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- ItemDesign and performance of a three-wavelength LED-based total scatter and backscatter integrating nephelometer(München : European Geopyhsical Union, 2011) Müller, T.; Laborde, M.; Kassell, G.; Wiedensohler, A.Integrating nephelometers are instruments that directly measure a value close to the light scattering coefficient of airborne particles. Different models of nephelometers have been used for decades for monitoring and research applications. Now, a series of nephelometers (Ecotech models M9003, Aurora 1000 and Aurora 3000) with newly designed light sources based on light emitting diodes are available. This article reports on the design of these integrating nephelometers and a comparison of the Aurora 3000 to another commercial instrument (TSI model 3563) that uses an incandescent lamp. Both instruments are three-wavelength, total and backscatter integrating nephelometers. We present a characterization of the new light source design of the Aurora 3000 and provide parameterizations for its angular sensitivity functions. These parameterizations facilitate to correct for measurement artefacts using Mie-theory. Furthermore, correction factors are provided as a function of the Ångström exponent. Comparison measurements against the TSI 3563 with laboratory generated white particles and ambient air are also shown and discussed. Both instruments agree well within the calibration uncertainties and detection limit for total scattering with differences less than 5 %. Differences for backscattering are higher by up to 11 %. Highest differences were found for the longest wavelengths, where the signal to noise ratio is lowest. Differences at the blue and green wavelengths are less than 4 % and 3 %, respectively, for both total and backscattering.
- 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.
- ItemAtmospheric dust modeling from meso to global scales with the online NMMB/BSC-Dust model – Part 2: Experimental campaigns in Northern Africa(München : European Geopyhsical Union, 2012) Haustein, K.; Pérez, C.; Baldasano, J.M.; Jorba, O.; Basart, S.; Miller, R.L.; Janjic, Z.; Black, T.; Nickovic, S.; Todd, M.C.; Washington, R.; Müller, D.; Tesche, M.; Weinzierl, B.; Esselborn, M.; Schladitz, A.The new NMMB/BSC-Dust model is intended to provide short to medium-range weather and dust forecasts from regional to global scales. It is an online model in which the dust aerosol dynamics and physics are solved at each model time step. The companion paper (Pérez et al., 2011) develops the dust model parameterizations and provides daily to annual evaluations of the model for its global and regional configurations. Modeled aerosol optical depth (AOD) was evaluated against AERONET Sun photometers over Northern Africa, Middle East and Europe with correlations around 0.6–0.7 on average without dust data assimilation. In this paper we analyze in detail the behavior of the model using data from the Saharan Mineral dUst experiment (SAMUM-1) in 2006 and the Bodélé Dust Experiment (BoDEx) in 2005. AOD from satellites and Sun photometers, vertically resolved extinction coefficients from lidars and particle size distributions at the ground and in the troposphere are used, complemented by wind profile data and surface meteorological measurements. All simulations were performed at the regional scale for the Northern African domain at the expected operational horizontal resolution of 25 km. Model results for SAMUM-1 generally show good agreement with satellite data over the most active Saharan dust sources. The model reproduces the AOD from Sun photometers close to sources and after long-range transport, and the dust size spectra at different height levels. At this resolution, the model is not able to reproduce a large haboob that occurred during the campaign. Some deficiencies are found concerning the vertical dust distribution related to the representation of the mixing height in the atmospheric part of the model. For the BoDEx episode, we found the diurnal temperature cycle to be strongly dependant on the soil moisture, which is underestimated in the NCEP analysis used for model initialization. The low level jet (LLJ) and the dust AOD over the Bodélé are well reproduced. The remaining negative AOD bias (due to underestimated surface wind speeds) can be substantially reduced by decreasing the threshold friction velocity in the model.
- ItemHygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain(München : European Geopyhsical Union, 2011) Liu, P.F.; Zhao, C.S.; Göbel, T.; Hallbauer, E.; Nowak, A.; Ran, L.; Xu, W.Y.; Deng, Z.Z.; Ma, N.; Mildenberger, K.; Henning, S.; Stratmann, F.; Wiedensohler, A.The hygroscopic properties of submicron aerosol particles were determined at a suburban site (Wuqing) in the North China Plain among a cluster of cities during the period 17 July to 12 August, 2009. A High Humidity Tandem Differential Mobility Analyser (HH-TDMA) instrument was applied to measure the hygroscopic growth factor (GF) at 90%, 95% and 98.5% relative humidity (RH) for particles with dry diameters between 50 and 250 nm. The probability distribution of GF (GF-PDF) averaged over the period shows a distinct bimodal pattern, namely, a dominant more-hygroscopic (MH) group and a smaller nearly-hydrophobic (NH) group. The MH group particles were highly hygroscopic, and their GF was relatively constant during the period with average values of 1.54 ± 0.02, 1.81 ± 0.04 and 2.45 ± 0.07 at 90%, 95% and 98.5% RH (D0 = 100 nm), respectively. The NH group particles grew very slightly when exposed to high RH, with GF values of 1.08 ± 0.02, 1.13 ± 0.06 and 1.24 ± 0.13 respectively at 90%, 95% and 98.5% RH (D0 = 100 nm). The hygroscopic growth behaviours at different RHs were well represented by a single-parameter Köhler model. Thus, the calculation of GF as a function of RH and dry diameter could be facilitated by an empirical parameterization of κ as function of dry diameter. A strong diurnal pattern in number fraction of different hygroscopic groups was observed. The average number fraction of NH particles during the day was about 8%, while during the nighttime fractions up to 20% were reached. Correspondingly, the state of mixing in terms of water uptake varied significantly during a day. Simulations using a particle-resolved aerosol box model (PartMC-MOSAIC) suggest that the diurnal variations of aerosol hygroscopicity and mixing state were mainly caused by the evolution of the atmospheric mixing layer. The shallow nocturnal boundary layer during the night facilitated the accumulation of freshly emitted carbonaceous particles (mainly hydrophobic) near the surface while in the morning turbulence entrained the more aged and more hygroscopic particles from aloft and diluted the NH particles near the surface resulting in a decrease in the fraction of NH particles.
- ItemSize-resolved measurement of the mixing state of soot in the megacity Beijing, China: Diurnal cycle, aging and parameterization(München : European Geopyhsical Union, 2012) Cheng, Y.F.; Su, H.; Rose, D.; Gunthe, S.S.; Berghof, M.; Wehner, B.; Achtert, P.; Nowak, A.; Takegawa, N.; Kondo, Y.; Shiraiwa, M.; Gong, Y.G.; Shao, M.; Hu, M.; Zhu, T.; Zhang, Y.H.; Carmichael, G.R.; Wiedensohler, A.; Andreae, M.O.; Pöschl, U.Soot particles are the most efficient light absorbing aerosol species in the atmosphere, playing an important role as a driver of global warming. Their climate effects strongly depend on their mixing state, which significantly changes their light absorbing capability and cloud condensation nuclei (CCN) activity. Therefore, knowledge about the mixing state of soot and its aging mechanism becomes an important topic in the atmospheric sciences. The size-resolved (30–320 nm diameter) mixing state of soot particles in polluted megacity air was measured at a suburban site (Yufa) during the CAREBeijing 2006 campaign in Beijing, using a volatility tandem differential mobility analyzer (VTDMA). Particles in this size range with non-volatile residuals at 300 °C were considered to be soot particles. On average, the number fraction of internally mixed soot in total soot particles (Fin), decreased from 0.80 to 0.57 when initial Dp increased from 30 to 320 nm. Further analysis reveals that: (1) Fin was well correlated with the aerosol hygroscopic mixing state measured by a CCN counter. More externally mixed soot particles were observed when particles showed more heterogeneous features with regard to hygroscopicity. (2) Fin had pronounced diurnal cycles. For particles in the accumulation mode (Dp at 100–320 nm), largest Fin were observed at noon time, with "apparent" turnover rates (kex → in) up to 7.8% h−1. (3) Fin was subject to competing effects of both aging and emissions. While aging increases Fin by converting externally mixed soot particles into internally mixed ones, emissions tend to reduce Fin by emitting more fresh and externally mixed soot particles. Similar competing effects were also found with air mass age indicators. (4) Under the estimated emission intensities, actual turnover rates of soot (kex → in) up to 20% h−1 were derived, which showed a pronounced diurnal cycle peaking around noon time. This result confirms that (soot) particles are undergoing fast aging/coating with the existing high levels of condensable vapors in the megacity Beijing. (5) Diurnal cycles of Fin were different between Aitken and accumulation mode particles, which could be explained by the faster growth of smaller Aitken mode particles into larger size bins. To improve the Fin prediction in regional/global models, we suggest parameterizing Fin by an air mass aging indicator, i.e., Fin = a + bx, where a and b are empirical coefficients determined from observations, and x is the value of an air mass age indicator. At the Yufa site in the North China Plain, fitted coefficients (a, b) were determined as (0.57, 0.21), (0.47, 0.21), and (0.52, 0.0088) for x (indicators) as [NOz]/[NOy], [E]/[X] ([ethylbenzene]/[m,p-xylene]) and ([IM] + [OM])/[EC] ([inorganic + organic matter]/[elemental carbon]), respectively. Such a parameterization consumes little additional computing time, but yields a more realistic description of Fin compared with the simple treatment of soot mixing state in regional/global models.
