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- ItemExplicit modeling of volatile organic compounds partitioning in the atmospheric aqueous phase(München : European Geopyhsical Union, 2013) Mouchel-Vallon, C.; Bräuer, P.; Camredon, M.; Valorso, R.; Madronich, S.; Hermann, M.; Aumont, B.The gas phase oxidation of organic species is a multigenerational process involving a large number of secondary compounds. Most secondary organic species are water-soluble multifunctional oxygenated molecules. The fully explicit chemical mechanism GECKO-A (Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere) is used to describe the oxidation of organics in the gas phase and their mass transfer to the aqueous phase. The oxidation of three hydrocarbons of atmospheric interest (isoprene, octane and α-pinene) is investigated for various NOx conditions. The simulated oxidative trajectories are examined in a new two dimensional space defined by the mean oxidation state and the solubility. The amount of dissolved organic matter was found to be very low (yield less than 2% on carbon atom basis) under a water content typical of deliquescent aerosols. For cloud water content, 50% (isoprene oxidation) to 70% (octane oxidation) of the carbon atoms are found in the aqueous phase after the removal of the parent hydrocarbons for low NOx conditions. For high NOx conditions, this ratio is only 5% in the isoprene oxidation case, but remains large for α-pinene and octane oxidation cases (40% and 60%, respectively). Although the model does not yet include chemical reactions in the aqueous phase, much of this dissolved organic matter should be processed in cloud drops and modify both oxidation rates and the speciation of organic species.
- ItemCharacterisation of a new Fast CPC and its application for atmospheric particle measurements(München : European Geopyhsical Union, 2011) Wehner, B.; Siebert, H.; Hermann, M.; Ditas, F.; Wiedensohler, A.A new Fast CPC (FCPC) using butanol as working fluid has been built based on the setup described by Wang et al. (2002). In this study, we describe the new instrument. The functionality and stable operation of the FCPC in the laboratory, as well as under atmospheric conditions, is demonstrated. The counting efficiency was measured for three temperature differences between FCPC saturator and condenser, 25, 27, and 29 K, subsequently resulting in a lower detection limit between 6.1 and 8.5 nm. Above 25 nm the FCPC reached 98–100% counting efficiency compared to an electrometer used as the reference instrument. The FCPC demonstrated its ability to perform continuous measurements over a few hours in the laboratory with respect to the total particle counting. The instrument has been implemented into the airborne measurement platform ACTOS to perform measurements in the atmospheric boundary layer. Therefore, a stable operation over two hours is required. The mixing time of the new FCPC was estimated in two ways using a time series with highly fluctuating particle number concentrations. The analysis of a sharp ramp due to a concentration change results in a mixing time of 5 ms while a spectral analysis of atmospheric data demonstrates that for frequencies up to 10 Hz coherent structures can be resolved before sampling noise dominates.
- ItemALADINA - An unmanned research aircraft for observing vertical and horizontal distributions of ultrafine particles within the atmospheric boundary layer(München : European Geopyhsical Union, 2015) Altstädter, B.; Platis, A.; Wehner, B.; Scholtz, A.; Wildmann, N.; Hermann, M.; Käthner, R.; Baars, H.; Bange, J.; Lampert, A.This paper presents the unmanned research aircraft Carolo P360 "ALADINA" (Application of Light-weight Aircraft for Detecting IN situ Aerosol) for investigating the horizontal and vertical distribution of ultrafine particles in the atmospheric boundary layer (ABL). It has a wingspan of 3.6 m, a maximum take-off weight of 25 kg and is equipped with aerosol instrumentation and meteorological sensors. A first application of the system, together with the unmanned research aircraft MASC (Multi-Purpose Airborne Carrier) of the Eberhard Karls University of Tübingen (EKUT), is described. As small payload for ALADINA, two condensation particle counters (CPC) and one optical particle counter (OPC) were miniaturised by re-arranging the vital parts and composing them in a space-saving way in the front compartment of the airframe. The CPCs are improved concerning the lower detection threshold and the response time to less than 1.3 s. Each system was characterised in the laboratory and calibrated with test aerosols. The CPCs are operated in this study with two different lower detection threshold diameters of 11 and 18 nm. The amount of ultrafine particles, which is an indicator for new particle formation, is derived from the difference in number concentrations of the two CPCs (ΔN). Turbulence and thermodynamic structure of the boundary layer are described by measurements of fast meteorological sensors that are mounted at the aircraft nose. A first demonstration of ALADINA and a feasibility study were conducted in Melpitz near Leipzig, Germany, at the Global Atmosphere Watch (GAW) station of the Leibniz Institute for Tropospheric Research (TROPOS) on 2 days in October 2013. There, various ground-based instruments are installed for long-term atmospheric monitoring. The ground-based infrastructure provides valuable additional background information to embed the flights in the continuous atmospheric context and is used for validation of the airborne results. The development