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    Aerosol 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.
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    Remote sensing and modelling analysis of the extreme dust storm hitting the Middle East and eastern Mediterranean in September 2015
    (Katlenburg-Lindau : EGU, 2017) Solomos, Stavros; Ansmann, Albert; Mamouri, Rodanthi-Elisavet; Binietoglou, Ioannis; Patlakas, Platon; Marinou, Eleni; Amiridis, Vassilis
    The extreme dust storm that affected the Middle East and the eastern Mediterranean in September 2015 resulted in record-breaking dust loads over Cyprus with aerosol optical depth exceeding 5.0 at 550ĝ€nm. We analyse this event using profiles from the European Aerosol Research Lidar Network (EARLINET) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), geostationary observations from the Meteosat Second Generation (MSG) Spinning Enhanced Visible and Infrared Imager (SEVIRI), and high-resolution simulations from the Regional Atmospheric Modeling System (RAMS). The analysis of modelling and remote sensing data reveals the main mechanisms that resulted in the generation and persistence of the dust cloud over the Middle East and Cyprus. A combination of meteorological and surface processes is found, including (a) the development of a thermal low in the area of Syria that results in unstable atmospheric conditions and dust mobilization in this area, (b) the convective activity over northern Iraq that triggers the formation of westward-moving haboobs that merge with the previously elevated dust layer, and (c) the changes in land use due to war in the areas of northern Iraq and Syria that enhance dust erodibility.
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    Satellite retrievals of dust aerosol over the Red Sea and the Persian Gulf (2005-2015)
    (Katlenburg-Lindau : EGU, 2017) Banks, Jamie R.; Brindley, Helen E.; Stenchikov, Georgiy; Schepanski, Kerstin
    The inter-annual variability of the dust aerosol presence over the Red Sea and the Persian Gulf is analysed over the period 2005-2015. Particular attention is paid to the variation in loading across the Red Sea, which has previously been shown to have a strong, seasonally dependent latitudinal gradient. Over the 11 years considered, the July mean 630 nm aerosol optical depth (AOD) derived from the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) varies between 0.48 and 1.45 in the southern half of the Red Sea. In the north, the equivalent variation is between 0.22 and 0.66. The temporal and spatial pattern of variability captured by SEVIRI is also seen in AOD retrievals from the MODerate Imaging Spectroradiometer (MODIS), but there is a systematic offset between the two records. Comparisons of both sets of retrievals with ship-and land-based AERONET measurements show a high degree of correlation with biases of <0.08. However, these comparisons typically only sample relatively low aerosol loadings. When both records are stratified by AOD retrievals from the Multi-angle Imaging SpectroRadiometer (MISR), opposing behaviour is revealed at high MISR AODs (>1), with offsets of C0.19 for MODIS and 0.06 for SEVIRI. Similar behaviour is also seen over the Persian Gulf. Analysis of the scattering angles at which retrievals from the SEVIRI and MODIS measurements are typically performed in these regions suggests that assumptions concerning particle sphericity may be responsible for the differences seen.
