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- ItemVertically resolved dust optical properties during SAMUM: Tinfou compared to Ouarzazate(Milton Park : Taylor & Francis, 2017) Heese, Birgit; Althausen, Dietrich; Dinter, Tilman; Esselborn, Michael; Müller, Thomas; Tesche, Matthias; Wiegner, MatthiasVertical profiles of dust key optical properties are presented from measurements during the Saharan Mineral Dust Experiment (SAMUM) by Raman and depolarization lidar at two ground-based sites and by airborne high spectral resolution lidar. One of the sites, Tinfou, is located close to the border of the Sahara in Southern Morocco and was the main in situ site during SAMUM. The other site was Ouarzazate airport, the main lidar site. From the lidar measurements the spatial distribution of the dust between Tinfou and Ouarzazate was derived for 1 d. The retrieved profiles of backscatter and extinction coefficients and particle depolarization ratios show comparable dust optical properties, a similar vertical structure of the dust layer, and a height of about 4 km asl at both sites. The airborne cross-section of the extinction coefficient at the two sites confirms the low variability in dust properties. Although the general picture of the dust layer was similar, the lidar measurements reveal a higher dust load closer to the dust source. Nevertheless, the observed intensive optical properties were the same. These results indicate that the lidar measurements at two sites close to the dust source are both representative for the SAMUM dust conditions.
- ItemSaharan Mineral Dust Experiments SAMUM-1 and SAMUM-2: What have we learned?(Milton Park : Taylor & Francis, 2011) Ansmann, Albert; Petzold, Andreas; Kandler, Konrad; Tegen, Ina; Wendisch, Manfred; Müller, Detlef; Weinzierl, Bernadett; Müller, Thomas; Heintzenberg, JostTwo comprehensive field campaigns were conducted in 2006 and 2008 in the framework of the Saharan Mineral Dust Experiment (SAMUM) project. The relationship between chemical composition, shape morphology, size distribution and optical effects of the dust particles was investigated. The impact of Saharan dust on radiative transfer and the feedback of radiative effects upon dust emission and aerosol transport were studied. Field observations (ground-based, airborne and remote sensing) and modelling results were compared within a variety of dust closure experiments with a strong focus on vertical profiling. For the first time, multiwavelength Raman/polarization lidars and an airborne high spectral resolution lidar were involved in major dust field campaigns and provided profiles of the volume extinction coefficient of the particles at ambient conditions (for the full dust size distribution), of particle-shape-sensitive optical properties at several wavelengths, and a clear separation of dust and smoke profiles allowing for an estimation of the single-scattering albedo of the biomass-burning aerosol. SAMUM–1 took place in southern Morocco close to the Saharan desert in the summer of 2006, whereas SAMUM–2 was conducted in Cape Verde in the outflow region of desert dust and biomass-burning smoke from western Africa in the winter of 2008. This paper gives an overview of the SAMUM concept, strategy and goals, provides snapshots (highlights) of SAMUM–2 observations and modelling efforts, summarizes main findings of SAMUM–1 and SAMUM–2 and finally presents a list of remaining problems and unsolved questions.
- ItemIn situ aerosol characterization at Cape Verde, Part 1: Particle number size distributions, hygroscopic growth and state of mixing of the marine and Saharan dust aerosol(Milton Park : Taylor & Francis, 2017) Schladitz, Alexander; Müller, Thomas; Nowak, Andreas; Kandler, Konrad; Lieke, Kirsten; Massling, Andreas; Wiedensohler, AlfredParticle number size distributions and hygroscopic properties of marine and Saharan dust aerosol were investigated during the SAMUM-2 field study at Cape Verde in winter 2008. Aitken and accumulation mode particles were mainly assigned to the marine aerosol, whereas coarse mode particles were composed of sea-salt and a variable fraction of Saharan mineral dust. A new methodical approach was used to derive hygroscopic growth and state of mixing for a particle size range (volume equivalent) from dpve = 26 nm to 10 μm. For hygroscopic particles with dpve < 100 nm, the median hygroscopicity parameter κ is 0.35. From 100 nm < dpve < 350 nm, κ increases to 0.65. For larger particles, κ at dpve = 350 nm was used. For nearly hydrophobic particles, κ is between 0 and 0.1 for dpve < 250 nm and decreases to 0 for dpve > 250 nm. The mixing state of Saharan dust in terms of the number fraction of nearly hydrophobic particles showed the highest variation and ranges from 0.3 to almost 1. This study was used to perform a successful mass closure at ambient conditions and demonstrates the important role of hygroscopic growth of large sea-salt particles.
