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    Multivariate non-parametric Euclidean distance model for hourly disaggregation of daily climate data
    (Wien [u.a.] : Springer, 2021) Görner, Christina; Franke, Johannes; Kronenberg, Rico; Hellmuth, Olaf; Bernhofer, Christian
    The algorithm for and results of a newly developed multivariate non-parametric model, the Euclidean distance model (EDM), for the hourly disaggregation of daily climate data are presented here. The EDM is a resampling method based on the assumption that the day to be disaggregated has already occurred once in the past. The Euclidean distance (ED) serves as a measure of similarity to select the most similar day from historical records. EDM is designed to disaggregate daily means/sums of several climate elements at once, here temperature (T), precipitation (P), sunshine duration (SD), relative humidity (rH), and wind speed (WS), while conserving physical consistency over all disaggregated elements. Since weather conditions and hence the diurnal cycles of climate elements depend on the weather pattern, a selection approach including objective weather patterns (OWP) was developed. The OWP serve as an additional criterion to filter the most similar day. For a case study, EDM was applied to the daily climate data of the stations Dresden and Fichtelberg (Saxony, Germany). The EDM results agree well with the observed data, maintaining their statistics. Hourly results fit better for climate elements with homogenous diurnal cycles, e.g., T with very high correlations of up to 0.99. In contrast, the hourly results of the SD and the WS provide correlations up to 0.79. EDM tends to overestimate heavy precipitation rates, e.g., by up to 15% for Dresden and 26% for Fichtelberg, potentially due to, e.g., the smaller data pool for such events, and the equal-weighted impact of P in the ED calculation. The OWPs lead to somewhat improved results for all climate elements in terms of similar climate conditions of the basic stations. Finally, the performance of EDM is compared with the disaggregation tool MELODIST (Förster et al. 2015). Both tools deliver comparable and well corresponding results. All analyses of the generated hourly data show that EDM is a very robust and flexible model that can be applied to any climate station. Since EDM can disaggregate daily data of climate projections, future research should address whether the model is capable to respect and (re)produce future climate trends. Further, possible improvements by including the flow direction and future OWPs should be investigated, also with regard to reduce the overestimation of heavy rainfall rates.
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    Increasing the spatial resolution of cloud property retrievals from Meteosat SEVIRI by use of its high-resolution visible channel: Evaluation of candidate approaches with MODIS observations
    (Katlenburg-Lindau : Copernicus, 2020) Werner, Frank; Deneke, Hartwig
    This study presents and evaluates several candidate approaches for downscaling observations from the Spinning Enhanced Visible and Infrared Imager (SEVIRI) in order to increase the horizontal resolution of subsequent cloud optical thickness (τ) and effective droplet radius (reff) retrievals from the native ≈ 3km×3km spatial resolution of the narrowband channels to ≈ 1km×1km. These methods make use of SEVIRI's coincident broadband high-resolution visible (HRV) channel. For four example cloud fields, the reliability of each downscaling algorithm is evaluated by means of collocated 1km×1km MODIS radiances, which are reprojected to the horizontal grid of the HRV channel and serve as reference for the evaluation. By using these radiances, smoothed with the modulation transfer function of the native SEVIRI channels, as retrieval input, the accuracy at the SEVIRI standard resolution can be evaluated and an objective comparison of the accuracy of the different downscaling algorithms can be made. For the example scenes considered in this study, it is shown that neglecting high-frequency variations below the SEVIRI standard resolution results in significant random absolute deviations of the retrieved τ and reff of up to ≈ 14 and ≈ 6μm, respectively, as well as biases. By error propagation, this also negatively impacts the reliability of the subsequent calculation of liquid water path (WL) and cloud droplet number concentration (ND), which exhibit deviations of up to ≈ 89gm-2 and ≈ 177cm-3, respectively. For τ , these deviations can be almost completely mitigated by the use of the HRV channel as a physical constraint and by applying most of the presented downscaling schemes. Uncertainties in retrieved reff at the native SEVIRI resolution are smaller, and the improvements from downscaling the observations are less obvious than for τ. Nonetheless, the right choice of downscaling scheme yields noticeable improvements in the retrieved reff. Furthermore, the improved reliability in retrieved cloud products results in significantly reduced uncertainties in derived WL and ND. In particular, one downscaling approach provides clear improvements for all cloud products compared to those obtained from SEVIRI's standard resolution and is recommended for future downscaling endeavors. This work advances efforts to mitigate impacts of scale mismatches among channels of multiresolution instruments on cloud retrievals. © Author(s) 2020.