of the boundary layer, derived from backscatter signals of a portable Raman lidar POLLYXT, allows a quick overview of the current vertical structure of atmospheric particles. Ground-based aerosol number concentrations are consistent with the results from flights in heights of a few metres. In addition, a direct comparison of ALADINA aerosol data and ground-based aerosol data, sampling the air at the same location for more than 1 h, shows comparable values within the range of ± 20 %. MASC was operated simultaneously with complementary flight patterns. It is equipped with the same meteorological instruments that offer the possibility to determine turbulent fluxes. Therefore, additional information about meteorological conditions was collected in the lowest part of the atmosphere. Vertical profiles up to 1000 m in altitude indicate a high variability with distinct layers of aerosol, especially for the small particles of a few nanometres in diameter on 1 particular day. The stratification was almost neutral and two significant aerosol layers were detected with total aerosol number concentrations up to 17 000 ± 3400 cm−3 between 180 and 220 m altitude and 14 000 ± 2800 cm−3 between 550 and 650 m. Apart from those layers, the aerosol distribution was well mixed and reached the total number concentration of less than 8000 ± 1600 cm−3. During another day, the distribution of the small particles in the lowermost ABL was related to the stratification, with continuously decreasing number concentrations from 16 000 ± 3200 cm−3 to a minimum of 4000 ± 800 cm−3 at the top of the inversion at 320 m. Above this, the total number concentration was rather constant. In the region of 500 to 600 m altitude, a significant difference of both CPCs was observed. This event occurred during the boundary layer development in the morning and represents a particle burst within the ABL.
- ItemPollution events observed during CARIBIC flights in the upper troposphere between South China and the Philippines(München : European Geopyhsical Union, 2010) Lai, S.C.; Baker, A.K.; Schuck, T.J.; van Velthoven, P.; Oram, D.E.; Zahn, A.; Hermann, M.; Weigelt, A.; Slemr, F.; Brenninkmeijer, C.A.M.; Ziereis, H.A strong pollution episode in the upper troposphere between South China and the Philippines was observed during CARIBIC flights in April 2007. Five pollution events were observed, where enhancements in aerosol and trace gas concentrations including CO, CO2, CH4, non-methane hydrocarbons (NMHCs) and halocarbons were observed along the flight tracks during four sequential flights. The importance of the contribution of biomass/biofuel burning was investigated using chemical tracers, emission factor analysis, back-trajectory analysis and satellite images. The Indochinese peninsula was identified as the probable source region of biomass/biofuel burning. However, enhancements in the urban/industrial tracer C2Cl4 during the events also indicate a substantial contribution from urban anthropogenic emissions. An estimation of the contribution of fossil fuel versus biomass/biofuel to the CO enhancement was made, indicating a biomass/biofuel burning contribution of ~54 to ~92% of the observed CO enhancements. Biomass/biofuel burning was found to be the most important source category during the sampling period.
- ItemComposition and evolution of volcanic aerosol from eruptions of Kasatochi, Sarychev and Eyjafjallajökull in 2008-2010 based on CARIBIC observations(München : European Geopyhsical Union, 2013) Andersson, S.M.; Martinsson, B.G.; Friberg, J.; Brenninkmeijer, C.A.M.; Rauthe-Schöch, A.; Hermann, M.; van Velthoven, P.F.J.; Zahn, A.Large volcanic eruptions impact significantly on climate and lead to ozone depletion due to injection of particles and gases into the stratosphere where their residence times are long. In this the composition of volcanic aerosol is an important but inadequately studied factor. Samples of volcanically influenced aerosol were collected following the Kasatochi (Alaska), Sarychev (Russia) and also during the Eyjafjallajökull (Iceland) eruptions in the period 2008–2010. Sampling was conducted by the CARIBIC platform during regular flights at an altitude of 10–12 km as well as during dedicated flights through the volcanic clouds from the eruption of Eyjafjallajökull in spring 2010. Elemental concentrations of the collected aerosol were obtained by accelerator-based analysis. Aerosol from the Eyjafjallajökull volcanic clouds was identified by high concentrations of sulphur and elements pointing to crustal origin, and confirmed by trajectory analysis. Signatures of volcanic influence were also used to detect volcanic aerosol in stratospheric samples collected following the Sarychev and Kasatochi eruptions. In total it was possible to identify 17 relevant samples collected between 1 and more than 100 days following the eruptions studied. The volcanically influenced aerosol mainly consisted of ash, sulphate and included a carbonaceous component. Samples collected in the volcanic cloud from Eyjafjallajökull were dominated by the ash and sulphate component (∼45% each) while samples collected in the tropopause region and LMS mainly consisted of sulphate (50–77%) and carbon (21–43%). These fractions were increasing/decreasing with the age of the aerosol. Because of the long observation period, it was possible to analyze the evolution of the relationship between the ash and sulphate components of the volcanic aerosol. From this analysis the residence time (1/e) of sulphur dioxide in the studied volcanic cloud was estimated to be 45 ± 22 days.
