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- ItemAtmospheric new particle formation at the research station Melpitz, Germany: Connection with gaseous precursors and meteorological parameters(Katlenburg-Lindau : EGU, 2018) Größ, Johannes; Hamed, Amar; Sonntag, André; Spindler, Gerald; Manninen, Hanna Elina; Nieminen, Tuomo; Kulmala, Markku; Hõrrak, Urmas; Plass-Dülmer, Christian; Wiedensohler, Alfred; Birmili, WolframThis paper revisits the atmospheric new particle formation (NPF) process in the polluted Central European troposphere, focusing on the connection with gas-phase precursors and meteorological parameters. Observations were made at the research station Melpitz (former East Germany) between 2008 and 2011 involving a neutral cluster and air ion spectrometer (NAIS). Particle formation events were classified by a new automated method based on the convolution integral of particle number concentration in the diameter interval 2-20 nm. To study the relevance of gaseous sulfuric acid as a precursor for nucleation, a proxy was derived on the basis of direct measurements during a 1-month campaign in May 2008. As a major result, the number concentration of freshly produced particles correlated significantly with the concentration of sulfur dioxide as the main precursor of sulfuric acid. The condensation sink, a factor potentially inhibiting NPF events, played a subordinate role only. The same held for experimentally determined ammonia concentrations. The analysis of meteorological parameters confirmed the absolute need for solar radiation to induce NPF events and demonstrated the presence of significant turbulence during those events. Due to its tight correlation with solar radiation, however, an independent effect of turbulence for NPF could not be established. Based on the diurnal evolution of aerosol, gas-phase, and meteorological parameters near the ground, we further conclude that the particle formation process is likely to start in elevated parts of the boundary layer rather than near ground level.
- ItemLong-range and local air pollution: What can we learn from chemical speciation of particulate matter at paired sites?(Katlenburg-Lindau : EGU, 2020) Pandolfi, Marco; Mooibroek, Dennis; Hopke, Philip; van Pinxteren, Dominik; Querol, Xavier; Herrmann, Hartmut; Alastuey, Andrés; Favez, Olivier; Hüglin, Christoph; Perdrix, Esperanza; Riffault, Véronique; Sauvage, Stéphane; van der Swaluw, Eric; Tarasova, Oksana; Colette, AugustinHere we report results of a detailed analysis of the urban and non-urban contributions to particulate matter (PM) concentrations and source contributions in five European cities, namely Schiedam (the Netherlands, NL), Lens (France, FR), Leipzig (Germany, DE), Zurich (Switzerland, CH) and Barcelona (Spain, ES). PM chemically speciated data from 12 European paired monitoring sites (one traffic, five urban, five regional and one continental background) were analysed by positive matrix factorisation (PMF) and Lenschow's approach to assign measured PM and source contributions to the different spatial levels. Five common sources were obtained at the 12 sites: sulfate-rich (SSA) and nitrate-rich (NSA) aerosols, road traffic (RT), mineral matter (MM), and aged sea salt (SS). These sources explained from 55 % to 88 % of PM mass at urban low-traffic-impact sites (UB) depending on the country. Three additional common sources were identified at a subset of sites/countries, namely biomass burning (BB) (FR, CH and DE), explaining an additional 9 %-13 % of PM mass, and residual oil combustion (V-Ni) and primary industrial (IND) (NL and ES), together explaining an additional 11 %-15 % of PM mass. In all countries, the majority of PM measured at UB sites was of a regional+continental (R+C) nature (64 %-74 %). The R+C PM increments due to anthropogenic emissions in DE, NL, CH, ES and FR represented around 66 %, 62 %, 52 %, 32 % and 23 %, respectively, of UB PM mass. Overall, the R+C PM increments due to natural and anthropogenic sources showed opposite seasonal profiles with the former increasing in summer and the latter increasing in winter, even if exceptions were observed. In ES, the anthropogenic R+C PM increment was higher in summer due to high contributions from regional SSA and V-Ni sources, both being mostly related to maritime shipping emissions at the Spanish sites. Conversely, in the other countries, higher anthropogenic R+C PM increments in winter were mostly due to high contributions from NSA and BB regional sources during the cold season. On annual