Size-segregated chemical composition of aerosol emissions in an urban road tunnel in Portugal

An atmospheric aerosol study was performed in 2008 inside an urban road tunnel, in Lisbon, Portugal. Using a high volume impactor, the aerosol was collected into four size fractions (PM0.5, PM0.5-1, PM1-2.5 and PM2.5-10) and analysed for particle mass (PM), organic and elemental carbon (OC and EC), polycyclic aromatic hydrocarbons (PAH), soluble inorganic ions and elemental composition. Three main groups of compounds were discriminated in the tunnel aerosol: carbonaceous, soil component and vehicle mechanical wear. Measurements indicate that Cu can be a good tracer for wear emissions of road traffic. Cu levels correlate strongly with Fe, Mn, Sn and Cr, showing a highly linear constant ratio in all size ranges, suggesting a unique origin through sizes. Ratios of Cu with other elements can be used to source apportion the trace elements present in urban atmospheres, mainly on what concerns coarse aerosol particles. (C) 2013 Elsevier Ltd. All rights reserved.

Impacts of 20th century aerosol emissions on the South Asian monsoon in the CMIP5 models

Comparison of single-forcing varieties of 20th century historical experiments in a subset of models from the Fifth Coupled Model Intercomparison Project (CMIP5) reveals that South Asian summer monsoon rainfall increases towards the present day in Greenhouse Gas (GHG)-only experiments with respect to pre-industrial levels, while it decreases in anthropogenic aerosol-only experiments. Comparison of these single-forcing experiments with the all-forcings historical experiment suggests aerosol emissions have dominated South Asian monsoon rainfall trends in recent decades, especially during the 1950s to 1970s. The variations in South Asian monsoon rainfall in these experiments follows approximately the time evolution of inter-hemispheric temperature gradient over the same period, suggesting a contribution from the large-scale background state relating to the asymmetric distribution of aerosol emissions about the equator. By examining the 24 available all-forcings historical experiments, we show that models including aerosol indirect effects dominate the negative rainfall trend. Indeed, models including only the direct radiative effect of aerosol show an increase in monsoon rainfall, consistent with the dominance of increasing greenhouse gas emissions and planetary warming on monsoon rainfall in those models. For South Asia, reduced rainfall in the models with indirect effects is related to decreased evaporation at the land surface rather than from anomalies in horizontal moisture flux, suggesting the impact of indirect effects on local aerosol emissions. This is confirmed by examination of aerosol loading and cloud droplet number trends over the South Asia region. Thus, while remote aerosols and their asymmetric distribution about the equator play a role in setting the inter-hemispheric temperature distribution on which the South Asian monsoon, as one of the global monsoons, operates, the addition of indirect aerosol effects acting on very local aerosol emissions also plays a role in declining monsoon rainfall. The disparity between the response of monsoon rainfall to increasing aerosol emissions in models containing direct aerosol effects only and those also containing indirect effects needs to be urgently investigated since the suggested future decline in Asian anthropogenic aerosol emissions inherent to the representative concentration pathways (RCPs) used for future climate projection may turn out to be optimistic. In addition, both groups of models show declining rainfall over China, also relating to local aerosol mechanisms. We hypothesize that aerosol emissions over China are large enough, in the CMIP5 models, to cause declining monsoon rainfall even in the absence of indirect aerosol effects. The same is not true for India.

Anthropogenic aerosol emissions and rainfall decline in South-West Australia - accompanying model results in NetCDF format