- ItemA parameterization of low visibilities for hazy days in the North China Plain(München : European Geopyhsical Union, 2012) Chen, J.; Zhao, C.S.; Ma, N.; Liu, P.F.; Göbel, T.; Hallbauer, E.; Deng, Z.Z.; Ran, L.; Xu, W.Y.; Liang, Z.; Liu, H.J.; Yan, P.; Zhou, X.J.; Wiedensohler, A.Visibility degradation is a pervasive and urgent environmental problem in China. The occurrence of low visibility events is frequent in the North China Plain, where the aerosol loading is quite high and aerosols are strongly hygroscopic. A parameterization of light extinction (Kex) for low visibilities on hazy days is proposed in this paper, based on visibility, relative humidity (RH), aerosol hygroscopic growth factors and particle number size distributions measured during the Haze in China (HaChi) Project. Observational results show that a high aerosol volume concentration is responsible for low visibility at RH <90%; while for RH >90%, decrease of visibility is mainly influenced by the increase of RH. The parameterization of Kex is developed on the basis of aerosol volume concentrations and RH, taking into accounts the sensitivity of visibility to the two factors and the availability of corresponding data. The extinction coefficients calculated with the parameterization schemes agree well with the directly measured values.
- ItemEmulating coupled atmosphere-ocean and carbon cycle models with a simpler model, MAGICC6 - Part 1: Model description and calibration(München : European Geopyhsical Union, 2011) Meinshausen, M.; Raper, S.C.B.; Wigley, T.M.L.Current scientific knowledge on the future response of the climate system to human-induced perturbations is comprehensively captured by various model intercomparison efforts. In the preparation of the Fourth Assessment Report (AR4) of the Intergovernmental Panel on Climate Change (IPCC), intercomparisons were organized for atmosphere-ocean general circulation models (AOGCMs) and carbon cycle models, named "CMIP3" and "C4MIP", respectively. Despite their tremendous value for the scientific community and policy makers alike, there are some difficulties in interpreting the results. For example, radiative forcings were not standardized across the various AOGCM integrations and carbon cycle runs, and, in some models, key forcings were omitted. Furthermore, the AOGCM analysis of plausible emissions pathways was restricted to only three SRES scenarios. This study attempts to address these issues. We present an updated version of MAGICC, the simple carbon cycle-climate model used in past IPCC Assessment Reports with enhanced representation of time-varying climate sensitivities, carbon cycle feedbacks, aerosol forcings and ocean heat uptake characteristics. This new version, MAGICC6, is successfully calibrated against the higher complexity AOGCMs and carbon cycle models. Parameterizations of MAGICC6 are provided. The mean of the emulations presented here using MAGICC6 deviates from the mean AOGCM responses by only 2.2% on average for the SRES scenarios. This enhanced emulation skill in comparison to previous calibrations is primarily due to: making a "like-with-like comparison" using AOGCM-specific subsets of forcings; employing a new calibration procedure; as well as the fact that the updated simple climate model can now successfully emulate some of the climate-state dependent effective climate sensitivities of AOGCMs. The diagnosed effective climate sensitivity at the time of CO2 doubling for the AOGCMs is on average 2.88 °C, about 0.33 °C cooler than the mean of the reported slab ocean climate sensitivities. In the companion paper (Part 2) of this study, we examine the combined climate system and carbon cycle emulations for the complete range of IPCC SRES emissions scenarios and the new RCP pathways.