average, the sources showing higher R+C increments were SSA (77 %-91 % of SSA source contribution at the urban level), NSA (51 %-94 %), MM (58 %-80 %), BB (42 %-78 %) and IND (91 % in NL). Other sources showing high R+C increments were photochemistry and coal combustion (97 %-99 %; identified only in DE). The highest regional SSA increment was observed in ES, especially in summer, and was related to ship emissions, enhanced photochemistry and peculiar meteorological patterns of the Western Mediterranean. The highest R+C and urban NSA increments were observed in NL and associated with high availability of precursors such as NOx and NH3. Conversely, on average, the sources showing higher local increments were RT (62 %-90 % at all sites) and V-Ni (65 %-80 % in ES and NL). The relationship between SSA and V-Ni indicated that the contribution of ship emissions to the local sulfate concentrations in NL has strongly decreased since 2007 thanks to the shift from high-sulfur-to low-sulfur-content fuel used by ships. An improvement of air quality in the five cities included here could be achieved by further reducing local (urban) emissions of PM, NOx and NH3 (from both traffic and non-traffic sources) but also SO2 and PM (from maritime ships and ports) and giving high relevance to non-urban contributions by further reducing emissions of SO2 (maritime shipping) and NH3 (agriculture) and those from industry, regional BB sources and coal combustion. © 2020 Copernicus GmbH. All rights reserved.
- ItemEARLINET evaluation of the CATS Level 2 aerosol backscatter coefficient product(Katlenburg-Lindau : EGU, 2019) Proestakis, Emmanouil; Amiridis, Vassilis; Marinou, Eleni; Binietoglou, Ioannis; Ansmann, Albert; Wandinger, Ulla; Hofer, Julian; Yorks, John; Nowottnick, Edward; Makhmudov, Abduvosit; Papayannis, Alexandros; Pietruczuk, Aleksander; Gialitaki, Anna; Apituley, Arnoud; Szkop, Artur; Muñoz Porcar, Constantino; Bortoli, Daniele; Dionisi, Davide; Althausen, Dietrich; Mamali, Dimitra; Balis, Dimitris; Nicolae, Doina; Tetoni, Eleni; Liberti, Gian Luigi; Baars, Holger; Mattis, Ina; Stachlewska, Iwona Sylwia; Voudouri, Kalliopi Artemis; Mona, Lucia; Mylonaki, Maria; Perrone, Maria Rita; Costa, Maria João; Sicard, Michael; Papagiannopoulos, Nikolaos; Siomos, Nikolaos; Burlizzi, Pasquale; Pauly, Rebecca; Engelmann, Ronny; Abdullaev, Sabur; Pappalardo, GelsominaWe present the evaluation activity of the European Aerosol Research Lidar Network (EARLINET) for the quantitative assessment of the Level 2 aerosol backscatter coefficient product derived by the Cloud-Aerosol Transport System (CATS) aboard the International Space Station (ISS; Rodier et al., 2015). The study employs correlative CATS and EARLINET backscatter measurements within a 50km distance between the ground station and the ISS overpass and as close in time as possible, typically with the starting time or stopping time of the EARLINET performed measurement time window within 90min of the ISS overpass, for the period from February 2015 to September 2016. The results demonstrate the good agreement of the CATS Level 2 backscatter coefficient and EARLINET. Three ISS overpasses close to the EARLINET stations of Leipzig, Germany; Évora, Portugal; and Dushanbe, Tajikistan, are analyzed here to demonstrate the performance of the CATS lidar system under different conditions. The results show that under cloud-free, relative homogeneous aerosol conditions, CATS is in good agreement with EARLINET, independent of daytime and nighttime conditions. CATS low negative biases are observed, partially attributed to the deficiency of lidar systems to detect tenuous aerosol layers of backscatter signal below the minimum detection thresholds; these are biases which may lead to systematic deviations and slight underestimations of the total aerosol optical depth (AOD) in climate studies. In addition, CATS misclassification of aerosol layers as clouds, and vice versa, in cases of coexistent and/or adjacent aerosol and cloud features, occasionally leads to non-representative, unrealistic, and cloud-contaminated aerosol profiles. Regarding solar illumination conditions, low negative biases in CATS backscatter coefficient profiles, of the order of 6.1%, indicate the good nighttime performance of CATS. During daytime, a reduced signal-to-noise ratio by solar background illumination prevents retrievals of weakly scattering atmospheric layers that would otherwise be detectable during nighttime, leading to higher negative biases, of the order of 22.3%. © Author(s) 2019.