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    EARLINET evaluation of the CATS Level 2 aerosol backscatter coefficient product
    (Katlenburg-Lindau : EGU, 2019) Proestakis, Emmanouil; Amiridis, Vassilis; Marinou, Eleni; Binietoglou, Ioannis; Ansmann, Albert; Wandinger, Ulla; Hofer, Julian; Yorks, John; Nowottnick, Edward; Makhmudov, Abduvosit; Papayannis, Alexandros; Pietruczuk, Aleksander; Gialitaki, Anna; Apituley, Arnoud; Szkop, Artur; Muñoz Porcar, Constantino; Bortoli, Daniele; Dionisi, Davide; Althausen, Dietrich; Mamali, Dimitra; Balis, Dimitris; Nicolae, Doina; Tetoni, Eleni; Liberti, Gian Luigi; Baars, Holger; Mattis, Ina; Stachlewska, Iwona Sylwia; Voudouri, Kalliopi Artemis; Mona, Lucia; Mylonaki, Maria; Perrone, Maria Rita; Costa, Maria João; Sicard, Michael; Papagiannopoulos, Nikolaos; Siomos, Nikolaos; Burlizzi, Pasquale; Pauly, Rebecca; Engelmann, Ronny; Abdullaev, Sabur; Pappalardo, Gelsomina
    We present the evaluation activity of the European Aerosol Research Lidar Network (EARLINET) for the quantitative assessment of the Level 2 aerosol backscatter coefficient product derived by the Cloud-Aerosol Transport System (CATS) aboard the International Space Station (ISS; Rodier et al., 2015). The study employs correlative CATS and EARLINET backscatter measurements within a 50km distance between the ground station and the ISS overpass and as close in time as possible, typically with the starting time or stopping time of the EARLINET performed measurement time window within 90min of the ISS overpass, for the period from February 2015 to September 2016. The results demonstrate the good agreement of the CATS Level 2 backscatter coefficient and EARLINET. Three ISS overpasses close to the EARLINET stations of Leipzig, Germany; Évora, Portugal; and Dushanbe, Tajikistan, are analyzed here to demonstrate the performance of the CATS lidar system under different conditions. The results show that under cloud-free, relative homogeneous aerosol conditions, CATS is in good agreement with EARLINET, independent of daytime and nighttime conditions. CATS low negative biases are observed, partially attributed to the deficiency of lidar systems to detect tenuous aerosol layers of backscatter signal below the minimum detection thresholds; these are biases which may lead to systematic deviations and slight underestimations of the total aerosol optical depth (AOD) in climate studies. In addition, CATS misclassification of aerosol layers as clouds, and vice versa, in cases of coexistent and/or adjacent aerosol and cloud features, occasionally leads to non-representative, unrealistic, and cloud-contaminated aerosol profiles. Regarding solar illumination conditions, low negative biases in CATS backscatter coefficient profiles, of the order of 6.1%, indicate the good nighttime performance of CATS. During daytime, a reduced signal-to-noise ratio by solar background illumination prevents retrievals of weakly scattering atmospheric layers that would otherwise be detectable during nighttime, leading to higher negative biases, of the order of 22.3%. © Author(s) 2019.
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    Particulate sulfur in the upper troposphere and lowermost stratosphere - Sources and climate forcing
    (Katlenburg-Lindau : EGU, 2017) Martinsson, Bengt G.; Friberg, Johan; Sandvik, Oscar S.; Hermann, Markus; van Velthoven, Peter F. J.; Zahn, Andreas
    This study is based on fine-mode aerosol samples collected in the upper troposphere (UT) and the lowermost stratosphere (LMS) of the Northern Hemisphere extratropics during monthly intercontinental flights at 8.8-12 km altitude of the IAGOS-CARIBIC platform in the time period 1999-2014. The samples were analyzed for a large number of chemical elements using the accelerator-based methods PIXE (particle-induced X-ray emission) and PESA (particle elastic scattering analysis). Here the particulate sulfur concentrations, obtained by PIXE analysis, are investigated. In addition, the satellite-borne lidar aboard CALIPSO is used to study the stratospheric aerosol load. A steep gradient in particulate sulfur concentration extends several kilometers into the LMS, as a result of increasing dilution towards the tropopause of stratospheric, particulate sulfur-rich air. The stratospheric air is diluted with tropospheric air, forming the extratropical transition layer (ExTL). Observed concentrations are related to the distance to the dynamical tropopause. A linear regression methodology handled seasonal variation and impact from volcanism. This was used to convert each data point into stand-alone estimates of a concentration profile and column concentration of particulate sulfur in a 3 km altitude band above the tropopause. We find distinct responses to volcanic eruptions, and that this layer in the LMS has a significant contribution to the stratospheric aerosol optical depth and thus to its radiative forcing. Further, the origin of UT particulate sulfur shows strong seasonal variation. We find that tropospheric sources dominate during the fall as a result of downward transport of the Asian tropopause aerosol layer (ATAL) formed in the Asian monsoon, whereas transport down from the Junge layer is the main source of UT particulate sulfur in the first half of the year. In this latter part of the year, the stratosphere is the clearly dominating source of particulate sulfur in the UT during times of volcanic influence and under background conditions.