- ItemCARIBIC aircraft measurements of Eyjafjallajökull volcanic clouds in April/May 2010(München : European Geopyhsical Union, 2012) Rauthe-Schöch, A.; Weigelt, A.; Hermann, M.; Martinsson, B.G.; Baker, A.K.; Heue, K.-P.; Brenninkmeijer, C.A.M.; Zahn, A.; Scharffe, D.; Eckhardt, S.; Stohl, A.; van Velthoven, P.F.J.The Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) project investigates physical and chemical processes in the Earth's atmosphere using a Lufthansa Airbus long-distance passenger aircraft. After the beginning of the explosive eruption of the Eyjafjallajökull volcano on Iceland on 14 April 2010, the first CARIBIC volcano-specific measurement flight was carried out over the Baltic Sea and Southern Sweden on 20 April. Two more flights followed: one over Ireland and the Irish Sea on 16 May and the other over the Norwegian Sea on 19 May 2010. During these three special mission flights the CARIBIC container proved its merits as a comprehensive flying laboratory. The elemental composition of particles collected over the Baltic Sea during the first flight (20 April) indicated the presence of volcanic ash. Over Northern Ireland and the Irish Sea (16 May), the DOAS system detected SO2 and BrO co-located with volcanic ash particles that increased the aerosol optical depth. Over the Norwegian Sea (19 May), the optical particle counter detected a strong increase of particles larger than 400 nm diameter in a region where ash clouds were predicted by aerosol dispersion models. Aerosol particle samples collected over the Irish Sea and the Norwegian Sea showed large relative enhancements of the elements silicon, iron, titanium and calcium. Non-methane hydrocarbon concentrations in whole air samples collected on 16 and 19 May 2010 showed a pattern of removal of several hydrocarbons that is typical for chlorine chemistry in the volcanic clouds. Comparisons of measured ash concentrations and simulations with the FLEXPART dispersion model demonstrate the difficulty of detailed volcanic ash dispersion modelling due to the large variability of the volcanic cloud sources, extent and patchiness as well as the thin ash layers formed in the volcanic clouds.
- ItemMobility particle size spectrometers: Calibration procedures and measurement uncertainties(Philadelphia, Pa : Taylor & Francis, 2017) Wiedensohler, A.; Wiesner, A.; Weinhold, K.; Birmili, W.; Hermann, M.; Merkel, M.; Müller, T.; Pfeifer, S.; Schmidt, A.; Tuch, T.; Velarde, F.; Quincey, P.; Seeger, S.; Nowak, A.Mobility particle size spectrometers (MPSS) belong to the essential instruments in aerosol science that determine the particle number size distribution (PNSD) in the submicrometer size range. Following calibration procedures and target uncertainties against standards and reference instruments are suggested for a complete MPSS quality assurance program: (a) calibration of the CPC counting efficiency curve (within 5% for the plateau counting efficiency; within 1 nm for the 50% detection efficiency diameter), (b) sizing calibration of the MPSS, using a certified polystyrene latex (PSL) particle size standard at 203 nm (within 3%), (c) intercomparison of the PNSD of the MPSS (within 10% and 20% of the dN/dlogDP concentration for the particle size range 20–200 and 200–800 nm, respectively), and (d) intercomparison of the integral PNC of the MPSS (within 10%). Furthermore, following measurement uncertainties have been investigated: (a) PSL particle size standards in the range from 100 to 500 nm match within 1% after sizing calibration at 203 nm. (b) Bipolar diffusion chargers based on the radioactive nuclides Kr85, Am241, and Ni63 and a new ionizer based on corona discharge follow the recommended bipolar charge distribution, while soft X-ray-based charges may alter faster than expected. (c) The use of a positive high voltage supply show a 10% better performance than a negative one. (d) The intercomparison of the integral PNC of an MPSS against the total number concentration is still within the target uncertainty at an ambient pressure of approximately 500 hPa. Copyright © 2018 Published with license by American Association for Aerosol Research.