- ItemAir pollution trapping in the Dresden Basin from gray-zone scale urban modeling(Katlenburg-Lindau : EGU, 2023) Weger, Michael; Heinold, BerndThe microscale variability of urban air pollution is essentially driven by the interaction between meteorology and urban topography, which remains challenging to represent spatially accurately and computationally efficiently in urban dispersion models. Natural topography can additionally exert a considerable amplifying effect on urban background pollution, depending on atmospheric stability. This requires an equally important representation in models, as even subtle terrain-height variations can enforce characteristic local flow regimes. In this model study, the effects of urban and natural topography on the local winds and air pollution dispersion in the Dresden Basin in the Eastern German Elbe valley are investigated. A new, efficient urban microscale model is used within a multiscale air quality modeling framework. The simulations that consider real meteorological and emission conditions focus on two periods in late winter and early summer, respectively, as well as on black carbon (BC), a key air pollutant mainly emitted from motorized traffic. As a complement to the commonly used mass concentrations, the particle age content (age concentration) is simulated. This concept, which was originally developed to study hydrological reservoir flows in a Eulerian framework, is adapted here for the first time for atmospheric boundary-layer modeling. The approach is used to identify stagnant or recirculating orographic air flows and resulting air pollution trapping. An empirical orthogonal function (EOF) analysis is applied to the simulation results to attribute the air pollution modes to specific weather patterns and quantify their significance. Air quality monitoring data for the region are used for model evaluation. The model results show a strong sensitivity to atmospheric conditions, but generally confirm increased BC levels in Dresden due to the valley location. The horizontal variability of mass concentrations is dominated by the patterns of traffic emissions, which overlay potential orography-driven pollutant accumulations. Therefore, an assessment of the orographic impact on air pollution is usually inconclusive. However, using the age-concentration metric, which filters out direct emission effects, previously undetected spatial patterns are discovered that are largely modulated by the surface orography. The comparison with a dispersion simulation assuming spatially homogeneous emissions also proves the robustness of the orographic flow information contained in the age-concentration distribution and shows it to be a suitable metric for assessing orographic air pollution trapping. The simulation analysis indicates several air quality hotspots on the southwestern slopes of the Dresden Basin and in the southern side valley, the Döhlen Basin, depending on the prevailing wind direction.
