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- ItemPolarization lidar: An extended three-signal calibration approach(Katlenburg-Lindau : Copernicus, 2019) Jimenez, Cristofer; Ansmann, Albert; Engelmann, Ronny; Haarig, Moritz; Schmidt, Jörg; Wandinger, UllaWe present a new formalism to calibrate a threesignal polarization lidar and to measure highly accurate height profiles of the volume linear depolarization ratios under realistic experimental conditions. The methodology considers elliptically polarized laser light, angular misalignment of the receiver unit with respect to the main polarization plane of the laser pulses, and cross talk among the receiver channels. A case study of a liquid-water cloud observation demonstrates the potential of the new technique. Long-term observations of the calibration parameters corroborate the robustness of the method and the long-term stability of the three-signal polarization lidar. A comparison with a second polarization lidar shows excellent agreement regarding the derived volume linear polarization ratios in different scenarios: A biomass burning smoke event throughout the troposphere and the lower stratosphere up to 16 km in height, a dust case, and also a cirrus cloud case. © Author(s) 2019.
- ItemInflux of African biomass burning aerosol during the Amazonian dry season through layered transatlantic transport of black carbon-rich smoke(Katlenburg-Lindau : EGU, 2020) Holanda, Bruna A.; Pöhlker, Mira L.; Walter, David; Saturno, Jorge; Sörgel, Matthias; Ditas, Jeannine; Ditas, Florian; Schulz, Christiane; Aurélio Franco, Marco; Wang, Qiaoqiao; Donth, Tobias; Artaxo, Paulo; Barbosa, Henrique M.J.; Borrmann, Stephan; Braga, Ramon; Brito, Joel; Cheng, Yafang; Dollner, Maximilian; Kaiser, JohannesW.; Klimach, Thomas; Knote, Christoph; Krüger, Ovid O.; Fütterer, Daniel; Lavrič, Jošt V.; Ma, Nan; Machado, Luiz A.T.; Ming, Jing; Morais, Fernando G.; Paulsen, Hauke; Sauer, Daniel; Schlager, Hans; Schneider, Johannes; Su, Hang; Weinzierl, Bernadett; Walser, Adrian; Wendisch, Manfred; Ziereis, Helmut; Zöger, Martin; Pöschl, Ulrich; Andreae, Meinrat O.; Pöhlker, ChristopherBlack carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline of the Amazon Basin, we observed a BCrich layer at ∼ 3:5 km altitude with a vertical extension of ∼ 0:3 km. Backward trajectories suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer and that the observed BB smoke had undergone more than 10 d of atmospheric transport and aging over the South Atlantic before reaching the Amazon Basin. The aged smoke is characterized by a dominant accumulation mode, centered at about 130 nm, with a particle concentration of Nacc D 850±330 cm-3. The rBC particles account for ∼ 15 % of the submicrometer aerosol mass and ∼ 40 % of the total aerosol number concentration. This corresponds to a mass concentration range from 0.5 to 2 μ g m-3 (1st to 99th percentiles) and a number concentration range from 90 to 530 cm-3. Along with rBC, high cCO (150 ± 30 ppb) and cO3 (56 ± 9 ppb) mixing ratios support the biomass burning origin and pronounced photochemical aging of this layer. Upon reaching the Amazon Basin, it started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations together with the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the northern and central Amazonian aerosol population during the BBinfluenced season (July to December). In fact, the early BB season (July to September) in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season (October to December) appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes in aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 11 to 6 ng m-3 ppb-1). Our results suggest that, despite the high fraction of BC particles, the African BB aerosol acts as efficient cloud condensation nuclei (CCN), with potentially important implications for aerosol-cloud interactions and the hydrological cycle in the Amazon. © 2020 Author(s).
- ItemBiomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240a.s.l.)(Katlenburg-Lindau : EGU, 2019) Chauvigné, Aurélien; Aliaga, Diego; Sellegri, Karine; Montoux, Nadège; Krejci, Radovan; Močnik, Griša; Moreno, Isabel; Müller, Thomas; Pandolfi, Marco; Velarde, Fernando; Weinhold, Kay; Ginot, Patrick; Wiedensohler, Alfred; Andrade, Marcos; Laj, PaoloThis study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20km away and 1.5km below the sampling site. The extended multi-year record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96Mm-1 respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68Mm-1 respectively) and higher values during the dry season (0.80, 11.23, and 14.51Mm-1 respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28% to 80% increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere. © Author(s) 2019.
- ItemThe impact of biomass burning and aqueous-phase processing on air quality: A multi-year source apportionment study in the Po Valley, Italy(Katlenburg-Lindau : EGU, 2020) Paglione, Marco; Gilardoni, Stefania; Rinaldi, Matteo; Decesari, Stefano; Zanca, Nicola; Sandrini, Silvia; Giulianelli, Lara; Bacco, Dimitri; Ferrari, Silvia; Poluzzi, Vanes; Scotto, Fabiana; Trentini, Arianna; Poulain, Laurent; Herrmann, Hartmut; Wiedensohler, Alfred; Canonaco, Francesco; Prévôt, André S.H.; Massoli, Paola; Carbone, Claudio; Facchini, Maria Cristina; Fuzzi, SandroThe Po Valley (Italy) is a well-known air quality hotspot characterized by particulate matter (PM) levels well above the limit set by the European Air Quality Directive and by the World Health Organization, especially during the colder season. In the framework of Emilia-Romagna regional project "Supersito", the southern Po Valley submicron aerosol chemical composition was characterized by means of high-resolution aerosol mass spectroscopy (HR-AMS) with the specific aim of organic aerosol (OA) characterization and source apportionment. Eight intensive observation periods (IOPs) were carried out over 4 years (from 2011 to 2014) at two different sites (Bologna, BO, urban background, and San Pietro Capofiume, SPC, rural background), to characterize the spatial variability and seasonality of the OA sources, with a special focus on the cold season. On the multi-year basis of the study, the AMS observations show that OA accounts for averages of 45 ± 8 % (ranging from 33 % to 58 %) and 46 ± 7 % (ranging from 36 % to 50 %) of the total non-refractory submicron particle mass (PM1-NR) at the urban and rural sites, respectively. Primary organic aerosol (POA) comprises biomass burning (23±13 % of OA) and fossil fuel (12±7 %) contributions with a marked seasonality in concentration. As expected, the biomass burning contribution to POA is more significant at the rural site (urban / rural concentration ratio of 0.67), but it is also an important source of POA at the urban site during the cold season, with contributions ranging from 14 % to 38 % of the total OA mass. Secondary organic aerosol (SOA) contributes to OA mass to a much larger extent than POA at both sites throughout the year (69 ± 16 % and 83 ± 16 % at the urban and rural sites, respectively), with important implications for public health. Within the secondary fraction of OA, the measurements highlight the importance of biomass burning aging products during the cold season, even at the urban background site. This biomass burning SOA fraction represents 14 %-44 % of the total OA mass in the cold season, indicating that in this region a major contribution of combustion sources to PM mass is mediated by environmental conditions and atmospheric reactivity. © 2020 Author(s).