It is commonly understood that the observed decline in precipitation in South-West Australia during the 20th century is caused by anthropogenic factors. Candidates therefore are changes to large-scale atmospheric circulations due to global warming, extensive deforestation and anthropogenic aerosol emissions - all of which are effective on different spatial and temporal scales. This contribution focusses on the role of rapidly rising aerosol emissions from anthropogenic sources in South-West Australia around 1970. An analysis of historical longterm rainfall data of the Bureau of Meteorology shows that South-West Australia as a whole experienced a gradual decline in precipitation over the 20th century. However, on smaller scales and for the particular example of the Perth catchment area, a sudden drop in precipitation around 1970 is apparent. Modelling experiments at a convection-resolving resolution of 3.3km using the Weather and Research Forecasting (WRF) model version 3.6.1 with the aerosol-aware Thompson-Eidhammer microphysics scheme are conducted for the period 1970-1974. A comparison of four runs with different prescribed aerosol emissions and without aerosol effects demonstrates that tripling the pre-1960s atmospheric CCN and IN concentrations can suppress precipitation by 2-9%, depending on the area and the season. This suggests that a combination of all three processes is required to account for the gradual decline in rainfall seen for greater South-West Australia and for the sudden drop observed in areas along the West Coast in the 1970s: changing atmospheric circulations, deforestation and anthropogenic aerosol emissions.

Aerosol contribution to the rapid warming of near-term climate under RCP 2.6

The importance of aerosol emissions for near term climate projections is investigated by analysing simulations with the HadGEM2-ES model under two different emissions scenarios: RCP2.6 and RCP4.5. It is shown that the near term warming projected under RCP2.6 is greater than under RCP4.5, even though the greenhouse gas forcing is lower. Rapid and substantial reductions in sulphate aerosol emissions due to a reduction of coal burning in RCP2.6 lead to a reduction in the negative shortwave forcing due to aerosol direct and indirect effects. Indirect effects play an important role over the northern hemisphere oceans, especially the subtropical northeastern Pacific where an anomaly of 5-10\,Wm$^{-2}$ develops. The pattern of surface temperature change is consistent with the expected response to this surface radiation anomaly, whilst also exhibiting features that reflect redistribution of energy, and feedbacks, within the climate system. These results demonstrate the importance of aerosol emissions as a key source of uncertainty in near term projections of global and regional climate.

Aerosol forcing in the Climate Model Intercomparison Project (CMIP5) simulations by HadGEM2-ES and the role of ammonium nitrate

The latest Hadley Centre climate model, HadGEM2-ES, includes Earth system components such as interactive chemistry and eight species of tropospheric aerosols. It has been run for the period 1860–2100 in support of the fifth phase of the Climate Model Intercomparison Project (CMIP5). Anthropogenic aerosol emissions peak between 1980 and 2020, resulting in a present-day all-sky top of the atmosphere aerosol forcing of −1.6 and −1.4 W m−2 with and without ammonium nitrate aerosols, respectively, for the sum of direct and first indirect aerosol forcings. Aerosol forcing becomes significantly weaker in the 21st century, being weaker than −0.5 W m−2 in 2100 without nitrate. However, nitrate aerosols become the dominant species in Europe and Asia and decelerate the decrease in global mean aerosol forcing. Considering nitrate aerosols makes aerosol radiative forcing 2–4 times stronger by 2100 depending on the representative concentration pathway, although this impact is lessened when changes in the oxidation properties of the atmosphere are accounted for. Anthropogenic aerosol residence times increase in the future in spite of increased precipitation, as cloud cover and aerosol-cloud interactions decrease in tropical and midlatitude regions. Deposition of fossil fuel black carbon onto snow and ice surfaces peaks during the 20th century in the Arctic and Europe but keeps increasing in the Himalayas until the middle of the 21st century. Results presented here confirm the importance of aerosols in influencing the Earth's climate, albeit with a reduced impact in the future, and suggest that nitrate aerosols will partially replace sulphate aerosols to become an important anthropogenic species in the remainder of the 21st century.