- ItemThe HD(CP)2 Observational Prototype Experiment (HOPE) - An overview(Katlenburg-Lindau : EGU, 2017) Macke, Andreas; Seifert, Patric; Baars, Holger; Barthlott, Christian; Beekmans, Christoph; Behrendt, Andreas; Bohn, Birger; Brueck, Matthias; Bühl, Johannes; Crewell, Susanne; Damian, Thomas; Deneke, Hartwig; Düsing, Sebastian; Foth, Andreas; Di Girolamo, Paolo; Hammann, Eva; Heinze, Rieke; Hirsikko, Anne; Kalisch, John; Kalthoff, Norbert; Kinne, Stefan; Kohler, Martin; Löhnert, Ulrich; Madhavan, Bomidi Lakshmi; Maurer, Vera; Muppa, Shravan Kumar; Schween, Jan; Serikov, Ilya; Siebert, Holger; Simmer, Clemens; Späth, Florian; Steinke, Sandra; Träumner, Katja; Trömel, Silke; Wehner, Birgit; Wieser, Andreas; Wulfmeyer, Volker; Xie, XinxinThe HD(CP)2 Observational Prototype Experiment (HOPE) was performed as a major 2-month field experiment in Jülich, Germany, in April and May 2013, followed by a smaller campaign in Melpitz, Germany, in September 2013. HOPE has been designed to provide an observational dataset for a critical evaluation of the new German community atmospheric icosahedral non-hydrostatic (ICON) model at the scale of the model simulations and further to provide information on land-surface-atmospheric boundary layer exchange, cloud and precipitation processes, as well as sub-grid variability and microphysical properties that are subject to parameterizations. HOPE focuses on the onset of clouds and precipitation in the convective atmospheric boundary layer. This paper summarizes the instrument set-ups, the intensive observation periods, and example results from both campaigns.
HOPE-Jülich instrumentation included a radio sounding station, 4 Doppler lidars, 4 Raman lidars (3 of them provide temperature, 3 of them water vapour, and all of them particle backscatter data), 1 water vapour differential absorption lidar, 3 cloud radars, 5 microwave radiometers, 3 rain radars, 6 sky imagers, 99 pyranometers, and 5 sun photometers operated at different sites, some of them in synergy. The HOPE-Melpitz campaign combined ground-based remote sensing of aerosols and clouds with helicopter- and balloon-based in situ observations in the atmospheric column and at the surface.
HOPE provided an unprecedented collection of atmospheric dynamical, thermodynamical, and micro- and macrophysical properties of aerosols, clouds, and precipitation with high spatial and temporal resolution within a cube of approximately 10 × 10 × 10km3. HOPE data will significantly contribute to our understanding of boundary layer dynamics and the formation of clouds and precipitation. The datasets have been made available through a dedicated data portal.
First applications of HOPE data for model evaluation have shown a general agreement between observed and modelled boundary layer height, turbulence characteristics, and cloud coverage, but they also point to significant differences that deserve further investigations from both the observational and the modelling perspective. - ItemFirst triple-wavelength lidar observations of depolarization and extinction-to-backscatter ratios of Saharan dus(Katlenburg-Lindau : EGU, 2022) Haarig, Moritz; Ansmann, Albert; Engelmann, Ronny; Baars, Holger; Toledano, Carlos; Torres, Benjamin; Althausen, Dietrich; Radenz, Martin; Wandinger, UllaTwo layers of Saharan dust observed over Leipzig, Germany, in February and March 2021 were used to provide the first-ever lidar measurements of the dust lidar ratio (extinction-to-backscatter ratio) and linear depolarization ratio at all three classical lidar wavelengths (355, 532 and 1064gnm). The pure-dust conditions during the first event exhibit lidar ratios of 47g±g8, 50g±g5 and 69g±g14gsr and particle linear depolarization ratios of 0.242g±g0.024, 0.299g±g0.018 and 0.206g±g0.010 at wavelengths of 355, 532 and 1064gnm, respectively. The second, slightly polluted-dust case shows a similar spectral behavior of the lidar and depolarization ratio with values of the lidar ratio of 49g±g4, 46g±g5 and 57g±g9gsr and the depolarization ratio of 0.174g±g0.041, 0.298g±g0.016 and 0.242g±g0.007 at 355, 532 and 1064gnm, respectively. The results were compared with Aerosol Robotic Network (AERONET) version 3 (v3) inversion solutions and the Generalized Retrieval of Aerosol and Surface Properties (GRASP) at six and seven wavelengths. Both retrieval schemes make use of a spheroid shape model for mineral dust. The spectral slope of the lidar ratio from 532 to 1064gnm could be well reproduced by the AERONET and GRASP retrieval schemes. Higher lidar ratios in the UV were retrieved by AERONET and GRASP. The enhancement was probably caused by the influence of fine-mode pollution particles in the boundary layer which are included in the columnar photometer measurements. Significant differences between the measured and retrieved wavelength dependence of the particle linear depolarization ratio were found. The potential sources for these uncertainties are discussed.