- ItemVertical aerosol distribution in the southern hemispheric midlatitudes as observed with lidar in Punta Arenas, Chile (53.2° and 70.9° W), during ALPACA(Katlenburg-Lindau : EGU, 2019) Foth, Andreas; Kanitz, Thomas; Engelmann, Ronny; Baars, Holger; Radenz, Martin; Seifert, Patric; Barja, Boris; Fromm, Michael; Kalesse, Heike; Ansmann, AlbertWithin this publication, lidar observations of the vertical aerosol distribution above Punta Arenas, Chile (53.2 S and 70.9 W), which have been performed with the Raman lidar PollyXT from December 2009 to April 2010, are presented. Pristine marine aerosol conditions related to the prevailing westerly circulation dominated the measurements. Lofted aerosol layers could only be observed eight times during the whole measurement period. Two case studies are presented showing long-range transport of smoke from biomass burning in Australia and regionally transported dust from the Patagonian Desert, respectively. The aerosol sources are identified by trajectory analyses with the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) and FLEXible PARTicle dispersion model (FLEXPART). However, seven of the eight analysed cases with lofted layers show an aerosol optical thickness of less than 0.05. From the lidar observations, a mean planetary boundary layer (PBL) top height of 1150 350m was determined. An analysis of particle backscatter coefficients confirms that the majority of the aerosol is attributed to the PBL, while the free troposphere is characterized by a very low background aerosol concentration. The ground-based lidar observations at 532 and 1064 nm are supplemented by the Aerosol Robotic Network (AERONET) Sun photometers and the space-borne Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The averaged aerosol optical thickness (AOT) determined by CALIOP was 0:02 0:01 in Punta Arenas from 2009 to 2010. © Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
- ItemThe EMEP Intensive Measurement Period campaign, 2008-2009: Characterizing carbonaceous aerosol at nine rural sites in Europe(Katlenburg-Lindau : EGU, 2019) Yttri, Karl Espen; Simpson, David; Bergström, Robert; Kiss, Gyula; Szidat, Sönke; Ceburnis, Darius; Eckhardt, Sabine; Hueglin, Christoph; Nøjgaard, Jacob Klenø; Perrino, Cinzia; Pisso, Ignazio; Prevot, Andre Stephan Henry; Putaud, Jean-Philippe; Spindler, Gerald; Vana, Milan; Zhang, Yan-Lin; Aas, WencheCarbonaceous aerosol (total carbon, TCp) was source apportioned at nine European rural background sites, as part of the European Measurement and Evaluation Programme (EMEP) Intensive Measurement Periods in fall 2008 and winter/spring 2009. Five predefined fractions were apportioned based on ambient measurements: elemental and organic carbon, from combustion of biomass (ECbb and OCbb) and from fossil-fuel (ECff and OCff) sources, and remaining non-fossil organic carbon (OCrnf), dominated by natural sources.OCrnf made a larger contribution to TCp than anthropogenic sources (ECbb, OCbb, ECff, and OCff) at four out of nine sites in fall, reflecting the vegetative season, whereas anthropogenic sources dominated at all but one site in winter/spring. Biomass burning (OCbb + ECbb) was the major anthropogenic source at the central European sites in fall, whereas fossil-fuel (OCff + ECff) sources dominated at the southernmost and the two northernmost sites. Residential wood burning emissions explained 30 %-50 % of TCp at most sites in the first week of sampling in fall, showing that this source can be the dominant one, even outside the heating season. In winter/spring, biomass burning was the major anthropogenic source at all but two sites, reflecting increased residential wood burning emissions in the heating season. Fossil-fuel sources dominated EC at all sites in fall, whereas there was a shift towards biomass burning for the southernmost sites in winter/spring.Model calculations based on base-case emissions (mainly officially reported national emissions) strongly underpredicted observational derived levels of OCbb and ECbb outside Scandinavia. Emissions based on a consistent bottom-up inventory for residential wood burning (and including intermediate volatility compounds, IVOCs) improved model results compared to the base-case emissions, but modeled levels were still substantially underestimated compared to observational derived OCbb and ECbb levels at the southernmost sites.Our study shows that natural sources are a major contributor to carbonaceous aerosol in Europe, even in fall and in winter/spring, and that residential wood burning emissions are equally as large as or larger than that of fossil-fuel sources, depending on season and region. The poorly constrained residential wood burning emissions for large parts of Europe show the obvious need to improve emission inventories, with harmonization of emission factors between countries likely being the most important step to improve model calculations for biomass burning emissions, and European PM2.5 concentrations in general. © Author(s) 2019.