Global estimate of aerosol direct radiative forcing from satellite measurements

Atmospheric aerosols cause scattering and absorption of incoming solar radiation. Additional anthropogenic aerosols released into the atmosphere thus exert a direct radiative forcing on the climate system1. The degree of present-day aerosol forcing is estimated from global models that incorporate a representation of the aerosol cycles1–3. Although the models are compared and validated against observations, these estimates remain uncertain. Previous satellite measurements of the direct effect of aerosols contained limited information about aerosol type, and were confined to oceans only4,5. Here we use state-of-the-art satellitebased measurements of aerosols6–8 and surface wind speed9 to estimate the clear-sky direct radiative forcing for 2002, incorporating measurements over land and ocean. We use a Monte Carlo approach to account for uncertainties in aerosol measurements and in the algorithm used. Probability density functions obtained for the direct radiative forcing at the top of the atmosphere give a clear-sky, global, annual average of 21.9Wm22 with standard deviation, 60.3Wm22. These results suggest that present-day direct radiative forcing is stronger than present model estimates, implying future atmospheric warming greater than is presently predicted, as aerosol emissions continue to decline10.

General circulation model estimates of aerosol transport and radiative forcing during the Indian Ocean Experiment

Aerosol sources, transport, and sinks are simulated, and aerosol direct radiative effects are assessed over the Indian Ocean for the Indian Ocean Experiment (INDOEX) Intensive Field Phase during January to March 1999 using the Laboratoire de Me´te´orologie Dynamique (LMDZT) general circulation model. The model reproduces the latitudinal gradient in aerosol mass concentration and optical depth (AOD). The model-predicted aerosol concentrations and AODs agree reasonably well with measurements but are systematically underestimated during high-pollution episodes, especially in the month of March. The largest aerosol loads are found over southwestern China, the Bay of Bengal, and the Indian subcontinent. Aerosol emissions from the Indian subcontinent are transported into the Indian Ocean through either the west coast or the east coast of India. Over the INDOEX region, carbonaceous aerosols are the largest contributor to the estimated AOD, followed by sulfate, dust, sea salt, and fly ash. During the northeast winter monsoon, natural and anthropogenic aerosols reduce the solar flux reaching the surface by 25 W m�2, leading to 10–15% less insolation at the surface. A doubling of black carbon (BC) emissions from Asia results in an aerosol single-scattering albedo that is much smaller than in situ measurements, reflecting the fact that BC emissions are not underestimated in proportion to other (mostly scattering) aerosol types. South Asia is the dominant contributor to sulfate aerosols over the INDOEX region and accounts for 60–70% of the AOD by sulfate. It is also an important but not the dominant contributor to carbonaceous aerosols over the INDOEX region with a contribution of less than 40% to the AOD by this aerosol species. The presence of elevated plumes brings significant quantities of aerosols to the Indian Ocean that are generated over Africa and Southeast and east Asia.

The impacts of European and Asian anthropogenic sulphur dioxide emissions on Sahel rainfall

In this study, the atmospheric component of a state-of-the-art climate model (HadGEM2-ES) has been used to investigate the impacts of regional anthropogenic sulphur dioxide emissions on boreal summer Sahel rainfall. The study focuses on the transient response of the West African monsoon (WAM) to a sudden change in regional anthropogenic sulphur dioxide emissions, including land surface feedbacks, but without sea surface temperature (SST) feedbacks. The response occurs in two distinct phases: 1) fast adjustment of the atmosphere on a time scale of days to weeks (up to 3 weeks) through aerosol-radiation and aerosol-cloud interactions with weak hydrological cycle changes and surface feedbacks. 2) adjustment of the atmosphere and land surface with significant local hydrological cycle changes and changes in atmospheric circulation (beyond 3 weeks). European emissions lead to an increase in shortwave (SW) scattering by increased sulphate burden, leading to a decrease in surface downward SW radiation which causes surface cooling over North Africa, a weakening of the Saharan heat low and WAM, and a decrease in Sahel precipitation. In contrast, Asian emissions lead to very little change in sulphate burden over North Africa, but they induce an adjustment of the Walker Circulation which leads again to a weakening of the WAM and a decrease in Sahel precipitation. The responses to European and Asian emissions during the second phase exhibit similar large scale patterns of anomalous atmospheric circulation and hydrological variables, suggesting a preferred response. The results support the idea that sulphate aerosol emissions contributed to the observed decline in Sahel precipitation in the second half of the twentieth century.

