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The ADRIMED campaign provides measurements of all key parameters regarding atmospheric composition in the Mediterranean area during the summer 2013. This is an opportunity to quantify the ability of current models to adequately represent the atmospheric composition in this complex region, which is influenced by anthropogenic emissions from Europe, Africa, the Middle-East and from shipping activities as well as mineral dust emissions mostly from the arid areas in Africa, sea-salt emissions, biomass burning emissions and biogenic emissions from the vegetation. The CHIMERE model in its present version is a chemistry-transport model which takes into account all these processes. We show here by simulating the period from 5 June to 15 July 2013 with the CHIMERE model and comparing the results to both routine and specific ADRIMED measurements that this model allows an adequate representation the atmospheric composition over the western Mediterranean, in terms of ozone concentration, particulate matter (PM) and aerosol optical depth (AOD). It is also shown that the concentrations of PM on all the considered area is dominated by mineral dust, even though local dust emissions in Europe are certainly overestimated by the model. A comparison with sulphate concentrations at Cape Corsica exhibits some discrepancies related to the regridding of shipping emissions.
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The aerosol radiative effect in the long-wave (LW) spectral range is sometimes not taken into account in atmospheric aerosol forcing studies at local scale because the LW aerosol effect is assumed to be negligible. At regional and global scale this effect is partially taken into account: aerosol absorption is taken into account but scattering is still neglected. However, aerosols with strong absorbing and scattering properties in the LW region, like mineral dust, can have a non-negligible radiative effect in the LW spectral range (both at surface and top of the atmosphere) which can counteract their cooling effect occurring in the short-wave spectral range. The first objective of this research is to perform a sensitivity study of mineral dust LW radiative forcing (RF) as a function of dust microphysical and optical properties using an accurate radiative transfer model which can compute vertically resolved short-wave and long-wave aerosol RF. Radiative forcing simulations in the LW range have shown an important sensitivity to the following parameters: aerosol load, radius of the coarse mode, refractive index, aerosol vertical distribution, surface temperature and surface albedo. The scattering effect has been estimated to contribute to the LW RF up to 18% at the surface and up to 38% at the top of the atmosphere. The second objective is the estimation of the short-wave and long-wave dust RF for 11 dust outbreaks observed in Barcelona. At the surface, the LW RF varies between +2.8 and +10.2 W m<sup>−2</sup>, which represents between 11 and 26% (with opposite sign) of the SW component, while at the top of the atmosphere the LW RF varies between +0.6 and +5.8 W m<sup>−2</sup>, which represents between 6 and 26% (with opposite sign) of the SW component.
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The predictions of two road dust suspension emission models were compared with the on-site mobile measurements of suspension emission factors. Such a quantitative comparison has not previously been reported in the reviewed literature. The models used were the Nordic collaboration model NORTRIP (NOn-exhaust Road TRaffic Induced Particle emissions) and the Swedish–Finnish FORE model (Forecasting Of Road dust Emissions). These models describe particulate matter generated by the wear of road surface due to traction control methods and processes that control the suspension of road dust particles into the air. An experimental measurement campaign was conducted using a mobile laboratory called SNIFFER, along two selected road segments in central Helsinki in 2007 and 2008. The suspended PM<sub>10</sub> concentration was measured behind the left rear tyre and the street background PM<sub>10</sub> concentration in front of the van. Both models reproduced the measured seasonal variation of suspension emission factors fairly well during both years at both measurement sites. However, both models substantially under-predicted the measured emission values. The article illustrates the challenges in conducting road suspension measurements in densely trafficked urban conditions, and the numerous requirements for input data that are needed for accurately applying road suspension emission models.
