20 results
Search Results
Now showing 1 - 10 of 20
- ItemNew particle formation and sub-10nm size distribution measurements during the A-LIFE field experiment in Paphos, Cyprus(Katlenburg-Lindau : EGU, 2020) Brilke, Sophia; Fölker, Nikolaus; Kandler, Konrad; Müller, Thomas; Gong, Xianda; Peischl, Jeff; Weinzierl, Bernadett; Winkler, Paul M.Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMAtrain) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 μ m was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMAtrain, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (< 10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements. © 2020 Author(s).
- ItemMeasurement report: Balloon-borne in situ profiling of Saharan dust over Cyprus with the UCASS optical particle counter(Katlenburg-Lindau : European Geosciences Union, 2021) Kezoudi, Maria; Tesche, Matthias; Smith, Helen; Tsekeri, Alexandra; Baars, Holger; Dollner, Maximilian; Estellés, Víctor; Bühl, Johannes; Weinzierl, Bernadett; Ulanowski, Zbigniew; Müller, Detlef; Amiridis, VassilisThis paper presents measurements of mineral dust concentration in the diameter range from 0.4 to 14.0 µm with a novel balloon-borne optical particle counter, the Universal Cloud and Aerosol Sounding System (UCASS). The balloon launches were coordinated with ground-based active and passive remote-sensing observations and airborne in situ measurements with a research aircraft during a Saharan dust outbreak over Cyprus from 20 to 23 April 2017. The aerosol optical depth at 500 nm reached values up to 0.5 during that event over Cyprus, and particle number concentrations were as high as 50 cm−3 for the diameter range between 0.8 and 13.9 µm. Comparisons of the total particle number concentration and the particle size distribution from two cases of balloon-borne measurements with aircraft observations show reasonable agreement in magnitude and shape despite slight mismatches in time and space. While column-integrated size distributions from balloon-borne measurements and ground-based remote sensing show similar coarse-mode peak concentrations and diameters, they illustrate the ambiguity related to the missing vertical information in passive sun photometer observations. Extinction coefficient inferred from the balloon-borne measurements agrees with those derived from coinciding Raman lidar observations at height levels with particle number concentrations smaller than 10 cm−3 for the diameter range from 0.8 to 13.9 µm. An overestimation of the UCASS-derived extinction coefficient of a factor of 2 compared to the lidar measurement was found for layers with particle number concentrations that exceed 25 cm−3, i.e. in the centre of the dust plume where particle concentrations were highest. This is likely the result of a variation in the refractive index and the shape and size dependency of the extinction efficiency of dust particles along the UCASS measurements. In the future, profile measurements of the particle number concentration and particle size distribution with the UCASS could provide a valuable addition to the measurement capabilities generally used in field experiments that are focussed on the observation of coarse aerosols and clouds.
- ItemAircraft-based observations of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) in the tropical upper troposphere over the Amazon region(Katlenburg-Lindau : EGU, 2018) Schulz, Christiane; Schneider, Johannes; Amorim Holanda, Bruna; Appel, Oliver; Costa, Anja; de Sá, Suzane S.; Dreiling, Volker; Fütterer, Daniel; Jurkat-Witschas, Tina; Klimach, Thomas; Knote, Christoph; Krämer, Martina; Martin, Scot T.; Mertes, Stephan; Pöhlker, Mira L.; Sauer, Daniel; Voigt, Christiane; Walser, Adrian; Weinzierl, Bernadett; Ziereis, Helmut; Zöger, Martin; Andreae, Meinrat O.; Artaxo, Paulo; Machado, Luiz A. T.; Pöschl, Ulrich; Wendisch, Manfred; Borrmann, StephanDuring the ACRIDICON-CHUVA field project (September-October 2014; based in Manaus, Brazil) aircraft-based in situ measurements of aerosol chemical composition were conducted in the tropical troposphere over the Amazon using the High Altitude and Long Range Research Aircraft (HALO), covering altitudes from the boundary layer (BL) height up to 14.4km. The submicron non-refractory aerosol was characterized by flash-vaporization/electron impact-ionization aerosol particle mass spectrometry. The results show that significant secondary organic aerosol (SOA) formation