- ItemWater uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics(München : European Geopyhsical Union, 2011) Dusek, U.; Frank, G.P.; Massling, A.; Zeromskiene, K.; Iinuma, Y.; Schmid, O.; Helas, G.; Hennig, T.; Wiedensohler, A.; Andreae, M.O.We investigate the CCN activity of freshly emitted biomass burning particles and their hygroscopic growth at a relative humidity (RH) of 85%. The particles were produced in the Mainz combustion laboratory by controlled burning of various wood types. The water uptake at sub- and supersaturations is parameterized by the hygroscopicity parameter, κ (c.f. Petters and Kreidenweis, 2007). For the wood burns, κ is low, generally around 0.06. The main emphasis of this study is a comparison of κ derived from measurements at sub- and supersaturated conditions (κG and κCCN), in order to see whether the water uptake at 85% RH can predict the CCN properties of the biomass burning particles. Differences in κGand κCCN can arise through solution non-idealities, the presence of slightly soluble or surface active compounds, or non-spherical particle shape. We find that κG and κCCN agree within experimental uncertainties (of around 30%) for particle sizes of 100 and 150 nm; only for 50 nm particles is κCCN larger than κG by a factor of 2. The magnitude of this difference and its dependence on particle size is consistent with the presence of surface active organic compounds. These compounds mainly facilitate the CCN activation of small particles, which form the most concentrated solution droplets at the point of activation. The 50 nm particles, however, are only activated at supersaturations higher than 1% and are therefore of minor importance as CCN in ambient clouds. By comparison with the actual chemical composition of the biomass burning particles, we estimate that the hygroscopicity of the water-soluble organic carbon (WSOC) fraction can be represented by a κWSOC value of approximately 0.2. The effective hygroscopicity of a typical wood burning particle can therefore be represented by a linear mixture of an inorganic component with κ ≅ 0.6, a WSOC component with κ ≅ 0.2, and an insoluble component with κ = 0.
- ItemA new climate dataset for systematic assessments of climate change impacts as a function of global warming(München : European Geopyhsical Union, 2012) Heinke, J.; Ostberg, S.; Schaphoff, S.; Frieler, K.; Müller, C.; Gerten, D.; Meinshausen, M.; Lucht, W.Interactions between food demand, biomass energy and forest preservation are driving both food prices and land-use changes, regionally and globally. This study presents a new model called Nexus Land-Use version 1.0 which describes these interactions through a generic representation of agricultural intensification mechanisms within agricultural lands. The Nexus Land-Use model equations combine biophysics and economics into a single coherent framework to calculate crop yields, food prices, and resulting pasture and cropland areas within 12 regions inter-connected with each other by international trade. The representation of cropland and livestock production systems in each region relies on three components: (i) a biomass production function derived from the crop yield response function to inputs such as industrial fertilisers; (ii) a detailed representation of the livestock production system subdivided into an intensive and an extensive component, and (iii) a spatially explicit distribution of potential (maximal) crop yields prescribed from the Lund-Postdam-Jena global vegetation model for managed Land (LPJmL). The economic principles governing decisions about land-use and intensification are adapted from the Ricardian rent theory, assuming cost minimisation for farmers. In contrast to the other land-use models linking economy and biophysics, crops are aggregated as a representative product in calories and intensification for the representative crop is a non-linear function of chemical inputs. The model equations and parameter values are first described in details. Then, idealised scenarios exploring the impact of forest preservation policies or rising energy price on agricultural intensification are described, and their impacts on pasture and cropland areas are investigated.
- ItemMeteorological and trace gas factors affecting the number concentration of atmospheric Aitken (DP Combining double low line 50 nm) particles in the continental boundary layer: Parameterization using a multivariate mixed effects model(München : European Geopyhsical Union, 2011) Mikkonen, S.; Korhonen, H.; Romakkaniemi, S.; Smith, J.N.; Joutsensaari, J.; Lehtinen, K.E.J.; Hamed, A.; Breider, T.J.; Birmili, W.; Spindler, G.; Plass-Duelmer, C.; Facchini, M.C.; Laaksonen, A.Measurements of aerosol size distribution and different gas and meteorological parameters, made in three polluted sites in Central and Southern Europe: Po Valley, Italy, Melpitz and Hohenpeissenberg in Germany, were analysed for this study to examine which of the meteorological and trace gas variables affect the number concentration of Aitken (Dp= 50 nm) particles. The aim of our study was to predict the number concentration of 50 nm particles by a combination of in-situ meteorological and gas phase parameters. The statistical model needs to describe, amongst others, the factors affecting the growth of newly formed aerosol particles (below 10 nm) to 50 nm size, but also sources of direct particle emissions in that size range. As the analysis method we used multivariate nonlinear mixed effects model. Hourly averages of gas and meteorological parameters measured at the stations were used as predictor variables; the best predictive model was attained with a combination of relative humidity, new particle formation event probability, temperature, condensation sink and concentrations of SO2, NO2 and ozone. The seasonal variation was also taken into account in the mixed model structure. Model simulations with the Global Model of Aerosol Processes (GLOMAP) indicate that the parameterization can be used as a part of a larger atmospheric model to predict the concentration of climatically active particles. As an additional benefit, the introduced model framework is, in theory, applicable for any kind of measured aerosol parameter.