Investigation of Aerosol Properties Using Environmental Atomic Force Microscopy

Atmospheric aerosols affect both global and regional climate by altering the radiative balance of the atmosphere and acting as cloud condensation nuclei. Despite an increased focus on the research of atmospheric aerosols due to concerns about global climate change, current methods to observe the morphology of aerosols and to measure their hygroscopic properties are limited in various ways by experimental procedure. The primary objectives of this thesis were to use atomic force microscopy to determine the morphology of atmospherically relevant aerosols and to investigate theutility of environmental atomic force microscopy for imaging aerosols as they respond to changes in relative humidity. Traditional aerosol generation and collection techniques were used in conjunction with atomic force microscopy to image commonorganic and inorganic aerosols. In addition, environmental AFM was used to image aerosols at a variety of relative humidity values. The results of this research demonstrated the utility of atomic force microscopy for measuring the morphology of aerosols. In addition, the utility of environmental AFM for measuring the hygroscopic properties of aerosols was demonstrated. Further research in this area will lead to an increased understanding of the role oforganic and inorganic aerosols in the atmosphere, allowing for the effects of anthropogenic aerosol emissions to be quantified and for more accurate climate models to be developed.

Dissolved organic carbon in rainwater from areas heavily impacted by sugar cane burning

This work reports on rainwater dissolved organic carbon (DOC) from Ribeirao Preto (RP) and Araraquara over a period of 3 years. The economies of these two cities, located in Sao Paulo state (Brazil), are based on agriculture and related industries, and the region is strongly impacted by the burning of sugar cane foliage before harvesting. Highest DOC concentrations were obtained when air masses traversed sugar cane fields burned on the same day as the rain event. Significant increases in the DOC volume weighted means (VWM) during the harvest period, for both sites, and a good linear correlation (r=0.83) between DOC and K (a biomass burning marker) suggest that regional scale organic carbon emissions prevail over long-range transport. The DOC VWMs and standard deviations were 272 +/- 22 mu mol L-1 (n=193) and 338 +/- 40 mu mol L-1 (n=80) for RP and Araraquara, respectively, values which are at least two times higher than those reported for other regions influenced by biomass burning, such as the Amazon. These high DOC levels are discussed in terms of agricultural activities, particularly the large usage of biogenic fuels in Brazil, as well as the analytical method used in this work, which includes volatile organic carbon when reporting DOC values. Taking into account rainfall volume, estimated annual rainwater DOC fluxes for RP (4.8 g C m(-2) yr(-1)) and Araraquara (5.4 g C m(-2) yr(-1)) were close to that previously found for the Amazon region (4.8 g C m(-2) yr(-1)). This work also discusses whether previous calculations of the global rainwater carbon flux may have been underestimated, since they did not consider large inputs from biomass combustion sources, and suffered from a possible analytical bias. (c) 2008 Elsevier Ltd. All rights reserved.