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    Continuous vertical aerosol profiling with a multi-wavelength Raman polarization lidar over the Pearl River Delta, China
    (Katlenburg-Lindau : EGU, 2017) Heese, Birgit; Baars, Holger; Bohlmann, Stephanie; Althausen, Dietrich; Deng, Ruru
    A dataset of particle optical properties of the highly polluted atmosphere over the Pearl River Delta (PRD), Guangzhou, China, is presented in this paper. The data were derived from the measurements of a multiwavelength Raman and depolarization lidar PollyXT and a co-located AERONET sun photometer. The measurement campaign was conducted from November 2011 to mid-June 2012. These are the first Raman lidar measurements in the PRD that lasted for several months. A mean value of aerosol optical depth (AOD) of 0.54±0.33 was observed by the sun photometer at 500 nm in the polluted atmosphere over this megacity for the whole measurement period. The lidar profiles frequently show lofted aerosol layers, which reach altitudes of up to 2 to 3 km and, especially during the spring season, up to 5 km. These layers contain between 12 and 56% of the total AOD, with the highest values in spring. The aerosol types in these lofted layers are classified by their optical properties. The observed lidar ratio values range from 30 to 80 sr with a mean value of 48.0±10.7 sr at 532 nm. The linear particle depolarization ratio at 532 nm lies mostly below 5 %, with a mean value of 3.6±3.7 %. The majority of the Ångström exponents lie between 0.5 and 1.5, indicating a mixture of fine- and coarsemode aerosols. These results reveal that mostly urban pollution particles mixed with particles produced from biomass and industrial burning are present in the atmosphere above the Pearl River Delta. Trajectory analyses show that these pollution mixtures arise mainly from local and regional sources.
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    Detection and attribution of aerosol-cloud interactions in large-domain large-eddy simulations with the ICOsahedral Non-hydrostatic model
    (Katlenburg-Lindau : EGU, 2020) Costa-Surós, Montserrat; Sourdeval, Odran; Acquistapace, Claudia; Baars, Holger; Carbajal Henken, Cintia; Genz, Christa; Hesemann, Jonas; Jimenez, Cristofer; König, Marcel; Kretzschmar, Jan; Madenach, Nils; Meyer, Catrin I.; Schrödner, Roland; Seifert, Patric; Senf, Fabian; Brueck, Matthias; Cioni, Guido; Engels, Jan Frederik; Fieg, Kerstin; Gorges, Ksenia; Heinze, Rieke; Kumar Siligam, Pavan; Burkhardt, Ulrike; Crewell, Susanne; Hoose, Corinna; Seifert, Axel; Tegen, Ina; Quaas, Johannes
    Clouds and aerosols contribute the largest uncertainty to current estimates and interpretations of the Earth's changing energy budget. Here we use a new-generation large-domain large-eddy model, ICON-LEM (ICOsahedral Non-hydrostatic Large Eddy Model), to simulate the response of clouds to realistic anthropogenic perturbations in aerosols serving as cloud condensation nuclei (CCN). The novelty compared to previous studies is that (i) the LEM is run in weather prediction mode and with fully interactive land surface over a large domain and (ii) a large range of data from various sources are used for the detection and attribution. The aerosol perturbation was chosen as peak-aerosol conditions over Europe in 1985, with more than fivefold more sulfate than in 2013. Observational data from various satellite and ground-based remote sensing instruments are used, aiming at the detection and attribution of this response. The simulation was run for a selected day (2 May 2013) in which a large variety of cloud regimes was present over the selected domain of central Europe. It is first demonstrated that the aerosol fields used in the model are consistent with corresponding satellite aerosol optical depth retrievals for both 1985 (perturbed) and 2013 (reference) conditions. In comparison to retrievals from groundbased lidar for 2013, CCN profiles for the reference conditions were consistent with the observations, while the ones for the 1985 conditions were not. Similarly, the detection and attribution process was successful for droplet number concentrations: the ones simulated for the 2013 conditions were consistent with satellite as well as new ground-based lidar retrievals, while the ones for the 1985 conditions were outside the observational range. For other cloud quantities, including cloud fraction, liquid water path, cloud base altitude and cloud lifetime, the aerosol response was small compared to their natural vari ability. Also, large uncertainties in satellite and ground-based observations make the detection and attribution difficult for these quantities. An exception to this is the fact that at a large liquid water path value (LWP > 200 g m-2), the control simulation matches the observations, while the perturbed one shows an LWP which is too large. The model simulations allowed for quantifying the radiative forcing due to aerosol-cloud interactions, as well as the adjustments to this forcing. The latter were small compared to the variability and showed overall a small positive radiative effect. The overall effective radiative forcing (ERF) due to aerosol-cloud interactions (ERFaci) in the simulation was dominated thus by the Twomey effect and yielded for this day, region and aerosol perturbation-2:6 W m-2. Using general circulation models to scale this to a global-mean present-day vs. pre-industrial ERFaci yields a global ERFaci of-0:8 W m-2 © 2020 Author(s).
