Arctic haze is a seasonal phenomenon with high concentrations of accumulation-mode aerosols occurring in the Arctic in winter and early spring. Chemistry transport models and climate chemistry models ...struggle to reproduce this phenomenon, and this has recently prompted changes in aerosol removal schemes to remedy the modeling problems. In this paper, we show that shortcomings in current emission data sets are at least as important. We perform a 3 yr model simulation of black carbon (BC) with the Lagrangian particle dispersion model FLEXPART. The model is driven with a new emission data set ("ECLIPSE emissions") which includes emissions from gas flaring. While gas flaring is estimated to contribute less than 3% of global BC emissions in this data set, flaring dominates the estimated BC emissions in the Arctic (north of 66° N). Putting these emissions into our model, we find that flaring contributes 42% to the annual mean BC surface concentrations in the Arctic. In March, flaring even accounts for 52% of all Arctic BC near the surface. Most of the flaring BC remains close to the surface in the Arctic, so that the flaring contribution to BC in the middle and upper troposphere is small. Another important factor determining simulated BC concentrations is the seasonal variation of BC emissions from residential combustion (often also called domestic combustion, which is used synonymously in this paper). We have calculated daily residential combustion emissions using the heating degree day (HDD) concept based on ambient air temperature and compare results from model simulations using emissions with daily, monthly and annual time resolution. In January, the Arctic-mean surface concentrations of BC due to residential combustion emissions are 150% higher when using daily emissions than when using annually constant emissions. While there are concentration reductions in summer, they are smaller than the winter increases, leading to a systematic increase of annual mean Arctic BC surface concentrations due to residential combustion by 68% when using daily emissions. A large part (93%) of this systematic increase can be captured also when using monthly emissions; the increase is compensated by a decreased BC burden at lower latitudes. In a comparison with BC measurements at six Arctic stations, we find that using daily-varying residential combustion emissions and introducing gas flaring emissions leads to large improvements of the simulated Arctic BC, both in terms of mean concentration levels and simulated seasonality. Case studies based on BC and carbon monoxide (CO) measurements from the Zeppelin observatory appear to confirm flaring as an important BC source that can produce pollution plumes in the Arctic with a high BC / CO enhancement ratio, as expected for this source type. BC measurements taken during a research ship cruise in the White, Barents and Kara seas north of the region with strong flaring emissions reveal very high concentrations of the order of 200–400 ng m−3. The model underestimates these concentrations substantially, which indicates that the flaring emissions (and probably also other emissions in northern Siberia) are rather under- than overestimated in our emission data set. Our results suggest that it may not be "vertical transport that is too strong or scavenging rates that are too low" and "opposite biases in these processes" in the Arctic and elsewhere in current aerosol models, as suggested in a recent review article (Bond et al., Bounding the role of black carbon in the climate system: a scientific assessment, J. Geophys. Res., 2013), but missing emission sources and lacking time resolution of the emission data that are causing opposite model biases in simulated BC concentrations in the Arctic and in the mid-latitudes.
Non-exhaust traffic induced emissions are a major source of particle mass in most European countries. This is particularly important in Nordic and Alpine countries where winter time road traction ...maintenance occurs, e.g. salting and sanding, and where studded tyres are used. In this paper, Part 1, the road dust sub-model of a coupled road dust and surface moisture model (NORTRIP) is described. The model provides a generalised process based formulation of the non-exhaust emissions, with emphasis on the contribution of road wear, suspension, surface dust loading and the effect of road surface moisture (retention of wear particles and suspended emissions). The model is intended for use as a tool for air quality managers to help study the impact of mitigation measures and policies. We present a description of the road dust sub-model and apply the model to two sites in Stockholm and Copenhagen where seven years of data with surface moisture measurements are available. For the site in Stockholm, where studded tyres are in use, the model predicts the PM10 concentrations very well with correlations (R2) in the range of R2 = 0.76–0.91 for daily mean PM10. The model also reproduces well the impact of a reduction in studded tyres at this site. For the site in Copenhagen the correlation is lower, in the range 0.44–0.51. The addition of salt is described in the model and at both sites this leads to improved correlations due to additional salt emissions. For future use of the model a number of model parameters, e.g. wear factors and suspension rates, still need to be refined. The effect of sanding on PM10 emissions is also presented but more information will be required before this can be confidently applied for management applications.
•A coupled road dust and surface moisture model is presented and applied.•The surface moisture strongly determines the temporal variation of the road dust emissions.•The model predicts very well the temporal variation of suspended road dust emissions.•Time scales for suspension are significantly longer than previous estimates.•The model calculates the contribution of road salting to the emitted PM10 concentrations.
