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- 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.
- 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.
- ItemEstimation of dust related ice nucleating particles in the atmosphere: Comparison of profiling and in-situ measurements(Les Ulis : EDP Sciences, 2019) Haarig, Moritz; Ansmann, Albert; Walser, Adrian; Baars, Holger; Urbanneck, Claudia; Weinzierl, Bernadett; Schöberl, Manuel; Dollner, Maximilian; Mamouri, Rodanthi; Althausen, DietrichVertical profiles of number concentrations of dust particles relevant for ice nucleation in clouds are derived from lidar measurements. The results are compared to coincidental airborne in-situ measurements of particle number and surface area concentrations in the dust layer. The observations were performed in long-range transported Saharan dust at Barbados and Asian dust at Cyprus. The Asian dust data analysis is ongoing. A comparison of Asian and Saharan dust will be given at the conference. Concentrations of ice nucleating particles in the order of 10 to 1000 per cm-3 in the dust layer are derived for a temperature of-25°C at Barbados. The method can be used to continuously monitor the concentration of ice nucleating dust particles vertically resolved from lidar measurements. © 2019 The Authors, published by EDP Sciences.
- 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.
- ItemProfiles of cloud condensation nuclei, dust mass concentration, and ice-nucleating-particle-relevant aerosol properties in the Saharan Air Layer over Barbados from polarization lidar and airborne in situ measurements(Katlenburg-Lindau : EGU, 2019) Haarig, Moritz; Walser, Adrian; Ansmann, Albert; Dollner, Maximilian; Althausen, Dietrich; Sauer, Daniel; Farrell, David; Weinzierl, BernadettThe present study aims to evaluate lidar retrievals of cloud-relevant aerosol properties by using polarization lidar and coincident airborne in situ measurements in the Saharan Air Layer (SAL) over the Barbados region. Vertical profiles of the number concentration of cloud condensation nuclei (CCN), large particles (diameter d > 500 nm), surface area, mass, and ice-nucleating particle (INP) concentration are derived from the lidar measurements and compared with CCN concentrations and the INP-relevant aerosol properties measured in situ with aircraft. The measurements were performed in the framework of the Saharan Aerosol Longrange Transport and Aerosol-Cloud-Interaction Experiment (SALTRACE) in summer 2013. The CCN number concentrations derived from lidar observations were up to a factor of 2 higher than the ones measured in situ aboard the research aircraft Falcon. Possible reasons for the difference are discussed. The number concentration of particles with a dry radius of more than 250 nm and the surface-area concentration obtained from the lidar observations and used as input for the INP parameterizations agreed well (< 30 %-50 % deviation) with the aircraft measurements. In a pronounced lofted dust layer during summer (10 July 2013), the lidar retrieval yielded 100-300 CCN per cubic centimeter at 0.2 % water supersaturation and 10-200 INPs per liter at-25?C. Excellent agreement was also obtained in the comparison of mass concentration profiles. During the SALTRACE winter campaign (March 2014), the dust layer from Africa was mixed with smoke particles which dominated the CCN number concentration. This example highlights the unique lidar potential to separate smoke and dust contributions to the CCN reservoir and thus to identify the sensitive role of smoke in trade wind cumuli developments over the tropical Atlantic during the winter season. © 2017 Georg Thieme Verlag. All rights reserved.
- ItemOptical and microphysical properties of smoke over Cape Verde inferred from multiwavelength lidar measurements(Milton Park : Taylor & Francis, 2017) Tesche, Matthias; Müller, Detlef; Gross, Silke; Ansmann, Albert; Althausen, Dietrich; Freudenthaler, Volker; Weinzierl, Bernadett; Veira, Andreas; Petzold, AndreasLidar measurements of mixed dust/smoke plumes over the tropical Atlantic ocean were carried out during the winter campaign of SAMUM-2 at Cape Verde. Profiles of backscatter and extinction coefficients, lidar ratios, and Ångstr¨om exponents related to pure biomass-burning aerosol from southern West Africa were extracted from these observations. Furthermore, these findings were used as input for an inversion algorithm to retrieve microphysical properties of pure smoke. Seven measurement days were found suitable for the procedure of aerosol-type separation and successive inversion of optical data that describe biomass-burning smoke. We inferred high smoke lidar ratios of 87 ± 17 sr at 355 nm and 79 ± 17 sr at 532 nm. Smoke lidar ratios and Ångstr¨om exponents are higher compared to the ones for the dust/smoke mixture. These numbers indicate higher absorption and smaller sizes for pure smoke particles compared to the dust/smoke mixture. Inversion of the smoke data set results in mean effective radii of 0.22 ± 0.08 μm with individual results varying between 0.10 and 0.36 μm. The single-scattering albedo for pure biomass-burning smoke was found to vary between 0.63 and 0.89 with a very low mean value of 0.75 ± 0.07. This is in good agreement with findings of airborne in situ measurements which showed values of 0.77 ± 0.03. Effective radii from the inversion were similar to the ones found for the fine mode of the in situ size distributions.
- ItemThermal IR radiative properties of mixed mineral dust and biomass aerosol during SAMUM-2(Milton Park : Taylor & Francis, 2011) Köhler, Claas H.; Trautmann, Thomas; Lindermeir, Erwin; Vreeling, Willem; Lieke, Kirsten; Kandler, Konrad; Weinzierl, Bernadett; Groß, Silke; Tesche, Matthias; Wendisch, ManfredGround-based high spectral resolution measurements of downwelling radiances from 800 to 1200 cm−1 were conducted between 20 January and 6 February 2008 within the scope of the SAMUM-2 field experiment. We infer the spectral signature of mixed biomass burning/mineral dust aerosols at the surface from these measurements and at top of the atmosphere from IASI observations. In a case study for a day characterized by the presence of high loads of both dust and biomass we attempt a closure with radiative transfer simulations assuming spherical particles. A detailed sensitivity analysis is performed to investigate the effect of uncertainties in the measurements ingested into the simulation on the simulated radiances. Distinct deviations between modelled and observed radiances are limited to a spectral region characterized by resonance bands in the refractive index. A comparison with results obtained during recent laboratory studies and field experiments reveals, that the deviations could be caused by the aerosol particles’ non-sphericity, although an unequivocal discrimination from measurement uncertainties is not possible. Based on radiative transfer simulations we estimate the aerosol’s direct radiative effect in the atmospheric window region to be 8 W m−2 at the surface and 1 W m−2 at top of the atmosphere.