Modelling monsoons: understanding and predicting current and future behaviour

The global monsoon system is so varied and complex that understanding and predicting its diverse behaviour remains a challenge that will occupy modellers for many years to come. Despite the difficult task ahead, an improved monsoon modelling capability has been realized through the inclusion of more detailed physics of the climate system and higher resolution in our numerical models. Perhaps the most crucial improvement to date has been the development of coupled ocean-atmosphere models. From subseasonal to interdecadal time scales, only through the inclusion of air-sea interaction can the proper phasing and teleconnections of convection be attained with respect to sea surface temperature variations. Even then, the response to slow variations in remote forcings (e.g., El Niño—Southern Oscillation) does not result in a robust solution, as there are a host of competing modes of variability that must be represented, including those that appear to be chaotic. Understanding the links between monsoons and land surface processes is not as mature as that explored regarding air-sea interactions. A land surface forcing signal appears to dominate the onset of wet season rainfall over the North American monsoon region, though the relative role of ocean versus land forcing remains a topic of investigation in all the monsoon systems. Also, improved forecasts have been made during periods in which additional sounding observations are available for data assimilation. Thus, there is untapped predictability that can only be attained through the development of a more comprehensive observing system for all monsoon regions. Additionally, improved parameterizations - for example, of convection, cloud, radiation, and boundary layer schemes as well as land surface processes - are essential to realize the full potential of monsoon predictability. A more comprehensive assessment is needed of the impact of black carbon aerosols, which may modulate that of other anthropogenic greenhouse gases. Dynamical considerations require ever increased horizontal resolution (probably to 0.5 degree or higher) in order to resolve many monsoon features including, but not limited to, the Mei-Yu/Baiu sudden onset and withdrawal, low-level jet orientation and variability, and orographic forced rainfall. Under anthropogenic climate change many competing factors complicate making robust projections of monsoon changes. Absent aerosol effects, increased land-sea temperature contrast suggests strengthened monsoon circulation due to climate change. However, increased aerosol emissions will reflect more solar radiation back to space, which may temper or even reduce the strength of monsoon circulations compared to the present day. Precipitation may behave independently from the circulation under warming conditions in which an increased atmospheric moisture loading, based purely on thermodynamic considerations, could result in increased monsoon rainfall under climate change. The challenge to improve model parameterizations and include more complex processes and feedbacks pushes computing resources to their limit, thus requiring continuous upgrades of computational infrastructure to ensure progress in understanding and predicting current and future behaviour of monsoons.

Revisiting the Earth's sea-level and energy budgets from 1961 to 2008

We review the sea-level and energy budgets together from 1961, using recent and updated estimates of all terms. From 1972 to 2008, the observed sea-level rise (1.8 ± 0.2 mm yr−1 from tide gauges alone and 2.1 ± 0.2 mm yr−1 from a combination of tide gauges and altimeter observations) agrees well with the sum of contributions (1.8 ± 0.4 mm yr−1) in magnitude and with both having similar increases in the rate of rise during the period. The largest contributions come from ocean thermal expansion (0.8 mm yr−1) and the melting of glaciers and ice caps (0.7 mm yr−1), with Greenland and Antarctica contributing about 0.4 mm yr−1. The cryospheric contributions increase through the period (particularly in the 1990s) but the thermosteric contribution increases less rapidly. We include an improved estimate of aquifer depletion (0.3 mm yr−1), partially offsetting the retention of water in dams and giving a total terrestrial storage contribution of −0.1 mm yr−1. Ocean warming (90% of the total of the Earth's energy increase) continues through to the end of the record, in agreement with continued greenhouse gas forcing. The aerosol forcing, inferred as a residual in the atmospheric energy balance, is estimated as −0.8 ± 0.4 W m−2 for the 1980s and early 1990s. It increases in the late 1990s, as is required for consistency with little surface warming over the last decade. This increase is likely at least partially related to substantial increases in aerosol emissions from developing nations and moderate volcanic activity

Aerosols implicated as a prime driver of twentieth-century North Atlantic climate variability

Systematic climate shifts have been linked to multidecadal variability in observed sea surface temperatures in the North Atlantic Ocean1. These links are extensive, influencing a range of climate processes such as hurricane activity2 and African Sahel3, 4, 5 and Amazonian5 droughts. The variability is distinct from historical global-mean temperature changes and is commonly attributed to natural ocean oscillations6, 7, 8, 9, 10. A number of studies have provided evidence that aerosols can influence long-term changes in sea surface temperatures11, 12, but climate models have so far failed to reproduce these interactions6, 9 and the role of aerosols in decadal variability remains unclear. Here we use a state-of-the-art Earth system climate model to show that aerosol emissions and periods of volcanic activity explain 76 per cent of the simulated multidecadal variance in detrended 1860–2005 North Atlantic sea surface temperatures. After 1950, simulated variability is within observational estimates; our estimates for 1910–1940 capture twice the warming of previous generation models but do not explain the entire observed trend. Other processes, such as ocean circulation, may also have contributed to variability in the early twentieth century. Mechanistically, we find that inclusion of aerosol–cloud microphysical effects, which were included in few previous multimodel ensembles, dominates the magnitude (80 per cent) and the spatial pattern of the total surface aerosol forcing in the North Atlantic. Our findings suggest that anthropogenic aerosol emissions influenced a range of societally important historical climate events such as peaks in hurricane activity and Sahel drought. Decadal-scale model predictions of regional Atlantic climate will probably be improved by incorporating aerosol–cloud microphysical interactions and estimates of future concentrations of aerosols, emissions of which are directly addressable by policy actions.