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    The realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere
    (Katlenburg-Lindau : Copernicus, 2022) Dragoneas, Antonis; Molleker, Sergej; Appel, Oliver; Hünig, Andreas; Böttger, Thomas; Hermann, Markus; Drewnick, Frank; Schneider, Johannes; Weigel, Ralf; Borrmann, Stephan
    We report on the developments that enabled the field deployment of a fully automated aerosol mass spectrometer, especially designed for high-altitude measurements on unpressurized aircraft. The merits of the two main categories of real-time aerosol mass spectrometry, i.e. (a) single-particle laser desorption and ionization and (b) continuous thermal desorption and electron impact ionization of aerosols, have been integrated into one compact apparatus with the aim to perform in situ real-time analysis of aerosol chemical composition. The demonstrated instrument, named the ERICA (European Research Council Instrument for Chemical composition of Aerosols), operated successfully aboard the high-altitude research aircraft M-55 Geophysica at altitudes up to 20 km while being exposed to ambient conditions of very low atmospheric pressure and temperature. A primary goal of those field deployments was the in situ study of the Asian tropopause aerosol layer (ATAL). During 11 research flights, the instrument operated for more than 49 h and collected chemical composition information of more than 150 000 single particles combined with quantitative chemical composition analysis of aerosol particle ensembles. This paper presents in detail the technical characteristics of the main constituent parts of the instrument, as well as the design considerations for its integration into the aircraft and its autonomous operation in the upper troposphere and lower stratosphere (UTLS). Additionally, system performance data from the first field deployments of the instrument are presented and discussed, together with exemplary mass spectrometry data collected during those flights.
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    Nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) for investigating hygroscopic properties of sub-10nm aerosol nanoparticles
    (Katlenburg-Lindau : Copernicus, 2020) Lei, Ting; Ma, Nan; Hong, Juan; Tuch, Thomas; Wang, Xin; Wang, Zhibin; Pöhlker, Mira; Ge, Maofa; Wang, Weigang; Mikhailov, Eugene; Hoffmann, Thorsten; Pöschl, Ulrich; Su, Hang; Wiedensohler, Alfred; Cheng, Yafang
    Interactions between water and nanoparticles are relevant for atmospheric multiphase processes, physical chemistry, and materials science. Current knowledge of the hygroscopic and related physicochemical properties of nanoparticles, however, is restricted by the limitations of the available measurement techniques. Here, we present the design and performance of a nano-hygroscopicity tandem differential mobility analyzer (nano-HTDMA) apparatus that enables high accuracy and precision in hygroscopic growth measurements of aerosol nanoparticles with diameters less than 10 nm. Detailed methods of calibration and validation are provided. Besides maintaining accurate and stable sheath and aerosol flow rates (1 %), high accuracy of the differential mobility analyzer (DMA) voltage (0:1 %) in the range of 0-50V is crucial for achieving accurate sizing and small sizing offsets between the two DMAs (1:4 %). To maintain a stable relative humidity (RH), the humidification system and the second DMA are placed in a well-insulated and air conditioner housing (0:1 K). We also tested and discussed different ways of preventing predeliquescence in the second DMA. Our measurement results for ammonium sulfate nanoparticles are in good agreement with Biskos et al. (2006b), with no significant size effect on the deliquescence and efflorescence relative humidity (DRH and ERH, respectively) at diameters down to 6 nm. For sodium sulfate nanoparticles, however, we find a pronounced size dependence of DRH and ERH between 20 and 6 nm nanoparticles. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.