In this paper the European Monitoring and Evaluation Programme (EMEP) MSC‐W model is used to assess our understanding of the sources of carbonaceous aerosol in Europe (organic carbon (OC), elemental ...carbon (EC), or their sum, total carbon (TC)). The modeling work makes use of new data from two extensive measurement campaigns in Europe, those of the CARBOSOL project and of the EMEP EC/OC campaign. As well as EC and OC measurements, we are able to compare with levoglucosan, a tracer of wood‐burning emissions, and with the source apportionment (SA) analysis of Gelencsér et al. (2007), which apportioned TC into primary versus secondary and fossil fuel versus biogenic origin. The model results suggest that emissions of primary EC and OC from fossil fuel sources are probably captured to better than a factor of two at most sites. Discrepancies for wintertime OC at some sites can likely be accounted for in terms of missing wood‐burning contributions. Two schemes for secondary organic aerosol (SOA) contribution are included in the model, and we show that model results for TC are very sensitive to the choice of scheme. In northern Europe the model seems to capture TC levels rather well with either SOA scheme, but in southern Europe the model strongly underpredicts TC. Comparison against the SA results shows severe underprediction of the SOA components. This modeling work confirms the difficulties of modeling SOA in Europe, but shows that primary emissions constitute a significant fraction of ambient TC.
In this paper we describe and quality assure the sampling system of a mobile research laboratory SNIFFER which was shown to be a useful tool for studying emission levels of respirable dust from ...street surfaces. The dust plume had bimodal structure; another mode rising to higher altitudes whereas the other mode remained at lower altitudes. The system was tested on a route in Helsinki, Finland, during spring 2005 and 2006. The PM
2.5 and PM
10 were positively correlated and the PM levels increased with the vehicle speed. SNIFFER was able to identify the characteristic emission levels on different streets. A clear downward trend in the concentrations was observed in all street locations between April and June. The composition of the street dust collected by SNIFFER was compared with springtime PM
10 aerosol samples from the air quality monitoring stations in Helsinki. The results showed similarities in the abundance and composition of the mineral fraction but contained significantly more salt particles.
Non-exhaust traffic induced emissions are a major source of airborne particulate matter in most European countries. This is particularly important in Nordic and Alpine countries where winter time ...road traction maintenance occurs, e.g. salting and sanding, and where studded tyres are used. Though the total mass generated by wear sources is a key factor in non-exhaust emissions, these emissions are also strongly controlled by surface moisture conditions. In this paper, Part 2, the road surface moisture sub-model of a coupled road dust and surface moisture model (NORTRIP) is described. We present a description of the road surface moisture part of the model and apply the coupled model to seven sites in Stockholm, Oslo, Helsinki and Copenhagen over 18 separate periods, ranging from 3.5 to 24 months. At two sites surface moisture measurements are available and the moisture sub-model is compared directly to these observations. The model predicts the frequency of wet roads well at both sites, with an average fractional bias of −2.6%. The model is found to correctly predict the hourly surface state, wet or dry, 85% of the time. From the 18 periods modelled using the coupled model an average absolute fractional bias of 15% for PM10 concentrations was found. Similarly the model predicts the 90'th daily mean percentiles of PM10 with an average absolute bias of 19% and an average correlation (R2) of 0.49. When surface moisture is not included in the modelling then this average correlation is reduced to 0.16, demonstrating the importance of the surface moisture conditions. Tests have been carried out to assess the sensitivity of the model to model parameters and input data. The model provides a useful tool for air quality management and for improving our understanding of non-exhaust traffic emissions.
•A coupled road dust and surface moisture non-exhaust emission model is applied to seven sites over 18 different periods.•Surface moisture is shown to be the dominant cause of variability of the road dust emissions.•The model explains half the variability seen in roadside PM10 measurements.•Salt is found to have an impact on the surface moisture and on the variability of emissions.
The ability of seven state-of-the-art chemistry–aerosol models to reproduce distributions of tropospheric ozone and its precursors, as well as aerosols over eastern Asia in summer 2008, is evaluated. ...The study focuses on the performance of models used to assess impacts of pollutants on climate and air quality as part of the EU ECLIPSE project. Models, run using the same ECLIPSE emissions, are compared over different spatial scales to in situ surface, vertical profiles and satellite data. Several rather clear biases are found between model results and observations, including overestimation of ozone at rural locations downwind of the main emission regions in China, as well as downwind over the Pacific. Several models produce too much ozone over polluted regions, which is then transported downwind. Analysis points to different factors related to the ability of models to simulate VOC-limited regimes over polluted regions and NOx limited regimes downwind. This may also be linked to biases compared to satellite NO2, indicating overestimation of NO2 over and to the north of the northern China Plain emission region. On the other hand, model NO2 is too low to the south and west of this region and over South Korea/Japan. Overestimation of ozone is linked to systematic underestimation of CO particularly at rural sites and downwind of the main Chinese emission regions. This is likely to be due to enhanced destruction of CO by OH. Overestimation of Asian ozone and its transport downwind implies that radiative forcing from this source may be overestimated. Model-observation discrepancies over Beijing do not appear to be due to emission controls linked to the Olympic Games in summer 2008.With regard to aerosols, most models reproduce the satellite-derived AOD patterns over eastern China. Our study nevertheless reveals an overestimation of ECLIPSE model mean surface BC and sulphate aerosols in urban China in summer 2008. The effect of the short-term emission mitigation in Beijing is too weak to explain the differences between the models. Our results rather point to an overestimation of SO2 emissions, in particular, close to the surface in Chinese urban areas. However, we also identify a clear underestimation of aerosol concentrations over northern India, suggesting that the rapid recent growth of emissions in India, as well as their spatial extension, is underestimated in emission inventories. Model deficiencies in the representation of pollution accumulation due to the Indian monsoon may also be playing a role. Comparison with vertical aerosol lidar measurements highlights a general underestimation of scattering aerosols in the boundary layer associated with overestimation in the free troposphere pointing to modelled aerosol lifetimes that are too long. This is likely linked to too strong vertical transport and/or insufficient deposition efficiency during transport or export from the boundary layer, rather than chemical processing (in the case of sulphate aerosols). Underestimation of sulphate in the boundary layer implies potentially large errors in simulated aerosol–cloud interactions, via impacts on boundary-layer clouds.This evaluation has important implications for accurate assessment of air pollutants on regional air quality and global climate based on global model calculations. Ideally, models should be run at higher resolution over source regions to better simulate urban–rural pollutant gradients and/or chemical regimes, and also to better resolve pollutant processing and loss by wet deposition as well as vertical transport. Discrepancies in vertical distributions require further quantification and improvement since these are a key factor in the determination of radiative forcing from short-lived pollutants.