The effect of regional changes in anthropogenic aerosols on rainfall of the East Asian summer monsoon

The response of East Asian Summer Monsoon (EASM) precipitation to long term changes in regional anthropogenic aerosols (sulphate and black carbon) is explored in an atmospheric general circulation model, the atmospheric component of the UK High-Resolution Global Environment Model v1.2 (HiGAM). Separately, sulphur dioxide (SO2) and black carbon (BC) emissions in 1950 and 2000 over East Asia are used to drive model simulations, while emissions are kept constant at year 2000 level outside this region. The response of the EASM is examined by comparing simulations driven by aerosol emissions representative of 1950 and 2000. The aerosol radiative effects are also determined using an off-line radiative transfer model. During June, July and August, the EASM was not significantly changed as either SO2 or BC emissions increased from 1950 to 2000 levels. However, in September, precipitation is significantly decreased by 26.4% for sulphate aerosol and 14.6% for black carbon when emissions are at the 2000 level. Over 80% of the decrease is attributed to changes in convective precipitation. The cooler land surface temperature over China in September (0.8 °C for sulphate and 0.5 °C for black carbon) due to increased aerosols reduces the surface thermal contrast that supports the EASM circulation. However, mechanisms causing the surface temperature decrease in September are different between sulphate and BC experiments. In the sulphate experiment, the sulphate direct and the 1st indirect radiative effects contribute to the surface cooling. In the BC experiment, the BC direct effect is the main driver of the surface cooling, however, a decrease in low cloud cover due to the increased heating by BC absorption partially counteracts the direct effect. This results in a weaker land surface temperature response to BC changes than to sulphate changes. The resulting precipitation response is also weaker, and the responses of the monsoon circulation are different for sulphate and black carbon experiments. This study demonstrates a mechanism that links regional aerosol emission changes to the precipitation changes of the EASM, and it could be applied to help understand the future changes in EASM precipitation in CMIP5 simulations.

Airborne measurements of trace gases and aerosols over the London metropolitan region

The Emissions around the M25 motorway (EM25) campaign took place over the megacity of London in the United Kingdom in June 2009 with the aim of characterising trace gas and aerosol composition and properties entering and emitted from the urban region. It featured two mobile platforms, the UK BAe-146 Facility for Airborne Atmospheric Measurements (FAAM) research aircraft and a ground-based mobile lidar van, both travelling in circuits around London, roughly following the path of the M25 motorway circling the city. We present an overview of findings from the project, which took place during typical UK summertime pollution conditions. Emission ratios of volatile organic compounds (VOCs) to acetylene and carbon monoxide emitted from the London region were consistent with measurements in and downwind of other large urban areas and indicated traffic and associated fuel evaporation were major sources. Sub-micron aerosol composition was dominated by secondary species including sulphate (24% of sub-micron mass in the London plume and 29% in the non-plume regional aerosol), nitrate (24% plume; 20% regional) and organic aerosol (29% plume; 31% regional). The primary sub-micron aerosol emissions from London were minor compared to the larger regional background, with only limited increases in aerosol mass in the urban plume compared to the background (~12% mass increase on average). Black carbon mass was the major exception and more than doubled in the urban plume, leading to a decrease in the single scattering albedo from 0.91 in the regional aerosol to 0.86 in the London plume, on average. Our observations indicated that regional aerosol plays a major role on aerosol concentrations around London, at least during typical summertime conditions, meaning future efforts to reduce PM levels in London must account for regional as well as local aerosol sources.