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- 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.
- ItemALADINA - An unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer(München : European Geopyhsical Union, 2015) Altstädter, B.; Platis, A.; Wehner, B.; Scholtz, A.; Wildmann, N.; Hermann, M.; Käthner, R.; Baars, H.; Bange, J.; Lampert, A.This paper presents the unmanned research aircraft Carolo P360 "ALADINA" (Application of Light-weight Aircraft for Detecting IN situ Aerosol) for investigating the horizontal and vertical distribution of ultrafine particles in the atmospheric boundary layer (ABL). It has a wingspan of 3.6 m, a maximum take-off weight of 25 kg and is equipped with aerosol instrumentation and meteorological sensors. A first application of the system, together with the unmanned research aircraft MASC (Multi-Purpose Airborne Carrier) of the Eberhard Karls University of Tübingen (EKUT), is described. As small payload for ALADINA, two condensation particle counters (CPC) and one optical particle counter (OPC) were miniaturised by re-arranging the vital parts and composing them in a space-saving way in the front compartment of the airframe. The CPCs are improved concerning the lower detection threshold and the response time to less than 1.3 s. Each system was characterised in the laboratory and calibrated with test aerosols. The CPCs are operated in this study with two different lower detection threshold diameters of 11 and 18 nm. The amount of ultrafine particles, which is an indicator for new particle formation, is derived from the difference in number concentrations of the two CPCs (ΔN). Turbulence and thermodynamic structure of the boundary layer are described by measurements of fast meteorological sensors that are mounted at the aircraft nose. A first demonstration of ALADINA and a feasibility study were conducted in Melpitz near Leipzig, Germany, at the Global Atmosphere Watch (GAW) station of the Leibniz Institute for Tropospheric Research (TROPOS) on 2 days in October 2013. There, various ground-based instruments are installed for long-term atmospheric monitoring. The ground-based infrastructure provides valuable additional background information to embed the flights in the continuous atmospheric context and is used for validation of the airborne results. The development of the boundary layer, derived from backscatter signals of a portable Raman lidar POLLYXT, allows a quick overview of the current vertical structure of atmospheric particles. Ground-based aerosol number concentrations are consistent with the results from flights in heights of a few metres. In addition, a direct comparison of ALADINA aerosol data and ground-based aerosol data, sampling the air at the same location for more than 1 h, shows comparable values within the range of ± 20 %. MASC was operated simultaneously with complementary flight patterns. It is equipped with the same meteorological instruments that offer the possibility to determine turbulent fluxes. Therefore, additional information about meteorological conditions was collected in the lowest part of the atmosphere. Vertical profiles up to 1000 m in altitude indicate a high variability with distinct layers of aerosol, especially for the small particles of a few nanometres in diameter on 1 particular day. The stratification was almost neutral and two significant aerosol layers were detected with total aerosol number concentrations up to 17 000 ± 3400 cm−3 between 180 and 220 m altitude and 14 000 ± 2800 cm−3 between 550 and 650 m. Apart from those layers, the aerosol distribution was well mixed and reached the total number concentration of less than 8000 ± 1600 cm−3. During another day, the distribution of the small particles in the lowermost ABL was related to the stratification, with continuously decreasing number concentrations from 16 000 ± 3200 cm−3 to a minimum of 4000 ± 800 cm−3 at the top of the inversion at 320 m. Above this, the total number concentration was rather constant. In the region of 500 to 600 m altitude, a significant difference of both CPCs was observed. This event occurred during the boundary layer development in the morning and represents a particle burst within the ABL.