- ItemThe Global Aerosol Synthesis and Science Project (GASSP): Measurements and Modeling to Reduce Uncertainty(Boston, Mass. : ASM, 2017) Reddington, C.L.; Carslaw, K.S.; Stier, P.; Schutgens, N.; Coe, H.; Liu, D.; Allan, J.; Browse, J.; Pringle, K.J.; Lee, L.A.; Yoshioka, M.; Johnson, J.S.; Regayre, L.A.; Spracklen, D.V.; Mann, G.W.; Clarke, A.; Hermann, M.; Henning, S.; Wex, H.; Kristensen, T.B.; Leaitch, W.R.; Pöschl, U.; Rose, D.; Andreae, M.O.; Schmale, J.; Kondo, Y.; Oshima, N.; Schwarz, J.P.; Nenes, A.; Anderson, B.; Roberts, G.C.; Snider, J.R.; Leck, C.; Quinn, P.K.; Chi, X.; Ding, A.; Jimenez, J.L.; Zhang, Q.The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in situ measurements of the particle size distribution, number concentration, and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, to create an extensive global dataset of aerosol in situ microphysical and chemical measurements, and to develop new ways to assess the uncertainty associated with comparing sparse point measurements with low-resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modelers and nonspecialist users. Available measurements are extensive, but they are biased to polluted regions of the Northern Hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model–data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.
- ItemVariability of black carbon mass concentrations, sub-micrometer particle number concentrations and size distributions: results of the German Ultrafine Aerosol Network ranging from city street to High Alpine locations(Amsterdam [u.a.] : Elsevier Science, 2018) Sun, J.; Birmili, W.; Hermann, M.; Tuch, T.; Weinhold, K.; Spindler, G.; Schladitz, A.; Bastian, S.; Löschau, G.; Cyrys, J.; Gu, J.; Flentje, H.; Briel, B.; Asbac, C.; Kaminski, H.; Ries, L.; Sohme, R.; Gerwig, H.; Wirtz, K.; Meinhardt, F.; Schwerin, A.; Bath, O.; Ma, N.; Wiedensohler, A.This work reports the first statistical analysis of multi-annual data on tropospheric aerosols from the German Ultrafine Aerosol Network (GUAN). Compared to other networks worldwide, GUAN with 17 measurement locations has the most sites equipped with particle number size distribution (PNSD) and equivalent black carbon (eBC) instruments and the most site categories in Germany ranging from city street/roadside to High Alpine. As we know, the variations of eBC and particle number concentration (PNC) are influenced by several factors such as source, transformation, transport and deposition. The dominant controlling factor for different pollutant parameters might be varied, leading to the different spatio-temporal variations among the measured parameters. Currently, a study of spatio-temporal variations of PNSD and eBC considering the influences of both site categories and spatial scale is still missing. Based on the multi-site dataset of GUAN, the goal of this study is to investigate how pollutant parameters may interfere with spatial characteristics and site categories. © 2019 The Authors
- ItemInvestigating African trace gas sources, vertical transport, and oxidation using IAGOS-CARIBIC measurements between Germany and South Africa between 2009 and 2011(Oxford [u.a.] : Elsevier, 2017) Thorenz, U.R.; Baker, A.K.; Leedham Elvidge, E.C.; Sauvage, C.; Riede, H.; van Velthoven, P.F.J.; Hermann, M.; Weigelt, A.; Oram, D.E.; Brenninkmeijer, C.A.M.; Zahn, A.; Williams, J.Between March 2009 and March 2011 a commercial airliner equipped with a custom built measurement container (IAGOS-CARIBIC observatory) conducted 13 flights between South Africa and Germany at 10–12 km altitude, traversing the African continent north-south. In-situ measurements of trace gases (CO, CH4, H2O) and aerosol particles indicated that strong surface sources (like biomass burning) and rapid vertical transport combine to generate maximum concentrations in the latitudinal range between 10°N and 10°S coincident with the inter-tropical convergence zone (ITCZ). Pressurized air samples collected during these flights were subsequently analyzed for a suite of trace gases including C2-C8 non-methane hydrocarbons (NMHC) and halocarbons. These shorter-lived trace gases, originating from both natural and anthropogenic sources, also showed near equatorial maxima highlighting the effectiveness of convective transport in this region. Two source apportionment methods were used to investigate the specific sources of NMHC: positive matrix factorization (PMF), which is used for the first time for NMHC analysis in the upper troposphere (UT), and enhancement ratios to CO. Using the PMF method three characteristic airmass types were identified based on the different trace gas concentrations they obtained: biomass burning, fossil fuel emissions, and “background” air. The first two sources were defined with reference to previously reported surface source characterizations, while the term “background” was given to air masses in which the concentration ratios approached that of the lifetime ratios. Comparison of enhancement ratios between NMHC and CO for the subset of air samples that had experienced recent contact with the planetary boundary layer (PBL) to literature values showed that the burning of savanna and tropical forest is likely the main source of NMHC in the African upper troposphere (10–12 km). Photochemical aging patterns for the samples with PBL contact revealed that the air had different degradation histories depending on the hemisphere in which they were emitted. In the southern hemisphere (SH) air masses experienced more dilution by clean background air whereas in the northern hemisphere (NH) air masses are less diluted or mixed with background air still containing longer lived NMHC. Using NMHC photochemical clocks ozone production was seen in the BB outflow above Africa in the NH.