- ItemIn situ aerosol characterization at Cape Verde, Part 2: Parametrization of relative humidity- and wavelength-dependent aerosol optical properties(Milton Park : Taylor & Francis, 2017) Schladitz, Alexander; Müller, Thomas; Nordmann, Stephan; Tesche, Matthias; Silke Groß, Silke Groß; Freudenthaler, Volker; Gasteiger, Josef; Wiedensohler, AlfredAn observation-based numerical study of humidity-dependent aerosol optical properties of mixed marine and Saharan mineral dust aerosol is presented. An aerosol model was developed based on measured optical and microphysical properties to describe the marine and Saharan dust aerosol at Cape Verde. A wavelength-dependent optical equivalent imaginary part of the refractive index and a scattering non-sphericity factor for Saharan dustwere derived. Simulations of humidity effects on optical properties by the aerosol model were validated with relative measurements of the extinction coefficient at ambient conditions. Parametrizations were derived to describe the humidity dependence of the extinction, scattering, and absorption coefficients as well as the asymmetry parameter and single scattering albedo. For wavelengths (300–950 nm) and dry dust volume fractions (0–1), aerosol optical properties as a function of relative humidity (RH = 0–90%) can be calculated from tabulated parameters. For instance, at a wavelength of 550 nm, a volume fraction of 0.5 of dust on the total particle volume (dry conditions) and a RH of 90%, the enhancements for the scattering, extinction and absorption coefficients are 2.55, 2.46 and 1.04, respectively, while the enhancements for the asymmetry parameter and single scattering albedo are 1.11 and 1.04.
- ItemCAMP: An instrumented platform for balloon-borne aerosol particle studies in the lower atmosphere(Katlenburg-Lindau : Copernicus, 2022) Pilz, Christian; Düsing, Sebastian; Wehner, Birgit; Müller, Thomas; Siebert, Holger; Voigtländer, Jens; Lonardi, MichaelAirborne observations of vertical aerosol particle distributions are crucial for detailed process studies and model improvements. Tethered balloon systems represent a less expensive alternative to aircraft to probe shallow atmospheric boundary layers (ABLs). This study presents the newly developed cubic aerosol measurement platform (CAMP) for balloon-borne observations of aerosol particle microphysical properties. With an edge length of 35 cm and a weight of 9 kg, the cube is an environmentally robust instrument platform intended for measurements at low temperatures, with a particular focus on applications in cloudy Arctic ABLs. The aerosol instrumentation on board CAMP comprises two condensation particle counters with different lower detection limits, one optical particle size spectrometer, and a miniaturized absorption photometer. Comprehensive calibrations and characterizations of the instruments were performed in laboratory experiments. The first field study with a tethered balloon system took place at the Leibniz Institute for Tropospheric Research (TROPOS) station in Melpitz, Germany, in the winter of 2019. At ambient temperatures between-8 and 15 C, the platform was operated up to a 1.5 km height on 14 flights under both clear-sky and cloudy conditions. The continuous aerosol observations at the ground station served as a reference for evaluating the CAMP measurements. Exemplary profiles are discussed to elucidate the performance of the system and possible process studies. Based on the laboratory instrument characterizations and the observations during the field campaign, CAMP demonstrated the capability to provide comprehensive aerosol particle measurements in cold and cloudy ABLs.