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The mixed-phase relative rates approach for determining aerosol particle organic heterogeneous reaction kinetics is often performed utilizing mass spectral tracers as a proxy for particle-phase reactant concentration. However, this approach may be influenced by signal contamination from oxidation products during the experiment. In the current study, the mixed-phase relative rates technique has been improved by combining a positive matrix factor (PMF) analysis with electron ionization aerosol mass spectrometry (unit-mass resolution), thereby removing the influence of <i>m / z</i> fragments from reaction products on the reactant signals. To demonstrate the advantages of this approach, the heterogeneous reaction between OH radicals and citric acid (CA) was investigated using a photochemical flow tube coupled to a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS). The measured heterogeneous rate constant (<i>k</i><sub>2</sub>) of citric acid toward OH was (3.31 ± 0.29) × 10<sup>−12</sup> cm<sup>3</sup> molecule<sup>−1</sup> s<sup>−1</sup> at 298 K and (30 ± 3)% relative humidity (RH) and was several times greater than the results utilizing individual <i>m / z</i> fragments. This phenomenon was further evaluated for particulate-phase organophosphates (triphenyl phosphate (TPhP), tris-1,3-dichloro-2-propyl phosphate (TDCPP) and tris-2-ethylhexyl phosphate (TEHP)), leading to <i>k</i><sub>2</sub> values significantly larger than previously reported. The results suggest that heterogeneous kinetics can be significantly underestimated when the structure of the products is highly similar to the reactant and when a non-molecular tracer is measured with a unit-mass resolution aerosol mass spectrometer. The results also suggest that the heterogeneous lifetime of organic aerosol in models can be overestimated due to underestimated OH uptake coefficients. Finally, a comparison of reported rate constants implies that the heterogeneous oxidation of aerosols will be dependent upon a number of factors related to the reaction system, and that a single rate constant for one system cannot be universally applied under all conditions.
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Despite the developments in the global modelling of chemistry and of the parameterization of the physical processes, carbon monoxide (CO) concentrations remain underestimated during Northern Hemisphere (NH) winter by most state-of-the-art chemistry transport models. The consequential model bias can in principle originate from either an underestimation of CO sources or an overestimation of its sinks. We address both the role of surface sources and sinks with a series of MOZART (Model for Ozone And Related Tracers) model sensitivity studies for the year 2008 and compare our results to observational data from ground-based stations, satellite observations, and vertical profiles from measurements on passenger aircraft. In our base case simulation using MACCity (Monitoring Atmospheric Composition and Climate project) anthropogenic emissions, the near-surface CO mixing ratios are underestimated in the Northern Hemisphere by more than 20 ppb from December to April, with the largest bias of up to 75 ppb over Europe in January. An increase in global biomass burning or biogenic emissions of CO or volatile organic compounds (VOCs) is not able to reduce the annual course of the model bias and yields concentrations over the Southern Hemisphere which are too high. Raising global annual anthropogenic emissions with a simple scaling factor results in overestimations of surface mixing ratios in most regions all year round. Instead, our results indicate that anthropogenic CO and, possibly, VOC emissions in the MACCity inventory are too low for the industrialized countries only during winter and spring. Reasonable agreement with observations can only be achieved if the CO emissions are adjusted seasonally with regionally varying scaling factors. A part of the model bias could also be eliminated by exchanging the original resistance-type dry deposition scheme with a parameterization for CO uptake by oxidation from soil bacteria and microbes, which reduces the boreal winter dry deposition fluxes. The best match to surface observations, satellite retrievals, and aircraft observations was achieved when the modified dry deposition scheme was combined with increased wintertime road traffic emissions over Europe and North America (factors up to 4.5 and 2, respectively). One reason for the apparent underestimation of emissions may be an exaggerated downward trend in the Representative Concentration Pathway (RCP) 8.5 scenario in these regions between 2000 and 2010, as this scenario was used to extrapolate the MACCity emissions from their base year 2000. This factor is potentially amplified by a lack of knowledge about the seasonality of emissions. A methane lifetime of 9.7 yr for our basic model and 9.8 yr for the optimized simulation agrees well with current estimates of global OH, but we cannot fully exclude a potential effect from errors in the geographical and seasonal distribution of OH concentrations on the modelled CO.