- ItemMercury distribution in the upper troposphere and lowermost stratosphere according to measurements by the IAGOS-CARIBIC observatory: 2014-2016(Katlenburg-Lindau : EGU, 2018) Slemr, Franz; Weigelt, Andreas; Ebinghaus, Ralf; Bieser, Johannes; Brenninkmeijer, Carl A. M.; Rauthe-Schöch, Armin; Hermann, Markus; Martinsson, Bengt G.; van Velthoven, Peter; Bönisch, Harald; Neumaier, Marco; Zahn, Andreas; Ziereis, HelmutMercury was measured onboard the IAGOS-CARIBIC passenger aircraft from May 2005 until February 2016 during near monthly sequences of mostly four intercontinental flights from Germany to destinations in North and South America, Africa and South and East Asia. Most of these mercury data were obtained using an internal default signal integration procedure of the Tekran instrument but since April 2014 more precise and accurate data were obtained using post-flight manual integration of the instrument raw signal. In this paper we use the latter data. Increased upper tropospheric total mercury (TM) concentrations due to large scale biomass burning were observed in the upper troposphere (UT) at the equator and southern latitudes during the flights to Latin America and South Africa in boreal autumn (SON) and boreal winter (DJF). TM concentrations in the lowermost stratosphere (LMS) decrease with altitude above the thermal tropopause but the gradient is less steep than reported before. Seasonal variation of the vertical TM distribution in the UT and LMS is similar to that of other trace gases with surface sources and stratospheric sinks. Speciation experiments suggest comparable TM and gaseous elementary mercury (GEM) concentrations at and below the tropopause leaving little space for Hg2+ (TM-thinsp;GEM) being the dominating component of TM here. In the stratosphere significant GEM concentrations were found to exist up to 4 km altitude above the thermal tropopause. Correlations with N2O as a reference tracer suggest stratospheric lifetimes of 72±37 and 74±27 years for TM and GEM, respectively, comparable to the stratospheric lifetime of COS. This coincidence, combined with pieces of evidence from us and other researchers, corroborates the hypothesis that Hg2+ formed by oxidation in the stratosphere attaches to sulfate particles formed mainly by oxidation of COS and is removed with them from the stratosphere by air mass exchange, gravitational sedimentation and cloud scavenging processes.
- ItemMultiresolution analysis of the spatiotemporal variability in global radiation observed by a dense network of 99 pyranometers(Katlenburg-Lindau : EGU, 2017) Madhavan, Bomidi Lakshmi; Deneke, Hartwig; Witthuhn, Jonas; Macke, AndreasThe time series of global radiation observed by a dense network of 99 autonomous pyranometers during the HOPE campaign around Jülich, Germany, are investigated with a multiresolution analysis based on the maximum overlap discrete wavelet transform and the Haar wavelet. For different sky conditions, typical wavelet power spectra are calculated to quantify the timescale dependence of variability in global transmittance. Distinctly higher variability is observed at all frequencies in the power spectra of global transmittance under broken-cloud conditions compared to clear, cirrus, or overcast skies. The spatial autocorrelation function including its frequency dependence is determined to quantify the degree of similarity of two time series measurements as a function of their spatial separation. Distances ranging from 100-m to 10-km are considered, and a rapid decrease of the autocorrelation function is found with increasing frequency and distance. For frequencies above 1-3-ming-1 and points separated by more than 1-km, variations in transmittance become completely uncorrelated. A method is introduced to estimate the deviation between a point measurement and a spatially averaged value for a surrounding domain, which takes into account domain size and averaging period, and is used to explore the representativeness of a single pyranometer observation for its surrounding region. Two distinct mechanisms are identified, which limit the representativeness; on the one hand, spatial averaging reduces variability and thus modifies the shape of the power spectrum. On the other hand, the correlation of variations of the spatially averaged field and a point measurement decreases rapidly with increasing temporal frequency. For a grid box of 10-km-×-10-km and averaging periods of 1.5-3-h, the deviation of global transmittance between a point measurement and an area-averaged value depends on the prevailing sky conditions: 2.8 (clear), 1.8 (cirrus), 1.5 (overcast), and 4.2-% (broken clouds). The solar global radiation observed at a single station is found to deviate from the spatial average by as much as 14-23 (clear), 8-26 (cirrus), 4-23 (overcast), and 31-79-Wg-mg-2 (broken clouds) from domain averages ranging from 1-km-×-1-km to 10-km-×-10-km in area.