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    CAMP: 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, Michael
    Airborne 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.
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    Application of TXRF in monitoring trace metals in particulate matter and cloud water
    (Katlenburg-Lindau : Copernicus, 2020) Fomba, Khanneh Wadinga; Deabji, Nabil; Barcha, Sayf El Islam; Ouchen, Ibrahim; Elbaramoussi, El Mehdi; El Moursli, Rajaa Cherkaoui; Harnafi, Mimoun; El Hajjaji, Souad; Mellouki, Abdelwahid; Herrmann, Hartmut
    Trace metals in ambient particulate matter and cloud are considered key elements of atmospheric processes as they affect air quality, environmental ecosystems, and cloud formation. However, they are often available at trace concentrations in these media such that their analysis requires high-precision and sensitive techniques. In this study, different analytical methods were applied to quantify trace metals in particulate matter (PM) samples collected on quartz and polycarbonate filters as well as cloud water, using the Total reflection X-Ray Fluorescence (TXRF) technique. These methods considered the measurement of filter samples directly without and with chemical pretreatment. Direct measurements involved the analysis of PM samples collected on polycarbonate filters and cloud water samples after they are brought onto TXRF carrier substrates. The chemical treatment method involved the assessment of different acid digestion procedures on PM sampled on quartz filters. The solutions applied were reverse aqua regia, nitric acid, and a combination of nitric acid and hydrogen peroxide. The effect of cold-plasma treatment of samples on polycarbonate filters before TXRF measurements was also investigated. Digestion with the reverse aqua regia solution provided lower blanks and higher recovery in comparison to other tested procedures. The detection limits of the elements ranged from 0.3 to 44 ng cm−2. Ca, K, Zn, and Fe showed the highest detection limits of 44, 35, 6, and 1 ng cm−2, while As and Se had the lowest of 0.3 and 0.8 ng cm−2, respectively. The method showed higher recovery for most trace metals when applied to commercially available reference materials and field samples. TXRF measurements showed good agreement with results obtained from ion chromatography measurements for elements such as Ca and K. Cold-plasma treatment did not significantly lead to an increase in the detected concentration, and the results were element specific. Baking of the quartz filters prior to sampling showed a reduction of more than 20 % of the filter blanks for elements such as V, Sr, Mn, Zn, and Sb. The methods were applied successfully on ambient particulate matter and cloud water samples collected from the Atlas Mohammed V station in Morocco and the Cape Verde Atmospheric Observatory. The obtained concentrations were within the range reported using different techniques from similar remote and background regions elsewhere, especially for elements of anthropogenic origins such as V, Pb, and Zn with concentrations of up to 10, 19, and 28 ng m−3, respectively. Enrichment factor analysis indicated that crustal matter dominated the abundance of most of the elements, while anthropogenic activities also contributed to the abundance of elements such as Sb, Se, and Pb. The results confirm that TXRF is a useful complementary sensitive technique for trace metal analysis of particulate matter in the microgram range as well as in cloud water droplets.
