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    Intercomparison 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, Alfred
    Aerodynamic 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.
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    Importance 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, Thomas
    Black 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.
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    Biomass 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, Paolo
    This 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.
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    An optical particle size spectrometer for aircraft-borne measurements in IAGOS-CARIBIC
    (München : European Geopyhsical Union, 2016) Hermann, Markus; Weigelt, Andreas; Assmann, Denise; Pfeifer, Sascha; Müller, Thomas; Conrath, Thomas; Voigtländer, Jens; Heintzenberg, Jost; Wiedensohler, Alfred; Martinsson, Bengt G.; Deshler, Terry; Brenninkmeijer, Carl A.M.; Zahn, Andreas
    The particle number size distribution is an important parameter to characterize the atmospheric aerosol and its influence on the Earth's climate. Here we describe a new optical particle size spectrometer (OPSS) for measurements of the accumulation mode particle number size distribution in the tropopause region on board a passenger aircraft (IAGOS-CARIBIC observatory: In-service Aircraft for a Global Observing System – Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container). A modified KS93 particle sensor from RION Co., Ltd., together with a new airflow system and a dedicated data acquisition system, is the key component of the CARIBIC OPSS. The instrument records individual particle pulse signal curves in the particle size range 130–1110 nm diameter (for a particle refractive index of 1.47-i0.006) together with a time stamp and thus allows the post-flight choice of the time resolution and the size distribution bin width. The CARIBIC OPSS has a 50 % particle detection diameter of 152 nm and a maximum asymptotic counting efficiency of 98 %. The instrument's measurement performance shows no pressure dependency and no particle coincidence for free tropospheric conditions. The size response function of the CARIBIC OPSS was obtained by a polystyrene latex calibration in combination with model calculations. Particle number size distributions measured with the new OPSS in the lowermost stratosphere agreed within a factor of 2 in concentration with balloon-borne measurements over western North America. Since June 2010 the CARIBIC OPSS is deployed once per month in the IAGOS-CARIBIC observatory.
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    The effect of rapid relative humidity changes on fast filter-based aerosol-particle light-absorption measurements: Uncertainties and correction schemes
    (Katlenburg-Lindau : Copernicus, 2019) Düsing, Sebastian; Wehner, Birgit; Müller, Thomas; Stöcker, Almond; Wiedensohler, Alfred
    Measuring vertical profiles of the particle light-absorption coefficient by using absorption photometers may face the challenge of fast changes in relative humidity (RH). These absorption photometers determine the particle light-absorption coefficient due to a change in light attenuation through a particle-loaded filter. The filter material, however, takes up or releases water with changing relative humidity (RH in %), thus influencing the light attenuation. A sophisticated set of laboratory experiments was therefore conducted to investigate the effect of fast RH changes (dRH/dt) on the particle light-absorption coefficient (σabs in Mm-1) derived with two absorption photometers. The RH dependence was examined based on different filter types and filter loadings with respect to loading material and areal loading density. The Single Channel Tricolor Absorption Photometer (STAP) relies on quartz-fiber filter, and the microAeth® MA200 is based on a polytetrafluoroethylene (PTFE) filter band. Furthermore, three cases were investigated: clean filters, filters loaded with black carbon (BC), and filters loaded with ammonium sulfate. The filter areal loading densities (ρ∗) ranged from 3.1 to 99.6 mg m-2 in the case of the STAP and ammonium sulfate and 1.2 to 37.6 mg m-2 in the case the MA200. Investigating BC-loaded cases, M8 scroll mrow miBCm 15pt was in the range of 2.9 to 43.0 and 1.1 to 16.3 mg m-2 for the STAP and MA200, respectively.

    Both instruments revealed opposing responses to relative humidity changes ("RH) with different magnitudes. The STAP shows a linear dependence on relative humidity changes. The MA200 is characterized by a distinct exponential recovery after its filter was exposed to relative humidity changes. At a wavelength of 624 nm and for the default 60 s running average output, the STAP reveals an absolute change in σabs per absolute change of RH ("σabsĝ•"RH) of 0.14 Mm-1 %-1 in the clean case, 0.29 Mm-1 %-1 in the case of BC-loaded filters, and 0.21 Mm-1 %-1 in the case filters loaded with ammonium sulfate. The 60 s running average of the particle light-absorption coefficient at 625 nm measured with the MA200 revealed a response of around -0.4 Mm-1 %-1 for all three cases. Whereas the response of the STAP varies over the different loading materials, in contrast, the MA200 was quite stable. The response was, for the STAP, in the range of 0.17 to 0.24 Mm-1 %-1 and, in the case of ammonium sulfate loading and in the BC-loaded case, 0.17 to 0.62 Mm-1 %-1. In the ammonium sulfate case, the minimum response shown by the MA200 was -0.42 with a maximum of -0.36 Mm-1 %-1 and a minimum of -0.42 and maximum -0.37 Mm-1 %-1 in the case of BC.

    A linear correction function for the STAP was developed here. It is provided by correlating 1 Hz resolved recalculated particle light-absorption coefficients and RH change rates. The linear response is estimated at 10.08 Mm-1 s-1 %-1. A correction approach for the MA200 is also provided; however, the behavior of the MA200 is more complex. Further research and multi-instrument measurements have to be conducted to fully understand the underlying processes, since the correction approach resulted in different correction parameters across various experiments. However, the exponential recovery after the filter of the MA200 experienced a RH change could be reproduced. However, the given correction approach has to be estimated with other RH sensors as well, since each sensor has a different response time. And, for the given correction approaches, the uncertainties could not be estimated, which was mainly due to the response time of the RH sensor. Therefore, we do not recommend using the given approaches. But they point in the right direction, and despite the imperfections, they are useful for at least estimating the measurement uncertainties due to relative humidity changes.

    Due to our findings, we recommend using an aerosol dryer upstream of absorption photometers to reduce the RH effect significantly. Furthermore, when absorption photometers are used in vertical measurements, the ascending or descending speed through layers of large relative humidity gradients has to be low to minimize the observed RH effect. But this is simply not possible in some scenarios, especially in unmixed layers or clouds. Additionally, recording the RH of the sample stream allows correcting for the bias during post-processing of the data. This data correction leads to reasonable results, according to the given example in this study. © Author(s) 2019.

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    Decreasing trends of particle number and black carbon mass concentrations at 16 observational sites in Germany from 2009 to 2018
    (Katlenburg-Lindau : EGU, 2020) Sun, Jia; Birmili, Wolfram; Hermann, Markus; Tuch, Thomas; Weinhold, Kay; Merkel, Maik; Rasch, Fabian; Müller, Thomas; Schladitz, Alexander; Bastian, Susanne; Löschau, Gunter; Cyrys, Josef; Gu, Jianwei; Flentje, Harald; Briel, Björn; Asbach, Christoph; Kaminski, Heinz; Ries, Ludwig; Sohmer, Ralf; Gerwig, Holger; Wirtz, Klaus; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ma, Nan; Wiedensohler, Alfred
    Anthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009-2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between-13.1% and-1.7% per year. The slopes of the PNCs vary from-17.2% to-1.7 %,-7.8% to-1.1 %, and-11.1% to-1.2% per year for 10-30, 30-200, and 200-800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies. © 2020 Author(s).
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    In 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, Alfred
    Particle 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.
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    In 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, Alfred
    An 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.