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    Sun photometer retrievals of Saharan dust properties over Barbados during SALTRACE
    (Katlenburg-Lindau : EGU, 2019) Toledano, Carlos; Torres, Benjamín; Velasco-Merino, Cristian; Althausen, Dietrich; Groß, Silke; Wiegner, Matthias; Weinzierl, Bernadett; Gasteiger, Josef; Ansmann, Albert; González, Ramiro; Mateos, David; Farrel, David; Müller, Thomas; Haarig, Moritz; Cachorro, Victoria E.
    The Saharan Aerosol Long-Range Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) was devoted to the investigation of Saharan dust properties over the Caribbean. The campaign took place in June-July 2013. A wide set of ground-based and airborne aerosol instrumentation was deployed at the island of Barbados for a comprehensive experiment. Several sun photometers performed measurements during this campaign: two AERONET (Aerosol Robotic Network) Cimel sun photometers and the Sun and Sky Automatic Radiometer (SSARA). The sun photometers were co-located with the ground-based multi-wavelength lidars BERTHA (Backscatter Extinction lidar Ratio Temperature Humidity profiling Apparatus) and POLIS (Portable Lidar System). Aerosol properties derived from direct sun and sky radiance observations are analyzed, and a comparison with the co-located lidar and in situ data is provided. The time series of aerosol optical depth (AOD) allows identifying successive dust events with short periods in between in which the marine background conditions were observed. The moderate aerosol optical depth in the range of 0.3 to 0.6 was found during the dust periods. The sun photometer infrared channel at the 1640nm wavelength was used in the retrieval to investigate possible improvements to aerosol size retrievals, and it was expected to have a larger sensitivity to coarse particles. The comparison between column (aerosol optical depth) and surface (dust concentration) data demonstrates the connection between the Saharan Air Layer and the boundary layer in the Caribbean region, as is shown by the synchronized detection of the successive dust events in both datasets. However the differences of size distributions derived from sun photometer data and in situ observations reveal the difficulties in carrying out a column closure study. © 2019 All rights reserved.
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    Constraining the Twomey effect from satellite observations: Issues and perspectives
    (Katlenburg-Lindau : EGU, 2020) Quaas, Johannes; Arola, Antti; Cairns, Brian; Christensen, Matthew; Deneke, Hartwig; Ekman, Annica M.L.; Feingold, Graham; Fridlind, Ann; Gryspeerdt, Edward; Hasekamp, Otto; Li, Zhanqing; Lipponen, Antti; Ma, Po-Lun; Mülmenstädt, Johannes; Nenes, Athanasios; Penner, Joyce E.; Rosenfeld, Daniel; Schrödner, Roland; Sinclair, Kenneth; Sourdeval, Odran; Stier, Philip; Tesche, Matthias; van Diedenhoven, Bastiaan; Wendisch, Manfred
    The Twomey effect describes the radiative forcing associated with a change in cloud albedo due to an increase in anthropogenic aerosol emissions. It is driven by the perturbation in cloud droplet number concentration (1Nd; ant) in liquid-water clouds and is currently understood to exert a cooling effect on climate. The Twomey effect is the key driver in the effective radiative forcing due to aerosol cloud interactions, but rapid adjustments also contribute. These adjustments are essentially the responses of cloud fraction and liquid water path to 1Nd; ant and thus scale approximately with it. While the fundamental physics of the influence of added aerosol particles on the droplet concentration (Nd) is well described by established theory at the particle scale (micrometres), how this relationship is expressed at the large-scale (hundreds of kilometres) perturbation, 1Nd; ant, remains uncertain. The discrepancy between process understanding at particle scale and insufficient quantification at the climate-relevant large scale is caused by co-variability of aerosol particles and updraught velocity and by droplet sink processes. These operate at scales on the order of tens of me-Tres at which only localised observations are available and at which no approach yet exists to quantify the anthropogenic perturbation. Different atmospheric models suggest diverse magnitudes of the