5 results
Search Results
Now showing 1 - 5 of 5
- ItemPrimary versus secondary contributions to particle number concentrations in the European boundary layer(München : European Geopyhsical Union, 2011) Reddington, C.L.; Carslaw, K.S.; Spracklen, D.V.; Frontoso, M.G.; Collins, L.; Merikanto, J.; Minikin, A.; Hamburger, T.; Coe, H.; Kulmala, M.; Aalto, P.; Flentje, H.; Plass-Dülmer, C.; Birmili, W.; Wiedensohler, A.; Wehner, B.; Tuch, T.; Sonntag, A.; O'Dowd, C.D.; Jennings, S.G.; Dupuy, R.; Baltensperger, U.; Weingartner, E.; Hansson, H.-C.; Tunved, P.; Laj, P.; Sellegri, K.; Boulon, J.; Putaud, J.-P.; Gruening, C.; Swietlicki, E.; Roldin, P.; Henzing, J.S.; Moerman, M.; Mihalopoulos, N.; Kouvarakis, G.; Ždímal, V.; Zíková, N.; Marinoni, A.; Bonasoni, P.; Duchi, R.It is important to understand the relative contribution of primary and secondary particles to regional and global aerosol so that models can attribute aerosol radiative forcing to different sources. In large-scale models, there is considerable uncertainty associated with treatments of particle formation (nucleation) in the boundary layer (BL) and in the size distribution of emitted primary particles, leading to uncertainties in predicted cloud condensation nuclei (CCN) concentrations. Here we quantify how primary particle emissions and secondary particle formation influence size-resolved particle number concentrations in the BL using a global aerosol microphysics model and aircraft and ground site observations made during the May 2008 campaign of the European Integrated Project on Aerosol Cloud Climate Air Quality Interactions (EUCAARI). We tested four different parameterisations for BL nucleation and two assumptions for the emission size distribution of anthropogenic and wildfire carbonaceous particles. When we emit carbonaceous particles at small sizes (as recommended by the Aerosol Intercomparison project, AEROCOM), the spatial distributions of campaign-mean number concentrations of particles with diameter >50 nm (N50) and >100 nm (N100) were well captured by the model (R2≥0.8) and the normalised mean bias (NMB) was also small (−18% for N50 and −1% for N100). Emission of carbonaceous particles at larger sizes, which we consider to be more realistic for low spatial resolution global models, results in equally good correlation but larger bias (R2≥0.8, NMB = −52% and −29%), which could be partly but not entirely compensated by BL nucleation. Within the uncertainty of the observations and accounting for the uncertainty in the size of emitted primary particles, BL nucleation makes a statistically significant contribution to CCN-sized particles at less than a quarter of the ground sites. Our results show that a major source of uncertainty in CCN-sized particles in polluted European air is the emitted size of primary carbonaceous particles. New information is required not just from direct observations, but also to determine the "effective emission size" and composition of primary particles appropriate for different resolution models.
- ItemExplaining global surface aerosol number concentrations in terms of primary emissions and particle formation(München : European Geopyhsical Union, 2010) Spracklen, D.V.; Carslaw, K.S.; Merikanto, J.; Mann, G.W.; Reddington, C.L.; Pickering, S.; Ogren, J.A.; Andrews, E.; Baltensperger, U.; Weingartner, E.; Boy, M.; Kulmala, M.; Laakso, L.; Lihavainen, H.; Kivekäs, N.; Komppula, M.; Mihalopoulos, N.; Kouvarakis, G.; Jennings, S.G.; O'Dowd, C.; Birmili, W.; Wiedensohler, A.; Weller, R.; Gras, J.; Laj, P.; Sellegri, K.; Bonn, B.; Krejci, R.; Laaksonen, A.; Hamed, A.; Minikin, A.; Harrison, R.M.; Talbot, R.; Sun, J.We synthesised observations of total particle number (CN) concentration from 36 sites around the world. We found that annual mean CN concentrations are typically 300–2000 cm−3 in the marine boundary layer and free troposphere (FT) and 1000–10 000 cm−3 in the continental boundary layer (BL). Many sites exhibit pronounced seasonality with summer time concentrations a factor of 2–10 greater than wintertime concentrations. We used these CN observations to evaluate primary and secondary sources of particle number in a global aerosol microphysics model. We found that emissions of primary particles can reasonably reproduce the spatial pattern of observed CN concentration (R2=0.46) but fail to explain the observed seasonal cycle (R2=0.1). The modeled CN concentration in the FT was biased low (normalised mean bias, NMB=−88%) unless a secondary source of particles was included, for example from binary homogeneous nucleation of sulfuric acid and water (NMB=−25%). Simulated CN concentrations in the continental BL were also biased low (NMB=−74%) unless the number emission of anthropogenic primary particles was increased or a mechanism that results in particle formation in the BL was included. We ran a number of simulations where we included an empirical BL nucleation mechanism either using the activation-type mechanism (nucleation rate, J, proportional to gas-phase sulfuric acid concentration to the power one) or kinetic-type mechanism (J proportional to sulfuric acid to the power two) with a range of nucleation coefficients. We found that the seasonal CN cycle observed at continental BL sites was better simulated by BL particle formation (R2=0.3) than by increasing the number emission from primary anthropogenic sources (R2=0.18). The nucleation constants that resulted in best overall match between model and observed CN concentrations were consistent with values derived in previous studies from detailed case studies at individual sites. In our model, kinetic and activation-type nucleation parameterizations gave similar agreement with observed monthly mean CN concentrations.
