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    Experimental assessment of a micro-pulse lidar system in comparison with reference lidar measurements for aerosol optical properties retrieval
    (Katlenburg-Lindau : European Geosciences Union, 2021) Córdoba-Jabonero, Carmen; Ansmann, Albert; Jiménez, Cristofer; Baars, Holger; López-Cayuela, María-Ángeles; Engelmann, Ronny
    Simultaneous observations of a polarized micro-pulse lidar (P-MPL) system and two reference European Aerosol Research Lidar Network lidars running at the Leipzig site Germany, 51.4g gN, 12.4g gE; 125gmga.s.l.) were performed during a comprehensive 2-month field intercomparison campaign in summer 2019. An experimental assessment regarding both the overlap (OVP) correction of the P-MPL signal profiles and the volume linear depolarization ratio (VLDR) analysis, together with its impact on the retrieval of the aerosol optical properties, is achieved; the experimental procedure used is also described. The optimal lidar-specific OVP function is experimentally determined, highlighting that the one delivered by the P-MPL manufacturer cannot be used long. Among the OVP functions examined, the averaged function between those obtained from the comparison of the P-MPL observations with those of the other two reference lidars seems to be the best proxy at both near- and far-field ranges. In addition, the impact of the OVP function on the accuracy of the retrieved profiles of the total particle backscatter coefficient (PBC) and the particle linear depolarization ratio (PLDR) is examined. The VLDR profile is obtained and compared with that derived from the reference lidar, showing that it needs to be corrected by a small offset value with good accuracy. Once P-MPL measurements are optimally (OVP, VLDR) corrected, both the PBC and PLDR profiles can be accurately derived and are in good agreement with reference aerosol retrievals. Overall, as a systematic requirement for lidar systems, an adequate OVP function determination and VLDR testing analysis needs to be performed on a regular basis to correct the P-MPL measurements in order to derive suitable aerosol products. A dust event observed in Leipzig in June 2019 is used for illustration.
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    Importance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations
    (Katlenburg-Lindau : Copernicus, 2022) Romshoo, Baseerat; Pöhlker, Mira; Wiedensohler, Alfred; Pfeifer, Sascha; Saturno, Jorge; Nowak, Andreas; Ciupek, Krzysztof; Quincey, Paul; Vasilatou, Konstantina; Ess, Michaela N.; Gini, Maria; Eleftheriadis, Konstantinos; Robins, Chris; Gaie-Levrel, François; Müller, Thomas
    Black carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.
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    Influx 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, Christopher
    Black 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).
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    Understanding aerosol microphysical properties from 10 years of data collected at Cabo Verde based on an unsupervised machine learning classification
    (Katlenburg-Lindau : EGU, 2022) Gong, Xianda; Wex, Heike; Müller, Thomas; Henning, Silvia; Voigtländer, Jens; Wiedensohler, Alfred; Stratmann, Frank
    The Cape Verde Atmospheric Observatory (CVAO), which is influenced by both marine and desert dust air masses, has been used for long-term measurements of different properties of the atmospheric aerosol from 2008 to 2017. These properties include particle number size distributions (PNSD), light-absorbing carbon (LAC) and concentrations of cloud condensation nuclei (CCN) together with their hygroscopicity. Here we summarize the results obtained for these properties and use an unsupervised machine learning algorithm for the classification of aerosol types. Five types of aerosols, i.e., marine, freshly formed, mixture, moderate dust and heavy dust, were classified. Air masses during marine periods are from the Atlantic Ocean and during dust periods are from the Sahara Desert. Heavy dust was more frequently present during wintertime, whereas the clean marine periods were more frequently present during springtime. It was observed that during the dust periods CCN number concentrations at a supersaturation of 0.30g% were roughly 2.5 times higher than during marine periods, but the hygroscopicity (κ) of particles in the size range from g1/4g30 to g1/4g175gnm during marine and dust periods were comparable. The long-term data presented here, together with the aerosol classification, can be used as a basis to improve our understanding of annual cycles of the atmospheric aerosol in the eastern tropical Atlantic Ocean and on aerosol-cloud interactions and it can be used as a basis for driving, evaluating and constraining atmospheric model simulations.
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    Cloud top heights and aerosol layer properties from EarthCARE lidar observations: The A-CTH and A-ALD products
    (Katlenburg-Lindau : Copernicus, 2023) Wandinger, Ulla; Haarig, Moritz; Baars, Holger; Donovan, David; van Zadelhoff, Gerd-Jan
    The high-spectral-resolution Atmospheric Lidar (ATLID) on the Earth Cloud, Aerosol and Radiation Explorer (EarthCARE) provides vertically resolved information on aerosols and clouds with unprecedented accuracy. Together with the Cloud Profiling Radar (CPR), the Multi-Spectral Imager (MSI), and the Broad-Band Radiometer (BBR) on the same platform, it allows for a new synergistic view on atmospheric processes related to the interaction of aerosols, clouds, precipitation, and radiation at the global scale. This paper describes the algorithms for the determination of cloud top height and aerosol layer information from ATLID Level 1b (L1b) and Level 2a (L2a) input data. The ATLID L2a Cloud Top Height (A-CTH) and Aerosol Layer Descriptor (A-ALD) products are developed to ensure the provision of atmospheric layer products in continuation of the heritage from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). Moreover, the products serve as input for synergistic algorithms that make use of data from ATLID and MSI. Therefore, the products are provided on the EarthCARE joint standard grid (JSG). A wavelet covariance transform (WCT) method with flexible thresholds is applied to determine layer boundaries from the ATLID Mie co-polar signal. Strong features detected with a horizontal resolution of 1 JSG pixel (approximately 1ĝ€¯km) or 11 JSG pixels are classified as thick or thin clouds, respectively. The top height of the uppermost cloud layer together with information on cloud layering are stored in the A-CTH product for further use in the generation of the ATLID-MSI Cloud Top Height (AM-CTH) synergy product. Aerosol layers are detected as weaker features at a resolution of 11 JSG pixels. Layer-mean optical properties are calculated from the ATLID L2a Extinction, Backscatter and Depolarization (A-EBD) product and stored in the A-ALD product, which also contains the aerosol optical thickness (AOT) of each layer, the stratospheric AOT, and the AOT of the entire atmospheric column. The latter parameter is used to produce the synergistic ATLID-MSI Aerosol Column Descriptor (AM-ACD) later in the processing chain. Several quality criteria are applied in the generation of A-CTH and A-ALD, and respective information is stored in the products. The functionality and performance of the algorithms are demonstrated by applying them to common EarthCARE test scenes. Conclusions are drawn for the application to real-world data and the validation of the products after the launch of EarthCARE.