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    Characterization and first results from LACIS-T : a moist-air wind tunnel to study aerosol–cloud–turbulence interactions
    (Katlenburg-Lindau : Copernicus, 2020) Niedermeier, Dennis; Voigtländer, Jens; Schmalfuß, Silvio; Busch, Daniel; Schumacher, Jörg; Shaw, Raymond A.; Stratmann, Frank
    The interactions between turbulence and cloud microphysical processes have been investigated primarily through numerical simulation and field measurements over the last 10 years. However, only in the laboratory we can be confident in our knowledge of initial and boundary conditions and are able to measure under statistically stationary and repeatable conditions. In the scope of this paper, we present a unique turbulent moist-air wind tunnel, called the Turbulent Leipzig Aerosol Cloud Interaction Simulator (LACIS-T) which has been developed at TROPOS in order to study cloud physical processes in general and interactions between turbulence and cloud microphysical processes in particular. The investigations take place under well-defined and reproducible turbulent and thermodynamic conditions covering the temperature range of warm, mixed-phase and cold clouds (25∘C>T>−40∘C ). The continuous-flow design of the facility allows for the investigation of processes occurring on small temporal (up to a few seconds) and spatial scales (micrometer to meter scale) and with a Lagrangian perspective. The here-presented experimental studies using LACIS-T are accompanied and complemented by computational fluid dynamics (CFD) simulations which help us to design experiments as well as to interpret experimental results. In this paper, we will present the fundamental operating principle of LACIS-T, the numerical model, and results concerning the thermodynamic and flow conditions prevailing inside the wind tunnel, combining both characterization measurements and numerical simulations. Finally, the first results are depicted from deliquescence and hygroscopic growth as well as droplet activation and growth experiments. We observe clear indications of the effect of turbulence on the investigated microphysical processes.
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    A global analysis of climate-relevant aerosol properties retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories
    (Katlenburg-Lindau : Copernicus, 2020) Laj, Paolo; Bigi, Alessandro; Rose, Clémence; Andrews, Elisabeth; Lund Myhre, Cathrine; Collaud Coen, Martine; Lin, Yong; Wiedensohler, Alfred; Schulz, Michael; Ogren, John A.; Fiebig, Markus; Prenni, Anthony; Reisen, Fabienne; Romano, Salvatore; Sellegri, Karine; Sharma, Sangeeta; Schauer, Gerhard; Sheridan, Patrick; Sherman, James Patrick; Schütze, Maik; Schwerin, Andreas; Tuch, Thomas; Sohmer, Ralf; Sorribas, Mar; Steinbacher, Martin; Sun, Junying; Titos, Gloria; Toczko, Barbara; Tulet, Pierre; Tunved, Peter; Vakkari, Ville; Velarde, Fernando; Velasquez, Patricio; Villani, Paolo; Vratolis, Sterios; Wang, Sheng-Hsiang; Weinhold, Kay; Gliß, Jonas; Weller, Rolf; Yela, Margarita; Yus-Diez, Jesus; Zdimal, Vladimir; Zieger, Paul; Zikova, Nadezda; Mortier, Augustin; Pandolfi, Marco; Petäja, Tuukka; Kim, Sang-Woo; Aas, Wenche; Putaud, Jean-Philippe; Mayol-Bracero, Olga; Keywood, Melita; Labrador, Lorenzo; Aalto, Pasi; Ahlberg, Erik; Alados Arboledas, Lucas; Alastuey, Andrés; Andrade, Marcos; Artíñano, Begoña; Ausmeel, Stina; Arsov, Todor; Asmi, Eija; Backman, John; Baltensperger, Urs; Bastian, Susanne; Bath, Olaf; Beukes, Johan Paul; Brem, Benjamin T.; Bukowiecki, Nicolas; Conil, Sébastien; Couret, Cedric; Day, Derek; Dayantolis, Wan; Degorska, Anna; Eleftheriadis, Konstantinos; Fetfatzis, Prodromos; Favez, Olivier; Flentje, Harald; Gini, Maria I.; Gregorič, Asta; Gysel-Beer, Martin; Hallar, A. Gannet; Hand, Jenny; Hoffer, Andras; Hueglin, Christoph; Hooda, Rakesh K.; Hyvärinen, Antti; Kalapov, Ivo; Kalivitis, Nikos; Kasper-Giebl, Anne; Kim, Jeong Eun; Kouvarakis, Giorgos; Kranjc, Irena; Krejci, Radovan; Kulmala, Markku; Labuschagne, Casper; Lee, Hae-Jung; Lihavainen, Heikki; Lin, Neng-Huei; Löschau, Gunter; Luoma, Krista; Marinoni, Angela; Martins Dos Santos, Sebastiao; Meinhardt, Frank; Merkel, Maik; Metzger, Jean-Marc; Mihalopoulos, Nikolaos; Nguyen, Nhat Anh; Ondracek, Jakub; Pérez, Noemi; Perrone, Maria Rita; Petit, Jean-Eudes; Picard, David; Pichon, Jean-Marc; Pont, Veronique; Prats, Natalia
    Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
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    A phenomenology of new particle formation (NPF) at 13 European sites
    (Katlenburg-Lindau : European Geosciences Union, 2021) Bousiotis, Dimitrios; Pope, Francis D.; Beddows, David C. S.; Dall'Osto, Manuel; Massling, Andreas; Nøjgaard, Jakob Klenø; Nordstrøm, Claus; Niemi, Jarkko V.; Portin, Harri; Petäjä, Tuukka; Perez, Noemi; Alastuey, Andrés; Querol, Xavier; Kouvarakis, Giorgos; Mihalopoulos, Nikos; Vratolis, Stergios; Eleftheriadis, Konstantinos; Wiedensohler, Alfred; Weinhold, Kay; Merkel, Maik; Tuch, Thomas; Harrison, Roy M.
    New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (<ĝ€¯200ĝ€¯km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400ĝ€¯% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions. © Author(s) 2021.
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    Influence of low-level blocking and turbulence on the microphysics of a mixed-phase cloud in an inner-Alpine valley
    (Katlenburg-Lindau : European Geosciences Union, 2021) Ramelli, Fabiola; Henneberger, Jan; David, Robert O.; Lauber, Annika; Pasquier, Julie T.; Wieder, Jörg; Bühl, Johannes; Seifert, Patric; Engelmann, Ronny; Hervo, Maxime; Lohmann, Ulrike
    Previous studies that investigated orographic precipitation have primarily focused on isolated mountain barriers. Here we investigate the influence of low-level blocking and shear-induced turbulence on the cloud microphysics and precipitation formation in a complex inner-Alpine valley. The analysis focuses on a mid-level cloud in a post-frontal environment and a low-level feeder cloud induced by an in-valley circulation. Observations were obtained from an extensive set of instruments including ground-based remote sensing instrumentation, in situ instrumentation on a tethered-balloon system and ground-based precipitation measurements. During this event, the boundary layer was characterized by a blocked low-level flow and enhanced turbulence in the region of strong vertical wind shear at the boundary between the blocked layer in the valley and the stronger cross-barrier flow aloft. Cloud radar observations indicated changes in the microphysical cloud properties within the turbulent shear layer including enhanced linear depolarization ratio (i.e., change in particle shape or density) and increased radar reflectivity (i.e., enhanced ice growth). Based on the ice particle habits observed at the surface, we suggest that riming, aggregation and needle growth occurred within the turbulent layer. Collisions of fragile ice crystals (e.g., dendrites, needles) and the Hallett-Mossop process might have contributed to secondary ice production. Additionally, in situ instrumentation on the tethered-balloon system observed the presence of a low-level feeder cloud above a small-scale topographic feature, which dissipated when the low-level flow turned from a blocked to an unblocked state. Our observations indicate that the low-level blocking (due to the downstream mountain barrier) created an in-valley circulation, which led to the production of local updrafts and the formation of a low-level feeder cloud. Although the feeder cloud did not enhance precipitation in this particular case (since the majority of the precipitation sublimated when falling through a subsaturated layer above), we propose that local flow effects such as low-level blocking can induce the formation of feeder clouds in mountain valleys and on the leeward slope of foothills upstream of the main mountain barrier, where they can act to enhance orographic precipitation through the seeder-feeder mechanism.