- ItemAerosol activation characteristics and prediction at the central European ACTRIS research station of Melpitz, Germany(Katlenburg-Lindau : EGU, 2022) Wang, Yuan; Henning, Silvia; Poulain, Laurent; Lu, Chunsong; Stratmann, Frank; Wang, Yuying; Niu, Shengjie; Pöhlker, Mira L.; Herrmann, Hartmut; Wiedensohler, AlfredUnderstanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1% to 0.7%, the median NCCN increases from 399 to 2144cm-3, which represents 10% to 48% of the total particle number concentration with a diameter range of 10-800nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SSCombining double low line0.1%, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of 1/440 to 100nm and almost stays constant at Dp of 100 to 200nm, whereas the degree of the external mixture keeps decreasing at Dp of 1/440 to 200nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ-Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ-Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ-Dp relationships for different regions and their seasonal variations.
- ItemRole of the dew water on the ground surface in HONO distribution: A case measurement in Melpitz(Katlenburg-Lindau : EGU, 2020) Ren, Yangang; Stieger, Bastian; Spindler, Gerald; Grosselin, Benoit; Mellouki, Abdelwahid; Tuch, Thomas; Wiedensohler, Alfred; Herrmann, HartmutTo characterize the role of dew water for the ground surface HONO distribution, nitrous acid (HONO) measurements with a Monitor for AeRosols and Gases in ambient Air (MARGA) and a LOng Path Absorption Photometer (LOPAP) instrument were performed at the Leibniz Institute for Tropospheric Research (TROPOS) research site in Melpitz, Germany, from 19 to 29 April 2018. The dew water was also collected and analyzed from 8 to 14 May 2019 using a glass sampler. The high time resolution of HONO measurements showed characteristic diurnal variations that revealed that (i) vehicle emissions are a minor source of HONO at Melpitz station; (ii) the heterogeneous conversion of NO2 to HONO on the ground surface dominates HONO production at night; (iii) there is significant nighttime loss of HONO with a sink strength of 0.16±0.12ppbv h-1; and (iv) dew water with mean NO-2 of 7.91±2.14 μgm-2 could serve as a temporary HONO source in the morning when the dew droplets evaporate. The nocturnal observations of HONO and NO2 allowed the direct evaluation of the ground uptake coefficients for these species at night: γNO2→HONO = 2.4±10-7 to 3.5±10-6, γHONO;ground = 1.7×10-5 to 2.8×10-4. A chemical model demonstrated that HONO deposition to the ground surface at night was 90 %-100% of the calculated unknown HONO source in the morning. These results suggest that dew water on the ground surface was controlling the temporal HONO distribution rather than straightforward NO2-HONO conversion. This can strongly enhance the OH reactivity throughout the morning time or in other planted areas that provide a large amount of ground surface based on the OH production rate calculation. © 2020 Copernicus GmbH. All rights reserved.