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The Model of Emissions of Gases and Aerosols from Nature (MEGANv2.1) together with the Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields were used to create a global emission data set of biogenic volatile organic compounds (BVOC) available on a monthly basis for the time period of 1980–2010. This data set, developed under the Monitoring Atmospheric Composition and Climate project (MACC), is called MEGAN–MACC. The model estimated mean annual total BVOC emission of 760 Tg (C) yr<sup>−1</sup> consisting of isoprene (70%), monoterpenes (11%), methanol (6%), acetone (3%), sesquiterpenes (2.5%) and other BVOC species each contributing less than 2%. <br><br> Several sensitivity model runs were performed to study the impact of different model input and model settings on isoprene estimates and resulted in differences of up to ±17% of the reference isoprene total. A greater impact was observed for a sensitivity run applying parameterization of soil moisture deficit that led to a 50% reduction of isoprene emissions on a global scale, most significantly in specific regions of Africa, South America and Australia. <br><br> MEGAN–MACC estimates are comparable to results of previous studies. More detailed comparison with other isoprene inventories indicated significant spatial and temporal differences between the data sets especially for Australia, Southeast Asia and South America. MEGAN–MACC estimates of isoprene, α-pinene and group of monoterpenes showed a reasonable agreement with surface flux measurements at sites located in tropical forests in the Amazon and Malaysia. The model was able to capture the seasonal variation of isoprene emissions in the Amazon forest.
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A regional air quality simulation framework including the Weather Research and Forecasting modeling system (WRF), the Community Multi-scale Air Quality modeling system (CMAQ), and precursor emissions to simulate tropospheric ozone over South and East Asia is introduced. Concentrations of tropospheric ozone and related species simulated by the framework are validated by comparing with observation data of surface monitoring, ozonesondes, and satellites obtained in 2010. The simulation demonstrates acceptable performance on tropospheric ozone over South and East Asia at regional scale. Future energy consumption, carbon dioxide (CO<sub>2</sub>), nitrogen oxides (NO<sub>x</sub>), and volatile organic compound (VOC) emissions in 2030 under three future scenarios are estimated. One of the scenarios assumes a business-as-usual (BAU) pathway, and other two scenarios consider implementation of additional energy and environmental strategies to reduce energy consumption, CO<sub>2</sub>, NO<sub>x</sub>, and VOC emissions in China and India. Future surface ozone under these three scenarios is predicted by the simulation. The simulation indicates future surface ozone significantly increases around India for a whole year and around northeastern China in summer. NO<sub>x</sub> is a main driver on significant seasonal increase of surface ozone, whereas VOC as well as increasing background ozone and methane is also an important factor on annual average of surface ozone in East Asia. Warmer weather around India is also preferable for significant increase of surface ozone. Additional energy and environmental strategies assumed in future scenarios are expected to be effective to reduce future surface ozone over South and East Asia.
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Hourly measurements of elemental carbon (EC) and organic carbon (OC) were made at Mong Kok, a roadside air quality monitoring station in Hong Kong, for a year, from May 2011 to April 2012. The monthly average EC concentrations were 3.8–4.9 μg C m<sup>−3</sup>, accounting for 9.2–17.7% of the PM<sub>2.5</sub> mass (21.5–49.7 μg m<sup>−3</sup>). The EC concentrations showed little seasonal variation and peaked twice daily, coinciding with the traffic rush hours of a day. Strong correlations were found between EC and NO<sub>x</sub> concentrations, especially during the rush hours in the morning, confirming vehicular emissions as the dominant source of EC at this site. The analysis by means of the minimum OC / EC ratio approach to determine the OC / EC ratio representative of primary vehicular emissions yields a value of 0.5 for (OC / EC)<sub>vehicle</sub>. By applying the derived (OC / EC)<sub>vehicle</sub> ratio to the data set, the monthly average vehicle-related OC was estimated to account for 17–64% of the measured OC throughout the year. Vehicle-related OC was also estimated using receptor modeling of a combined data set of hourly NO<sub>x</sub>, OC, EC and volatile organic compounds characteristic of different types of vehicular emissions. The OC<sub>vehicle</sub> estimations by the two different approaches were in good agreement. When both EC and vehicle-derived organic matter (OM) (assuming an OM-to-OC ratio of 1.4) are considered, vehicular carbonaceous aerosols contributed ~ 7.3 μg m<sup>−3</sup> to PM<sub>2.5</sub>, accounting for ~ 20% of PM<sub>2.5</sub> mass (38.3 μg m<sup>−3</sup>) during winter, when Hong Kong received significant influence of air pollutants transported from outside, and ~ 30% of PM<sub>2.5</sub> mass (28.2 μg m<sup>−3</sup>) during summertime, when local emission sources were dominant. A reduction of 3.8 μg m<sup>−3</sup> in vehicular carbonaceous aerosols was estimated during 07:00–11:00 (i.e., rush hours on weekdays) on Sundays and public holidays. This could mainly be attributed to less on-road public transportation (e.g., diesel-powered buses) in comparison with non-holidays. These multiple lines of evidence confirm local vehicular emissions as an important source of PM<sub>2.5</sub> in an urban roadside environment and suggest the importance of vehicular emission control in reducing exposure to PM<sub>2.5</sub> in busy roadside environments.