by isoprene oxidation products occurs in the upper troposphere (UT), leading to increased organic aerosol mass concentrations above 10km altitude. The median organic mass concentrations in the UT above 10km range between 1.0 and 2.5μgm-3 (referring to standard temperature and pressure; STP) with interquartile ranges of 0.6 to 3.2μgm-3 (STP), representing 78% of the total submicron non-refractory aerosol particle mass. The presence of isoprene-epoxydiol-derived secondary organic aerosol (IEPOX-SOA) was confirmed by marker peaks in the mass spectra. We estimate the contribution of IEPOX-SOA to the total organic aerosol in the UT to be about 20%. After isoprene emission from vegetation, oxidation processes occur at low altitudes and/or during transport to higher altitudes, which may lead to the formation of IEPOX (one oxidation product of isoprene). Reactive uptake or condensation of IEPOX on preexisting particles leads to IEPOX-SOA formation and subsequently increasing organic mass in the UT. This organic mass increase was accompanied by an increase in the nitrate mass concentrations, most likely due to NOx production by lightning. Analysis of the ion ratio of NO+ to NO2+ indicated that nitrate in the UT exists mainly in the form of organic nitrate. IEPOX-SOA and organic nitrates are coincident with each other, indicating that IEPOX-SOA forms in the UT either on acidic nitrate particles forming organic nitrates derived from IEPOX or on already neutralized organic nitrate aerosol particles.
- ItemThe importance of the representation of air pollution emissions for the modeled distribution and radiative effects of black carbon in the Arctic(Katlenburg-Lindau : EGU, 2019) Schacht, Jacob; Heinold, Bernd; Quaas, Johannes; Backman, John; Cherian, Ribu; Ehrlich, Andre; Herber, Andreas; Huang, Wan Ting Katty; Kondo, Yutaka; Massling, Andreas; Sinha, P.R.; Weinzierl, Bernadett; Zanatta, Marco; Tegen, InaAerosol particles can contribute to the Arctic amplification (AA) by direct and indirect radiative effects. Specifically, black carbon (BC) in the atmosphere, and when deposited on snow and sea ice, has a positive warming effect on the top-of-atmosphere (TOA) radiation balance during the polar day. Current climate models, however, are still struggling to reproduce Arctic aerosol conditions.We present an evaluation study with the global aerosol-climate model ECHAM6.3-HAM2.3 to examine emission-related uncertainties in the BC distribution and the direct radiative effect of BC. The model results are comprehensively compared against the latest ground and airborne aerosol observations for the period 2005-2017, with a focus on BC. Four different setups of air pollution emissions are tested. The simulations in general match well with the observed amount and temporal variability in near-surface BC in the Arctic. Using actual daily instead of fixed biomass burning emissions is crucial for reproducing individual pollution events but has only a small influence on the seasonal cycle of BC. Compared with commonly used fixed anthropogenic emissions for the year 2000, an up-to-date inventory with transient air pollution emissions results in up to a 30% higher annual BC burden locally. This causes a higher annual mean all-sky net direct radiative effect of BC of over 0.1Wm-2 at the top of the atmosphere over the Arctic region (60-90° N), being locally more than 0.2Wm-2 over the eastern Arctic Ocean. We estimate BC in the Arctic as leading to an annual net gain of 0.5Wm-2 averaged over the Arctic region but to a local gain of up to 0.8Wm-2 by the direct radiative effect of atmospheric BC plus the effect by the BC-in-snow albedo reduction. Long-range transport is identified as one of the main sources of uncertainties for ECHAM6.3-HAM2.3, leading to an overestimation of BC in atmospheric layers above 500 hPa, especially in summer. This is related to a misrepresentation in wet removal in one identified case at least, which was observed during the ARCTAS (Arctic Research of the Composition of the Troposphere from Aircraft and Satellites) summer aircraft campaign. Overall, the current model version has significantly improved since previous intercomparison studies and now performs better than the multi-model average in the Aerosol Comparisons between Observation and Models (AEROCOM) initiative in terms of the spatial and temporal distribution of Arctic BC. © 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).