- ItemAbsorption instruments inter-comparison campaign at the Arctic Pallas station(Katlenburg-Lindau : European Geosciences Union, 2021) Asmi, Eija; Backman, John; Servomaa, Henri; Virkkula, Aki; Gini, Maria I.; Eleftheriadis, Konstantinos; Müller, Thomas; Ohata, Sho; Kondo, Yutaka; Hyvärinen, AnttiAerosol light absorption was measured during a 1-month field campaign in June-July 2019 at the Pallas Global Atmospheric Watch (GAW) station in northern Finland. Very low aerosol concentrations prevailed during the campaign, which posed a challenge for the instruments' detection capabilities. The campaign provided a real-world test for different absorption measurement techniques supporting the goals of the European Metrology Programme for Innovation and Research (EMPIR) Black Carbon (BC) project in developing aerosol absorption standard and reference methods. In this study we compare the results from five filter-based absorption techniques - aethalometer models AE31 and AE33, a particle soot absorption photometer (PSAP), a multi-angle absorption photometer (MAAP), and a continuous soot monitoring system (COSMOS) - and from one indirect technique called extinction minus scattering (EMS). The ability of the filter-based techniques was shown to be adequate to measure aerosol light absorption coefficients down to around 0.01g¯Mm-1 levels when data were averaged to 1-2g¯h. The hourly averaged atmospheric absorption measured by the reference MAAP was 0.09g¯Mm-1 (at a wavelength of 637g¯nm). When data were averaged for >1g¯h, the filter-based methods agreed to around 40g¯%. COSMOS systematically measured the lowest absorption coefficient values, which was expected due to the sample pre-treatment in the COSMOS inlet. PSAP showed the best linear correlation with MAAP (slopeCombining double low line0.95, R2Combining double low line0.78), followed by AE31 (slopeCombining double low line0.93). A scattering correction applied to PSAP data improved the data accuracy despite the added noise. However, at very high scattering values the correction led to an underestimation of the absorption. The AE31 data had the highest noise and the correlation with MAAP was the lowest (R2Combining double low line0.65). Statistically the best linear correlations with MAAP were obtained for AE33 and COSMOS (R2 close to 1), but the biases at around the zero values led to slopes clearly below 1. The sample pre-treatment in the COSMOS instrument resulted in the lowest fitted slope. In contrast to the filter-based techniques, the indirect EMS method was not adequate to measure the low absorption values found at the Pallas site. The lowest absorption at which the EMS signal could be distinguished from the noise was >0.1g¯Mm-1 at 1-2g¯h averaging times. The mass absorption cross section (MAC) value measured at a range 0-0.3g¯Mm-1 was calculated using the MAAP and a single particle soot photometer (SP2), resulting in a MAC value of 16.0±5.7g¯m2g-1. Overall, our results demonstrate the challenges encountered in the aerosol absorption measurements in pristine environments and provide some useful guidelines for instrument selection and measurement practices. We highlight the need for a calibrated transfer standard for better inter-comparability of the absorption results. © Author(s) 2021.
- ItemIntercomparison of 15 aerodynamic particle size spectrometers (APS 3321): Uncertainties in particle sizing and number size distribution(München : European Geopyhsical Union, 2016) Pfeifer, Sascha; Müller, Thomas; Weinhold, Kay; Zikova, Nadezda; dos Santos, Sebastiao Martins; Marinoni, Angela; Bischof, Oliver F.; Kykal, Carsten; Ries, Ludwig; Meinhardt, Frank; Aalto, Pasi; Mihalopoulos, Nikolaos; Wiedensohler, AlfredAerodynamic particle size spectrometers are a well-established method to measure number size distributions of coarse mode particles in the atmosphere. Quality assurance is essential for atmospheric observational aerosol networks to obtain comparable results with known uncertainties. In a laboratory study within the framework of ACTRIS (Aerosols, Clouds, and Trace gases Research Infrastructure Network), 15 aerodynamic particle size spectrometers (APS model 3321, TSI Inc., St. Paul, MN, USA) were compared with a focus on flow rates, particle sizing, and the unit-to-unit variability of the particle number size distribution. Flow rate deviations were relatively small (within a few percent), while the sizing accuracy was found to be within 10 % compared to polystyrene latex (PSL) reference particles. The unit-to-unit variability in terms of the particle number size distribution during this study was within 10 % to 20 % for particles in the range of 0.9 up to 3 µm, which is acceptable for atmospheric measurements. For particles smaller than that, the variability increased up to 60 %, probably caused by differences in the counting efficiencies of individual units. Number size distribution data for particles smaller than 0.9 µm in aerodynamic diameter should only be used with caution. For particles larger than 3 µm, the unit-to-unit variability increased as well. A possible reason is an insufficient sizing accuracy in combination with a steeply sloping particle number size distribution and the increasing uncertainty due to decreasing counting. Particularly this uncertainty of the particle number size distribution must be considered if higher moments of the size distribution such as the particle volume or mass are calculated, which require the conversion of the aerodynamic diameter measured to a volume equivalent diameter. In order to perform a quantitative quality assurance, a traceable reference method for the particle number concentration in the size range 0.5–3 µm is needed.
