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- Item3+2 + X : what is the most useful depolarization input for retrieving microphysical properties of non-spherical particles from lidar measurements using the spheroid model of Dubovik et al. (2006)?(Katlenburg-Lindau : Copernicus, 2019) Tesche, Matthias; Kolgotin, Alexei; Haarig, Moritz; Burton, Sharon P.; Ferrare, Richard A.; Hostetler, Chris A.; Müller, DetlefThe typical multiwavelength aerosol lidar data set for inversion of optical to microphysical parameters is composed of three backscatter coefficients (β) at 355, 532, and 1064 nm and two extinction coefficients (α) at 355 and 532 nm. This data combination is referred to as a 3β C 2α or 3 + 2 data set. This set of data is sufficient for retrieving some important microphysical particle parameters if the particles have spherical shape. Here, we investigate the effect of including the particle linear depolarization ratio (δ) as a third input parameter for the inversion of lidar data. The inversion algorithm is generally not used if measurements show values of d that exceed 0.10 at 532 nm, i.e. in the presence of nonspherical particles such as desert dust, volcanic ash, and, under special circumstances, biomass-burning smoke. We use experimental data collected with instruments that are capable of measuring d at all three lidar wavelengths with an inversion routine that applies the spheroidal light-scattering model of Dubovik et al. (2006) with a fixed axis-ratio distribution to replicate scattering properties of non-spherical particles. The inversion gives the fraction of spheroids required to replicate the optical data as an additional output parameter. This is the first systematic test of the effect of using all theoretically possible combinations of d taken at 355, 532, and 1064 nm as input in the lidar data inversion. We find that depolarization information of at least one wavelength already provides useful information for the inversion of optical data that have been collected in the presence of non-spherical mineral dust particles. However, any choice of d will give lower values of the single-scattering albedo than the traditional 3 + 2 data set. We find that input data sets that include d355 give a spheroid fraction that closely resembles the dust ratio we obtain from using β532 and d532 in a methodology applied in aerosol-type separation. The use of d355 in data sets of two or three d? reduces the spheroid fraction that is retrieved when using d532 and d1064. Use of the latter two parameters without accounting for d355 generally leads to high spheroid fractions that we consider not trustworthy. The use of three d instead of two δ, including the constraint that one of these is measured at 355 nm does not provide any advantage over using 3 + 2 + d355 for the observations with varying contributions of mineral dust considered here. However, additional measurements at wavelengths different from 355 nm would be desirable for application to a wider range of aerosol scenarios that may include non-spherical smoke particles, which can have values of d355 that are indistinguishable from those found for mineral dust. We therefore conclude that - depending on measurement capability - the future standard input for inversion of lidar data taken in the presence of mineral dust particles and using the spheroid model of Dubovik et al. (2006) might be 3+2Cδ355 or 3 + 2 + δ355 + δ532. © 2019 The Author(s).
- ItemRetrieval of ice-nucleating particle concentrations from lidar observations and comparison with UAV in situ measurements(Katlenburg-Lindau : EGU, 2019) Marinou, Eleni; Tesche, Matthias; Nenes, Athanasios; Ansmann, Albert; Schrod, Jann; Mamali, Dimitra; Tsekeri, Alexandra; Pikridas, Michael; Baars, Holger; Engelmann, Ronny; Voudouri, Kalliopi-Artemis; Solomos, Stavros; Sciare, Jean; Groß, Silke; Ewald, Florian; Amiridis, VassilisAerosols that are efficient ice-nucleating particles (INPs) are crucial for the formation of cloud ice via heterogeneous nucleation in the atmosphere. The distribution of INPs on a large spatial scale and as a function of height determines their impact on clouds and climate. However, in situ measurements of INPs provide sparse coverage over space and time. A promising approach to address this gap is to retrieve INP concentration profiles by combining particle concentration profiles derived by lidar measurements with INP efficiency parameterizations for different freezing mechanisms (immersion freezing, deposition nucleation). Here, we assess the feasibility of this new method for both ground-based and spaceborne lidar measurements, using in situ observations collected with unmanned aerial vehicles (UAVs) and subsequently analyzed with the FRIDGE (FRankfurt Ice nucleation Deposition freezinG Experiment) INP counter from an experimental campaign at Cyprus in April 2016. Analyzing five case studies we calculated the cloud-relevant particle number concentrations using lidar measurements (n250,dry with an uncertainty of 20 % to 40 % and Sdry with an uncertainty of 30 % to 50 %), and we assessed the suitability of the different INP parameterizations with respect to the temperature range and the type of particles considered. Specifically, our analysis suggests that our calculations using the parameterization of Ullrich et al. (2017) (applicable for the temperature range −50 to −33 ∘C) agree within 1 order of magnitude with the in situ observations of nINP; thus, the parameterization of Ullrich et al. (2017) can efficiently address the deposition nucleation pathway in dust-dominated environments. Additionally, our calculations using the combination of the parameterizations of DeMott et al. (2015, 2010) (applicable for the temperature range −35 to −9 ∘C) agree within 2 orders of magnitude with the in situ observations of INP concentrations (nINP) and can thus efficiently address the immersion/condensation pathway of dust and nondust particles. The same conclusion is derived from the compilation of the parameterizations of DeMott et al. (2015) for dust and Ullrich et al. (2017) for soot.
- ItemEARLINET 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, GelsominaWe 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.
- 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.
- ItemSun 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.