- ItemPollution events observed during CARIBIC flights in the upper troposphere between South China and the Philippines(München : European Geopyhsical Union, 2010) Lai, S.C.; Baker, A.K.; Schuck, T.J.; van Velthoven, P.; Oram, D.E.; Zahn, A.; Hermann, M.; Weigelt, A.; Slemr, F.; Brenninkmeijer, C.A.M.; Ziereis, H.A strong pollution episode in the upper troposphere between South China and the Philippines was observed during CARIBIC flights in April 2007. Five pollution events were observed, where enhancements in aerosol and trace gas concentrations including CO, CO2, CH4, non-methane hydrocarbons (NMHCs) and halocarbons were observed along the flight tracks during four sequential flights. The importance of the contribution of biomass/biofuel burning was investigated using chemical tracers, emission factor analysis, back-trajectory analysis and satellite images. The Indochinese peninsula was identified as the probable source region of biomass/biofuel burning. However, enhancements in the urban/industrial tracer C2Cl4 during the events also indicate a substantial contribution from urban anthropogenic emissions. An estimation of the contribution of fossil fuel versus biomass/biofuel to the CO enhancement was made, indicating a biomass/biofuel burning contribution of ~54 to ~92% of the observed CO enhancements. Biomass/biofuel burning was found to be the most important source category during the sampling period.
- ItemOverview of the synoptic and pollution situation over Europe during the EUCAARI-LONGREX field campaign(München : European Geopyhsical Union, 2011) Hamburger, T.; McMeeking, G.; Minikin, A.; Birmili, W.; Dall'Osto, M.; O'Dowd, C.; Flentje, H.; Henzing, B.; Junninen, H.; Kristensson, A.; de Leeuw, G.; Stohl, A.; Burkhart, J.F.; Coe, H.; Krejci, R.; Petzold, A.In May 2008 the EUCAARI-LONGREX aircraft field campaign was conducted within the EUCAARI intensive observational period. The campaign aimed at studying the distribution and evolution of air mass properties on a continental scale. Airborne aerosol and trace gas measurements were performed aboard the German DLR Falcon 20 and the British FAAM BAe-146 aircraft. This paper outlines the meteorological situation over Europe during May 2008 and the temporal and spatial evolution of predominantly anthropogenic particulate pollution inside the boundary layer and the free troposphere. Time series data of six selected ground stations are used to discuss continuous measurements besides the single flights. The observations encompass total and accumulation mode particle number concentration (0.1–0.8 μm) and black carbon mass concentration as well as several meteorological parameters. Vertical profiles of total aerosol number concentration up to 10 km are compared to vertical profiles probed during previous studies. During the first half of May 2008 an anticyclonic blocking event dominated the weather over Central Europe. It led to increased pollutant concentrations within the centre of the high pressure inside the boundary layer. Due to long-range transport the accumulated pollution was partly advected towards Western and Northern Europe. The measured aerosol number concentrations over Central Europe showed in the boundary layer high values up to 14 000 cm−3 for particles in diameter larger 10 nm and 2300 cm−3 for accumulation mode particles during the high pressure period, whereas the middle free troposphere showed rather low concentrations of particulates. Thus a strong negative gradient of aerosol concentrations between the well mixed boundary layer and the clean middle troposphere occurred.
- ItemThe RCP greenhouse gas concentrations and their extensions from 1765 to 2300(Dordrecht [u.a.] : Springer, 2011) Meinshausen, M.; Smith, S.J.; Calvin, K.; Daniel, J.S.; Kainuma, M.L.T.; Lamarque, J.; Matsumoto, K.; Montzka, S.A.; Raper, S.C.B.; Riahi, K.; Thomson, A.; Velders, G.J.M.; van Vuuren, D.P.P.We present the greenhouse gas concentrations for the Representative Concentration Pathways (RCPs) and their extensions beyond 2100, the Extended Concentration Pathways (ECPs). These projections include all major anthropogenic greenhouse gases and are a result of a multi-year effort to produce new scenarios for climate change research. We combine a suite of atmospheric concentration observations and emissions estimates for greenhouse gases (GHGs) through the historical period (1750-2005) with harmonized emissions projected by four different Integrated Assessment Models for 2005-2100. As concentrations are somewhat dependent on the future climate itself (due to climate feedbacks in the carbon and other gas cycles), we emulate median response characteristics of models assessed in the IPCC Fourth Assessment Report using the reduced-complexity carbon cycle climate model MAGICC6. Projected 'best-estimate' global-mean surface temperature increases (using inter alia a climate sensitivity of 3°C) range from 1.5°C by 2100 for the lowest of the four RCPs, called both RCP3-PD and RCP2. 6, to 4.5°C for the highest one, RCP8. 5, relative to pre-industrial levels. Beyond 2100, we present the ECPs that are simple extensions of the RCPs, based on the assumption of either smoothly stabilizing concentrations or constant emissions: For example, the lower RCP2. 6 pathway represents a strong mitigation scenario and is extended by assuming constant emissions after 2100 (including net negative CO2 emissions), leading to CO2 concentrations returning to 360 ppm by 2300. We also present the GHG concentrations for one supplementary extension, which illustrates the stringent emissions implications of attempting to go back to ECP4. 5 concentration levels by 2250 after emissions during the 21st century followed the higher RCP6 scenario. Corresponding radiative forcing values are presented for the RCP and ECPs.