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    Optical and geometrical aerosol particle properties over the United Arab Emirates
    (Katlenburg-Lindau : EGU, 2020) Filioglou, Maria; Giannakaki, Elina; Backman, John; Kesti, Jutta; Hirsikko, Anne; Engelmann, Ronny; O’Connor, Ewan; Leskinen, Jari T.T.; Shang, Xiaoxia; Korhonen, Hannele; Lihavainen, Heikki; Romakkaniemi, Sami; Komppula, Mika
    One year of ground-based night-time Raman lidar observations has been analysed under the Optimization of Aerosol Seeding In rain enhancement Strategies (OASIS) project, in order to characterize the aerosol particle properties over a rural site in the United Arab Emirates. In total, 1130 aerosol particle layers were detected during the 1-year measurement campaign which took place between March 2018 and February 2019. Several subsequent aerosol layers could be observed simultaneously in the atmosphere up to 11 km. The observations indicate that the measurement site is a receptor of frequent dust events, but predominantly the dust is mixed with aerosols of anthropogenic and/or marine origin. The mean aerosol optical depth over the measurement site ranged at 0.37±0.12 and 0.21±0.11 for 355 and 532 nm, respectively. Moreover, mean lidar ratios of 43±11 sr at a wavelength of 355 nm and 39±10 sr at 532 nm were found. The average linear particle depolarization ratio measured over the course of the campaign was 15±6% and 19±7% at the 355 and 532 nm wavelengths, respectively. Since the region is both a source and a receptor of mineral dust, we have also explored the properties of Arabian mineral dust of the greater area of the United Arab of Emirates and the Arabian Peninsula. The observed Arabian dust particle properties were 45±5 (42±5) sr at 355 (532) nm for the lidar ratio, 25±2% (31±2 %) for the linear particle depolarization ratio at 355 (532) nm, and 0.3±0.2 (0.2±0.2) for the extinction-related Angstrom exponent (backscatterrelated Angstrom exponent) between 355 and 532 nm. This study is the first to report comprehensive optical properties of the Arabian dust particles based on 1-year long observations, using to their fullest the capabilities of a multi-wavelength Raman lidar instrument. The results suggest that the mineral dust properties over the Middle East and western Asia, including the observation site, are comparable to those of African mineral dust with regard to the particle depolarization ratios, but not for lidar ratios. The smaller lidar ratio values in this study compared to the reference studies are attributed to the difference in the geochemical characteristics of the soil originating in the study region compared to northern Africa. © 2020 Royal Society of Chemistry. All rights reserved.
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    Chemical characteristics of cloud water and the impacts on aerosol properties at a subtropical mountain site in Hong Kong SAR
    (Katlenburg-Lindau : EGU, 2020) Li, Tao; Wang, Zhe; Wang, Yaru; Wu, Chen; Liang, Yiheng; Xia, Men; Yu, Chuan; Yun, Hui; Wang, Weihao; Wang, Yan; Guo, Jia; Herrmann, Hartmut; Wang, Tao
    To investigate the cloud water chemistry and the effects of cloud processing on aerosol properties, comprehensive field observations of cloud water, aerosols, and gasphase species were conducted at a mountaintop site in Hong Kong SAR in October and November 2016. The chemical composition of cloud water including water-soluble ions, dissolved organic matter (DOM), carbonyl compounds (refer to aldehydes and acetone), carboxylic acids, and trace metals was quantified. The measured cloud water was very acidic with a mean pH of 3.63, as the ammonium (174 μeq L-1) was insufficient for neutralizing the dominant sulfate (231 μeq L-1) and nitrate (160 μeq L-1). Substantial DOM (9.3 mgC L-1) was found in cloud water, with carbonyl compounds and carboxylic acids accounting for 18% and 6% in carbon molar concentrations, respectively. Different from previous observations, concentrations of methylglyoxal (19.1 μM; μM is equal to μmol L-1) and glyoxal (6.72 μM) were higher than that of formaldehyde (1.59 μM). The partitioning of carbonyls between cloud water and the gas phase was also investigated. The measured aqueous fractions of dicarbonyls were comparable to the theoretical estimations, while significant aqueous-phase supersaturation was found for less soluble monocarbonyls. Both organics and sulfate were significantly produced in cloud water, and the aqueous formation of organics was more enhanced by photochemistry and under less acidic conditions. Moreover, elevated sulfate and organics were measured in the cloudprocessed aerosols, and they were expected to contribute largely to the increase in droplet-mode aerosol mass fraction. This study demonstrates the significant role of clouds in altering the chemical compositions and physical properties of aerosols via scavenging and aqueous chemical processing, providing valuable information about gas-cloud-aerosol interactions in subtropical and coastal regions. © 2020 Author(s). This work is distributed under the Creative Commons Attribution 4.0 License.