- ItemHighly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol(Washington, DC : ACS Publ., 2019) Bianchi, Federico; Kurtén, Theo; Riva, Matthieu; Mohr, Claudia; Rissanen, Matti P.; Roldin, Pontus; Berndt, Torsten; Crounse, John D.; Wennberg, Paul O.; Mentel, Thomas F.; Wildt, Jürgen; Junninen, Heikki; Jokinen, Tuija; Kulmala, Markku; Worsnop, Douglas R.; Thornton, Joel A.; Donahue, Neil; Kjaergaard, Henrik G.; Ehn, MikaelHighly oxygenated organic molecules (HOM) are formed in the atmosphere via autoxidation involving peroxy radicals arising from volatile organic compounds (VOC). HOM condense on pre-existing particles and can be involved in new particle formation. HOM thus contribute to the formation of secondary organic aerosol (SOA), a significant and ubiquitous component of atmospheric aerosol known to affect the Earth's radiation balance. HOM were discovered only very recently, but the interest in these compounds has grown rapidly. In this Review, we define HOM and describe the currently available techniques for their identification/quantification, followed by a summary of the current knowledge on their formation mechanisms and physicochemical properties. A main aim is to provide a common frame for the currently quite fragmented literature on HOM studies. Finally, we highlight the existing gaps in our understanding and suggest directions for future HOM research. © 2019 American Chemical Society.
- ItemInfrequent new particle formation over the remote boreal forest of Siberia(Amsterdam [u.a.] : Elsevier Science, 2018) Wiedensohler, A.; Ma, N.; Birmili, W.; Heintzenberg, J.; Ditas, F.; Andreae, M.O.; Panov, A.Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Ltd
- ItemVariability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations(Amsterdam [u.a.] : Elsevier Science, 2018) Sun, J.; Birmili, W.; Hermann, M.; Tuch, T.; Weinhold, K.; Spindler, G.; Schladitz, A.; Bastian, S.; Löschau, G.; Cyrys, J.; Gu, J.; Flentje, H.; Briel, B.; Asbac, C.; Kaminski, H.; Ries, L.; Sohme, R.; Gerwig, H.; Wirtz, K.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ma, N.; Wiedensohler, A.This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
- ItemDo new sea spray aerosol source functions improve the results of a regional aerosol model?(Amsterdam [u.a.] : Elsevier Science, 2018) Barthel, Stefan; Tegen, Ina; Wolke, RalfSea spray aerosol particle is a dominating part of the global aerosol mass load of natural origin. Thus, it strongly influences the atmospheric radiation balance and cloud properties especially over the oceans. Uncertainties of the estimated climate impacts by this aerosol type are partly caused by the uncertainties in the particle size dependent emission fluxes of sea spray aerosol particle. We present simulations with a regional aerosol transport model system in two domains, for three months and compared the model results to measurements at four stations using various sea spray aerosol particle source source functions. Despite these limitations we found the results using different source functions are within the range of most model uncertainties. Especially the model's ability to produce realistic wind speeds is crucial. Furthermore, the model results are more affected by a function correcting the emission flux for the effect of the sea surface temperature than by the use of different source functions. © 2018 The Authors
- ItemEURODELTA III exercise: An evaluation of air quality models’ capacity to reproduce the carbonaceous aerosol(Amsterdam : Elsevier, 2019) Mircea, Mihaela; Bessagnet, Bertrand; D'Isidoro, Massimo; Pirovano, Guido; Aksoyoglu, Sebnem; Ciarelli, Giancarlo; Tsyro, Svetlana; Manders, Astrid; Bieser, Johannes; Stern, Rainer; Vivanco, Marta García; Cuvelier, Cornelius; Aas, Wenche; Prévôt, André S.H.; Aulinger, Armin; Briganti, Gino; Calori, Giuseppe; Cappelletti, Andrea; Colette, Augustin; Couvidat, Florian; Fagerli, Hilde; Finardi, Sandro; Kranenburg, Richard; Rouïl, Laurence; Silibello, Camillo; Spindler, Gerald; Poulain, Laurent; Herrmann, Hartmut; Jimenez, Jose L.; Day, Douglas A.; Tiitta, Petri; Carbone, SamaraThe carbonaceous aerosol accounts for an important part of total aerosol mass, affects human health and climate through its effects on physical and chemical properties of the aerosol, yet the understanding of its atmospheric sources and sinks is still incomplete. This study shows the state-of-the-art in modelling carbonaceous aerosol over Europe by comparing simulations performed with seven chemical transport models (CTMs) currently in air quality assessments in Europe: CAMx, CHIMERE, CMAQ, EMEP/MSC-W, LOTOS-EUROS, MINNI and RCGC. The simulations were carried out in the framework of the EURODELTA III modelling exercise and were evaluated against field measurements from intensive campaigns of European Monitoring and Evaluation Programme (EMEP) and the European Integrated Project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI). Model simulations were performed over the same domain, using as much as possible the same input data and covering four seasons: summer (1–30 June 2006), winter (8 January – 4 February 2007), autumn (17 September- 15 October 2008) and spring (25 February - 26 March 2009). The analyses of models’ performances in prediction of elemental carbon (EC) for the four seasons and organic aerosol components (OA) for the last two seasons show that all models generally underestimate the measured concentrations. The maximum underestimation of EC is about 60% and up to about 80% for total organic matter (TOM). The underestimation of TOM outside of highly polluted area is a consequence of an underestimation of secondary organic aerosol (SOA), in particular of its main contributor: biogenic secondary aerosol (BSOA). This result is independent on the SOA modelling approach used and season. The concentrations and daily cycles of total primary organic matter (TPOM) are generally better reproduced by the models since they used the same anthropogenic emissions. However, the combination of emissions and model formulation leads to overestimate TPOM concentrations in 2009 for most of the models. All models capture relatively well the SOA daily cycles at rural stations mainly due to the spatial resolution used in the simulations. For the investigated carbonaceous aerosol compounds, the differences between the concentrations simulated by different models are lower than the differences between the concentrations simulated with a model for different seasons. © 2019 The Authors