- ItemAerosol characteristics and particle production in the upper troposphere over the Amazon Basin(Katlenburg-Lindau : EGU, 2018) Andreae, Meinrat O.; Afchine, Armin; Albrecht, Rachel; Holanda, Bruna Amorim; Artaxo, Paulo; Barbosa, Henrique M. J.; Borrmann, Stephan; Cecchini, Micael A.; Costa, Anja; Dollner, Maximilian; Fütterer, Daniel; Järvinen, Emma; Jurkat, Tina; Klimach, Thomas; Konemann, Tobias; Knote, Christoph; Krämer, Martina; Krisna, Trismono; Machado, Luiz A. T.; Mertes, Stephan; Minikin, Andreas; Pöhlker, Christopher; Pöhlker, Mira L.; Pöschl, Ulrich; Rosenfeld, Daniel; Sauer, Daniel; Schlager, Hans; Schnaiter, Martin; Schneider, Johannes; Schulz, Christiane; Spanu, Antonio; Sperling, Vinicius B.; Voigt, Christiane; Walser, Adrian; Wang, Jian; Weinzierl, Bernadett; Wendisch, Manfred; Ziereis, HelmutAirborne observations over the Amazon Basin showed high aerosol particle concentrations in the upper troposphere (UT) between 8 and 15ĝ€km altitude, with number densities (normalized to standard temperature and pressure) often exceeding those in the planetary boundary layer (PBL) by 1 or 2 orders of magnitude. The measurements were made during the German–Brazilian cooperative aircraft campaign ACRIDICON–CHUVA, where ACRIDICON stands for
Aerosol, Cloud, Precipitation, and Radiation Interactions and Dynamics of Convective Cloud Systems
and CHUVA is the acronym forCloud Processes of the Main Precipitation Systems in Brazil: A Contribution to Cloud Resolving Modeling and to the GPM (global precipitation measurement)
, on the German High Altitude and Long Range Research Aircraft (HALO). The campaign took place in September–October 2014, with the objective of studying tropical deep convective clouds over the Amazon rainforest and their interactions with atmospheric trace gases, aerosol particles, and atmospheric radiation.
Aerosol enhancements were observed consistently on all flights during which the UT was probed, using several aerosol metrics, including condensation nuclei (CN) and cloud condensation nuclei (CCN) number concentrations and chemical species mass concentrations. The UT particles differed sharply in their chemical composition and size distribution from those in the PBL, ruling out convective transport of combustion-derived particles from the boundary layer (BL) as a source. The air in the immediate outflow of deep convective clouds was depleted of aerosol particles, whereas strongly enhanced number concentrations of small particles (< 90ĝ€nm diameter) were found in UT regions that had experienced outflow from deep convection in the preceding 5–72ĝ€h. We also found elevated concentrations of larger (> 90ĝ€nm) particles in the UT, which consisted mostly of organic matter and nitrate and were very effective CCN.
Our findings suggest a conceptual model, where production of new aerosol particles takes place in the continental UT from biogenic volatile organic material brought up by deep convection and converted to condensable species in the UT. Subsequently, downward mixing and transport of upper tropospheric aerosol can be a source of particles to the PBL, where they increase in size by the condensation of biogenic volatile organic compound (BVOC) oxidation products. This may be an important source of aerosol particles for the Amazonian PBL, where aerosol nucleation and new particle formation have not been observed. We propose that this may have been the dominant process supplying secondary aerosol particles in the pristine atmosphere, making clouds the dominant control of both removal and production of atmospheric particles. - 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.
