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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.
- ItemAerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters(Katlenburg-Lindau : EGU, 2016) Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ∼ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.
- ItemAn optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC(München : European Geopyhsical Union, 2016) Hermann, Markus; Weigelt, Andreas; Assmann, Denise; Pfeifer, Sascha; Müller, Thomas; Conrath, Thomas; Voigtländer, Jens; Heintzenberg, Jost; Wiedensohler, Alfred; Martinsson, Bengt G.; Deshler, Terry; Brenninkmeijer, Carl A.M.; Zahn, AndreasThe particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System – Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130–1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.
- ItemVertically resolved dust optical properties during SAMUM: Tinfou compared to Ouarzazate(Milton Park : Taylor & Francis, 2017) Heese, Birgit; Althausen, Dietrich; Dinter, Tilman; Esselborn, Michael; Müller, Thomas; Tesche, Matthias; Wiegner, MatthiasVertical profiles of dust key optical properties are presented from measurements during the Saharan Mineral Dust Experiment (SAMUM) by Raman and depolarization lidar at two ground-based sites and by airborne high spectral resolution lidar. One of the sites, Tinfou, is located close to the border of the Sahara in Southern Morocco and was the main in situ site during SAMUM. The other site was Ouarzazate airport, the main lidar site. From the lidar measurements the spatial distribution of the dust between Tinfou and Ouarzazate was derived for 1 d. The retrieved profiles of backscatter and extinction coefficients and particle depolarization ratios show comparable dust optical properties, a similar vertical structure of the dust layer, and a height of about 4 km asl at both sites. The airborne cross-section of the extinction coefficient at the two sites confirms the low variability in dust properties. Although the general picture of the dust layer was similar, the lidar measurements reveal a higher dust load closer to the dust source. Nevertheless, the observed intensive optical properties were the same. These results indicate that the lidar measurements at two sites close to the dust source are both representative for the SAMUM dust conditions.
- ItemVertical profiling of Saharan dust with Raman lidars and airborne HSRL in southern Morocco during SAMUM(Milton Park : Taylor & Francis, 2017) Tesche, Matthias; Ansmann, Albert; MüLLER, Detlef; Althausen, Dietrich; Mattis, Ina; Heese, Birgit; Freudenthaler, Volker; Wiegner, Matthias; Esselborn, Michael; Pisani, Gianluca; Knippertz, PeterThree ground-based Raman lidars and an airborne high-spectral-resolution lidar (HSRL) were operated duringSAMUM 2006 in southern Morocco to measure height profiles of the volume extinction coefficient, the extinction-to-backscatter ratio and the depolarization ratio of dust particles in the Saharan dust layer at several wavelengths. Aerosol Robotic Network (AERONET) Sun photometer observations and radiosoundings of meteorological parameters complemented the ground-based activities at the SAMUM station of Ouarzazate. Four case studies are presented. Two case studies deal with the comparison of observations of the three ground-based lidars during a heavy dust outbreak and of the ground-based lidars with the airborne lidar. Two further cases show profile observations during satellite overpasses on 19 May and 4 June 2006. The height resolved statistical analysis reveals that the dust layer top typically reaches 4–6 km height above sea level (a.s.l.), sometimes even 7 km a.s.l.. Usually, a vertically inhomogeneous dust plume with internal dust layers was observed in the morning before the evolution of the boundary layer started. The Saharan dust layer was well mixed in the early evening. The 500 nm dust optical depth ranged from 0.2–0.8 at the field site south of the High Atlas mountains, Ångström exponents derived from photometer and lidar data were between 0–0.4. The volume extinction coefficients (355, 532 nm) varied from 30–300Mm−1 with a mean value of 100Mm−1 in the lowest 4 km a.s.l.. On average, extinction-to-backscatter ratios of 53–55 sr (±7–13 sr) were obtained at 355, 532 and 1064 nm.