Twomey effect even when applying the same anthropogenic aerosol emission perturbation. Thus, observational data are needed to quantify and constrain the Twomey effect. At the global scale, this means satellite data. There are four key uncertainties in determining 1Nd; ant, namely the quantification of (i) the cloud-Active aerosol the cloud condensation nuclei (CCN) concentrations at or above cloud base, (ii) Nd, (iii) the statistical approach for inferring the sensitivity of Nd to aerosol particles from the satellite data and (iv) uncertainty in the anthropogenic perturbation to CCN concentrations, which is not easily accessible from observational data. This review discusses deficiencies of current approaches for the different aspects of the problem and proposes several ways forward: in terms of CCN, retrievals of optical quantities such as aerosol optical depth suffer from a lack of vertical resolution, size and hygroscopicity information, non-direct relation to the concentration of aerosols, difficulty to quantify it within or below clouds, and the problem of insufficient sensitivity at low concentrations, in addition to retrieval errors. A future path forward can include utilising co-located polarimeter and lidar instruments, ideally including high-spectral-resolution lidar capability at two wavelengths to maximise vertically resolved size distribution information content. In terms of Nd, a key problem is the lack of operational retrievals of this quantity and the inaccuracy of the retrieval especially in broken-cloud regimes. As for the Nd-To-CCN sensitivity, key issues are the updraught distributions and the role of Nd sink processes, for which empirical assessments for specific cloud regimes are currently the best solutions. These considerations point to the conclusion that past studies using existing approaches have likely underestimated the true sensitivity and, thus, the radiative forcing due to the Twomey effect. © 2020 BMJ Publishing Group. All rights reserved.
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    Microphysical characterization of long-range transported biomass burning particles from North America at three EARLINET stations
    (Katlenburg-Lindau : EGU, 2017) Ortiz-Amezcua, Pablo; Guerrero-Rascado, Juan Luis; Granados-Muñoz, María José; Benavent-Oltra, José Antonio; Böckmann, Christine; Samaras, Stefanos; Stachlewska, Iwona S.; Janicka, Łucja; Baars, Holger; Bohlmann, Stephanie; Alados-Arboledas, Lucas
    Strong events of long-range transported biomass burning aerosol were detected during July 2013 at three EARLINET (European Aerosol Research Lidar Network) stations, namely Granada (Spain), Leipzig (Germany) and Warsaw (Poland). Satellite observations from MODIS (Moderate Resolution Imaging Spectroradiometer) and CALIOP (Cloud-Aerosol Lidar with Orthogonal Polarization) instruments, as well as modeling tools such as HYSPLIT (Hybrid Single-Particle Lagrangian Integrated Trajectory) and NAAPS (Navy Aerosol Analysis and Prediction System), have been used to estimate the sources and transport paths of those North American forest fire smoke particles. A multiwavelength Raman lidar technique was applied to obtain vertically resolved particle optical properties, and further inversion of those properties with a regularization algorithm allowed for retrieving microphysical information on the studied particles. The results highlight the presence of smoke layers of 1-2 km thickness, located at about 5 km a.s.l. altitude over Granada and Leipzig and around 2.5 km a.s.l. at Warsaw. These layers were intense, as they accounted for more than 30 % of the total AOD (aerosol optical depth) in all cases, and presented optical and microphysical features typical for different aging degrees: Color ratio of lidar ratios (LR532/LR355) around 2, α-related ängström exponents of less than 1, effective radii of 0.3 μm and large values of single scattering albedos (SSA), nearly spectrally independent. The intensive microphysical properties were compared with columnar retrievals form co-located AERONET (Aerosol Robotic Network) stations. The intensity of the layers was also characterized in terms of particle volume concentration, and then an experimental relationship between this magnitude and the particle extinction coefficient was established.