- ItemDetrainment Dominates CCN Concentrations Around Non-Precipitating Convective Clouds Over the Amazon(Hoboken, NJ : Wiley, 2022) Braga, Ramon C.; Rosenfeld, Daniel; Andreae, Meinrat O.; Pöhlker, Christopher; Pöschl, Ulrich; Voigt, Christiane; Weinzierl, Bernadett; Wendisch, Manfred; Pöhlker, Mira L.; Harrison, DanielWe investigated the relationship between the number concentration of cloud droplets (Nd) in ice-free convective clouds and of particles large enough to act as cloud condensation nuclei (CCN) measured at the lateral boundaries of cloud elements. The data were collected during the ACRIDICON-CHUVA aircraft campaign over the Amazon Basin. The results indicate that the CCN particles at the lateral cloud boundaries are dominated by detrainment from the cloud. The CCN concentrations detrained from non-precipitating convective clouds are smaller compared to below cloud bases. The detrained CCN particles from precipitating cloud volumes have relatively larger sizes, but lower concentrations. Our findings indicate that CCN particles ingested from below cloud bases are activated into cloud droplets, which evaporate at the lateral boundaries and above cloud base and release the CCN again to ambient cloud-free air, after some cloud processing. These results support the hypothesis that the CCN around the cloud are cloud-processed.
- ItemVertical wind retrieved by airborne lidar and analysis of island induced gravity waves in combination with numerical models and in situ particle measurements(München : European Geopyhsical Union, 2016) Chouza, Fernando; Reitebuch, Oliver; Jähn, Michael; Rahm, Stephan; Weinzierl, BernadettThis study presents the analysis of island induced gravity waves observed by an airborne Doppler wind lidar (DWL) during SALTRACE. First, the instrumental corrections required for the retrieval of high spatial resolution vertical wind measurements from an airborne DWL are presented and the measurement accuracy estimated by means of two different methods. The estimated systematic error is below −0.05 m s−1 for the selected case of study, while the random error lies between 0.1 and 0.16 m s−1 depending on the estimation method. Then, the presented method is applied to two measurement flights during which the presence of island induced gravity waves was detected. The first case corresponds to a research flight conducted on 17 June 2013 in the Cabo Verde islands region, while the second case corresponds to a measurement flight on 26 June 2013 in the Barbados region. The presence of trapped lee waves predicted by the calculated Scorer parameter profiles was confirmed by the lidar and in situ observations. The DWL measurements are used in combination with in situ wind and particle number density measurements, large-eddy simulations (LES), and wavelet analysis to determine the main characteristics of the observed island induced trapped waves.
- ItemParticle settling and vertical mixing in the Saharan Air Layer as seen from an integrated model, lidar, and in situ perspective(München : European Geopyhsical Union, 2017) Gasteiger, Josef; Groß, Silke; Sauer, Daniel; Haarig, Moritz; Ansmann, Albert; Weinzierl, BernadettLong-range transport of aerosol in the Saharan Air Layer (SAL) across the Atlantic plays an important role for weather, climate, and ocean fertilization. However, processes occurring within the SAL and their effects on aerosol properties are still unclear. In this work we study particle settling and vertical mixing within the SAL based on measured and modeled vertical aerosol profiles in the upper 1 km of the transported SAL. We use ground-based lidar measurements and airborne particle counter measurements over the western Atlantic, collected during the SALTRACE campaign, as well as space-based CALIOP lidar measurements from Africa to the western Atlantic in the summer season. In our model we take account of the optical properties and the Stokes gravitational settling of irregularly shaped Saharan dust particles. We test two hypotheses about the occurrence of vertical mixing within the SAL over the Atlantic to explain the aerosol profiles observed by the lidars and the particle counter. Our first hypothesis (H1) assumes that no mixing occurs in the SAL leading to a settling-induced separation of particle sizes. The second hypothesis (H2) assumes that vertical mixing occurs in the SAL allowing large super-micron dust particles to stay airborne longer than without mixing. The uncertainties of the particle linear depolarization ratio (δl) profiles measured by the ground-based lidars are comparable to the modeled differences between H1 and H2 and do not allow us to conclude which hypothesis fits better. The SALTRACE in situ data on size-resolved particle number concentrations show a presence of large particles near the SAL top that is inconsistent with H1. The analysis of the CALIOP measurements also reveals that the average δl profile over the western Atlantic is inconsistent with H1. Furthermore, it was found that the average δl profile in the upper 1 km of the SAL does not change along its transport path over the Atlantic. These findings give evidence that vertical mixing within the SAL is a common phenomenon with significant consequences for the evolution of the size distribution of super-micron dust particles during transport over the Atlantic. Further research is needed to precisely characterize the processes that are relevant for this phenomenon.