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 PM10 concentration was measured behind the left rear tyre and the street background PM10 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.
Surface analyses of atmospheric aerosols from different continental sources, such as forest fires and coal and straw burning, show that organic surfactants are found on such aerosols. The predominant ...organic species detected by time‐of‐flight secondary ion mass spectrometry on the sulfate aerosols are fatty acids of different carbon chain length up to the C32 acid. These observations are consistent with literature accounts of functional group analysis of bulk samples, but this is the first direct evidence of fatty acid films on the surface of sulfate aerosols. Surface analysis leads to the conclusion that fatty acid films on continental aerosols may be more common than has been previously suggested.
De-icing of road surfaces is necessary in many countries during winter to improve vehicle traction. Large amounts of salt, most often sodium chloride, are applied every year. Most of this salt is ...removed through drainage or traffic spray processes but a certain amount may be suspended, after drying of the road surface, into the air and will contribute to the concentration of particulate matter. Though some measurements of salt concentrations are available near roads, the link between road maintenance salting activities and observed concentrations of salt in ambient air is yet to be quantified. In this study the NORTRIP road dust emission model, which estimates the emissions of both dust and salt from the road surface, is applied at five sites in four Nordic countries for ten separate winter periods where daily mean ambient air measurements of salt concentrations are available. The model is capable of reproducing many of the salt emission episodes, both in time and intensity, but also fails on other occasions. The observed mean concentration of salt in PM10, over all ten datasets, is 4.2 μg/m3 and the modelled mean is 2.8 μg/m3, giving a fractional bias of −0.38. The RMSE of the mean concentrations, over all 10 datasets, is 2.9 μg/m3 with an average R2 of 0.28. The mean concentration of salt is similar to the mean exhaust contribution during the winter periods of 2.6 μg/m3. The contribution of salt to the kerbside winter mean PM10 concentration is estimated to increase by 4.1 ± 3.4 μg/m3 for every kg/m2 of salt applied on the road surface during the winter season. Additional sensitivity studies showed that the accurate logging of salt applications is a prerequisite for predicting salt emissions, as well as good quality data on precipitation. It also highlights the need for more simultaneous measurements of salt loading together with ambient air concentrations to help improve model parameterisations of salt and moisture removal processes.
•For the first time emissions of road salt have been modelled.•The model successfully reproduces many of the observational datasets.•Salt emissions in PM10, during winter, are as high as exhaust emissions.•A relationship between road salt application and concentrations is presented.
The global aerosol-climate model ECHAM-HAMMOZ was used to investigate changes in the aerosol burden and aerosol radiative effects in the coming decades. Four different emissions scenarios were ...applied for 2030 (two of them applied also for 2020) and the results were compared against the reference year 2005. Two of the scenarios are based on current legislation reductions: one shows the maximum potential of reductions that can be achieved by technical measures, and the other is targeted to short-lived climate forcers (SLCFs). We have analyzed the results in terms of global means and additionally focused on eight subregions. Based on our results, aerosol burdens show an overall decreasing trend as they basically follow the changes in primary and precursor emissions. However, in some locations, such as India, the burdens could increase significantly. The declining emissions have an impact on the clear-sky direct aerosol effect (DRE), i.e. the cooling effect. The DRE could decrease globally 0.06-0.4 W m-2 by 2030 with some regional increases, for example, over India (up to 0.84 W m-2). The global changes in the DRE depend on the scenario and are smallest in the targeted SLCF simulation. The aerosol indirect radiative effect could decline 0.25-0.82 W m-2 by 2030. This decrease takes place mostly over the oceans, whereas the DRE changes are greatest over the continents. Our results show that targeted emission reduction measures can be a much better choice for the climate than overall high reductions globally. Our simulations also suggest that more than half of the near-future forcing change is due to the radiative effects associated with aerosol-cloud interactions.
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