide the headwater of several major rivers in Asia. In situ observations of snow cover extent since the 1960s suggest that the snowpack in the region have retreated significantly, accompanied by a surface warming of 2–2.5 °C observed over the peak altitudes (5000 m). Using a high-resolution ocean–atmosphere global climate model and an observationally constrained black carbon (BC) aerosol forcing, we attribute the observed altitude dependence of the warming trends as well as the spatial pattern of reductions in snow depths and snow cover extent to various anthropogenic factors. At the Tibetan Plateau altitudes, the increase in atmospheric CO2 concentration exerted a warming of 1.7 °C, BC 1.3 °C where as cooling aerosols cause about 0.7 °C cooling, bringing the net simulated warming consistent with the anomalously large observed warming. We therefore conclude that BC together with CO2 has contributed to the snow retreat trends. In particular, BC increase is the major factor in the strong elevation dependence of the observed surface warming. The atmospheric warming by BC as well as its surface darkening of snow is coupled with the positive snow albedo feedbacks to account for the disproportionately large role of BC in high-elevation regions. These findings reveal that BC impact needs to be properly accounted for in future regional climate projections, in particular on high-altitude cryosphere.
Oil and gas impacts on air quality in federal lands in the Bakken region: an overview of the Bakken Air Quality Study and first results

The Bakken formation contains billions of barrels of oil and gas trapped in rock and shale. Horizontal drilling and hydraulic fracturing methods have allowed for extraction of these resources, leading to exponential growth of oil production in the region over the past decade. Along with this development has come an increase in associated emissions to the atmosphere. Concern about potential impacts of these emissions on federal lands in the region prompted the National Park Service to sponsor the Bakken Air Quality Study over two winters in 2013–2014. Here we provide an overview of the study and present some initial results aimed at better understanding the impact of local oil and gas emissions on regional air quality. Data from the study, along with long-term monitoring data, suggest that while power plants are still an important emissions source in the region, emissions from oil and gas activities are impacting ambient concentrations of nitrogen oxides and black carbon and may dominate recent observed trends in pollutant concentrations at some of the study sites. Measurements of volatile organic compounds also definitively show that oil and gas emissions were present in almost every air mass sampled over a period of more than 4 months.
Observed spatiotemporal variability of boundary-layer turbulence over flat, heterogeneous terrain

In the spring of 2013, extensive measurements with multiple Doppler lidar systems were performed. The instruments were arranged in a triangle with edge lengths of about 3 km in a moderately flat, agriculturally used terrain in northwestern Germany. For 6 mostly cloud-free convective days, vertical velocity variance profiles were calculated. Weighted-averaged surface fluxes proved to be more appropriate than data from individual sites for scaling the variance profiles; but even then, the scatter of profiles was mostly larger than the statistical error. The scatter could not be explained by mean wind speed or stability, whereas time periods with significantly increased variance contained broader thermals. Periods with an elevated maximum of the variance profiles could also be related to broad thermals. Moreover, statistically significant spatial differences of variance were found. They were not influenced by the existing surface heterogeneity. Instead, thermals were preserved between two sites when the travel time was shorter than the large-eddy turnover time. At the same time, no thermals passed for more than 2 h at a third site that was located perpendicular to the mean wind direction in relation to the first two sites. Organized structures of turbulence with subsidence prevailing in the surroundings of thermals can thus partly explain significant spatial variance differences existing for several hours. Therefore, the representativeness of individual variance profiles derived from measurements at a single site cannot be assumed.
PLAM – a meteorological pollution index for air quality and its applications in fog-haze forecasts in North China

Using surface meteorological observation and high-resolution emission data, this paper discusses the application of the PLAM/h index (Parameter Linking Air-quality to Meteorological conditions/haze) in the prediction of large-scale low visibility and fog-haze events. Based on the two-dimensional probability density function diagnosis model for emissions, the study extends the diagnosis and prediction of the meteorological pollution index PLAM to the regional visibility fog-haze intensity. The results show that combining the influence of regular meteorological conditions and emission factors together in the PLAM/h parameterization scheme is very effective in improving the diagnostic identification ability of the fog-haze weather in North China. The determination coefficients for four seasons (spring, summer, autumn, and winter) between PLAM/h and visibility observation are 0.76, 0.80, 0.96, and 0.86, respectively, and all of their significance levels exceed 0.001, showing the ability of PLAM/h to predict the seasonal changes and differences of fog-haze weather in the North China region. The high-value correlation zones are located in Jing-Jin-Ji (Beijing, Tianjin, Hebei), Bohai Bay rim, and southern Hebei–northern Henan, indicating that the PLAM/h index is related to the distribution of frequent heavy fog-haze weather in North China and the distribution of emission high-value zone. Through comparative analysis of the heavy fog-haze events and large-scale clear-weather processes in winter and summer, it is found that PLAM/h index 24 h forecast is highly correlated with the visibility observation. Therefore, the PLAM/h index has good capability in identification, analysis, and forecasting.