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Previous studies showed that, over the global ocean, there is hemispheric asymmetry in aerosols and no noticeable asymmetry in cloud fraction (CF). In the current study, we focus on the tropical Atlantic (30° N–30° S) which is characterized by significant amounts of Saharan dust dominating other aerosol species over the North Atlantic. Over a limited area such as the tropical Atlantic, our study showed that strong meridional asymmetry in dust aerosols was accompanied by meridional CF asymmetry, by contrast to the global ocean. During the 10 yr study period (July 2002–June 2012), NASA Aerosol Reanalysis (aka MERRAero) showed that, when the meridional asymmetry in dust aerosol optical thickness (AOT) was the most pronounced (particularly in July), dust AOT averaged separately over the tropical North Atlantic was one order of magnitude higher than dust AOT averaged over the tropical South Atlantic. In the presence of such strong meridional asymmetry in dust AOT in July, CF averaged separately over the tropical North Atlantic exceeded CF averaged over the tropical South Atlantic by 20%. In July, along the Saharan Air Layer, Moderate Resolution Imaging Spectroradiometer (MODIS) CF data showed significant cloud cover (up to 0.8–0.9), which contributed to above-mentioned meridional CF asymmetry. Both Multi-Angle Imaging SpectroRadiometer (MISR) measurements and MERRAero data were in agreement on seasonal variations in meridional aerosol asymmetry. Meridional asymmetry in total AOT over the Atlantic was the most pronounced between March and July, when dust presence over the North Atlantic was maximal. In September and October, there was no noticeable meridional asymmetry in total AOT over the tropical Atlantic.
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The Arctic climate system includes numerous highly interactive small-scale physical processes in the atmosphere, sea ice, and ocean. During and since the International Polar Year 2007–2009, significant advances have been made in understanding these processes. Here, these recent advances are reviewed, synthesized, and discussed. In atmospheric physics, the primary advances have been in cloud physics, radiative transfer, mesoscale cyclones, coastal, and fjordic processes as well as in boundary layer processes and surface fluxes. In sea ice and its snow cover, advances have been made in understanding of the surface albedo and its relationships with snow properties, the internal structure of sea ice, the heat and salt transfer in ice, the formation of superimposed ice and snow ice, and the small-scale dynamics of sea ice. For the ocean, significant advances have been related to exchange processes at the ice–ocean interface, diapycnal mixing, double-diffusive convection, tidal currents and diurnal resonance. Despite this recent progress, some of these small-scale physical processes are still not sufficiently understood: these include wave–turbulence interactions in the atmosphere and ocean, the exchange of heat and salt at the ice–ocean interface, and the mechanical weakening of sea ice. Many other processes are reasonably well understood as stand-alone processes but the challenge is to understand their interactions with and impacts and feedbacks on other processes. Uncertainty in the parameterization of small-scale processes continues to be among the greatest challenges facing climate modelling, particularly in high latitudes. Further improvements in parameterization require new year-round field campaigns on the Arctic sea ice, closely combined with satellite remote sensing studies and numerical model experiments.