- ItemImportance of size representation and morphology in modelling optical properties of black carbon: comparison between laboratory measurements and model simulations(Katlenburg-Lindau : Copernicus, 2022) Romshoo, Baseerat; Pöhlker, Mira; Wiedensohler, Alfred; Pfeifer, Sascha; Saturno, Jorge; Nowak, Andreas; Ciupek, Krzysztof; Quincey, Paul; Vasilatou, Konstantina; Ess, Michaela N.; Gini, Maria; Eleftheriadis, Konstantinos; Robins, Chris; Gaie-Levrel, François; Müller, ThomasBlack carbon (BC) from incomplete combustion of biomass or fossil fuels is the strongest absorbing aerosol component in the atmosphere. Optical properties of BC are essential in climate models for quantification of their impact on radiative forcing. The global climate models, however, consider BC to be spherical particles, which causes uncertainties in their optical properties. Based on this, an increasing number of model-based studies provide databases and parameterization schemes for the optical properties of BC, using more realistic fractal aggregate morphologies. In this study, the reliability of the different modelling techniques of BC was investigated by comparing them to laboratory measurements. The modelling techniques were examined for bare BC particles in the first step and for BC particles with organic material in the second step. A total of six morphological representations of BC particles were compared, three each for spherical and fractal aggregate morphologies. In general, the aggregate representation performed well for modelling the particle light absorption coefficient σabs, single-scattering albedo SSA, and mass absorption cross-section MACBC for laboratory-generated BC particles with volume mean mobility diameters dp,V larger than 100nm. However, for modelling Ångström absorption exponent AAE, it was difficult to suggest a method due to size dependence, although the spherical assumption was in better agreement in some cases. The BC fractal aggregates are usually modelled using monodispersed particles, since their optical simulations are computationally expensive. In such studies, the modelled optical properties showed a 25% uncertainty in using the monodisperse size method. It is shown that using the polydisperse size distribution in combination with fractal aggregate morphology reduces the uncertainty in measured σabs to 10% for particles with dp,V between 60-160nm. Furthermore, the sensitivities of the BC optical properties to the various model input parameters such as the real and imaginary parts of the refractive index (mre and mim), the fractal dimension (Df), and the primary particle radius (app) of an aggregate were investigated. When the BC particle is small and rather fresh, the change in the Df had relatively little effect on the optical properties. There was, however, a significant relationship between app and the particle light scattering, which increased by a factor of up to 6 with increasing total particle size. The modelled optical properties of BC are well aligned with laboratory-measured values when the following assumptions are used in the fractal aggregate representation: mre between 1.6 and 2, mim between 0.50 and 1, Df from 1.7 to 1.9, and app between 10 and 14nm. Overall, this study provides experimental support for emphasizing the importance of an appropriate size representation (polydisperse size method) and an appropriate morphological representation for optical modelling and parameterization scheme development of BC.
- ItemVariability in the mass absorption cross section of black carbon (BC) aerosols is driven by BC internal mixing state at a central European background site (Melpitz, Germany) in winter(Katlenburg-Lindau : European Geosciences Union, 2021) Yuan, Jinfeng; Modini, Robin Lewis; Zanatta, Marco; Herber, Andreas B.; Müller, Thomas; Wehner, Birgit; Poulain, Laurent; Tuch, Thomas; Baltensperger, Urs; Gysel-Beer, MartinProperties of atmospheric black carbon (BC) particles were characterized during a field experiment at a rural background site (Melpitz, Germany) in February 2017. BC absorption at a wavelength of 870 nm was measured by a photoacoustic extinctiometer, and BC physical properties (BC mass concentration, core size distribution and coating thickness) were measured by a single-particle soot photometer (SP2). Additionally, a catalytic stripper was used to intermittently remove BC coatings by alternating between ambient and thermo-denuded conditions. From these data the mass absorption cross section of BC (MACBC) and its enhancement factor (EMAC) were inferred for essentially waterfree aerosol as present after drying to low relative humidity (RH). Two methods were applied independently to investigate the coating effect on EMAC: A correlation method (MACBC; ambient vs. BC coating thickness) and a denuding method (MACBC; ambient vs. MACBC; denuded). Observed EMAC values varied from 1.0 to 1.6 (lower limit from denuding method) or 1:2 to 1.9 (higher limit from correlation method), with the mean coating volume fraction ranging from 54% to 78% in the dominating mass equivalent BC core diameter range of 200?220 nm.MACBC and EMAC were strongly correlated with coating thickness of BC. By contrast, other potential drivers of EMAC variability, such as different BC sources (air mass origin and absorption Angström exponent), coating composition (ratio of inorganics to organics) and BC core size distribution, had only minor effects. These results for ambient BC measured at Melpitz during winter show that the lensing effect caused by coatings on BC is the main driver of the variations in MACBC and EMAC, while changes in other BC particle properties such as source, BC core size or coating composition play only minor roles at this rural background site with a large fraction of aged particles. Indirect evidence suggests that potential dampening of the lensing effect due to unfavorable morphology was most likely small or even negligible.
- 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.