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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.
- ItemShip-borne aerosol profiling with lidar over the Atlantic Ocean: From pure marine conditions to complex dust-smoke mixtures(Göttingen : Copernicus GmbH, 2018) Bohlmann, S.; Baars, H.; Radenz, M.; Engelmann, R.; Macke, A.The multi-wavelength Raman lidar PollyXT has been regularly operated aboard the research vessel Polarstern on expeditions across the Atlantic Ocean from north to south and vice versa. The lidar measurements of the RV Polarstern cruises PS95 from Bremerhaven, Germany, to Cape Town, Republic of South Africa (November 2015), and PS98 from Punta Arenas, Chile, to Bremerhaven, Germany (April/May 2016), are presented and analysed in detail. The latest set-up of PollyXT allows improved coverage of the marine boundary layer (MBL) due to an additional near-range receiver. Three case studies provide an overview of the aerosol detected over the Atlantic Ocean. In the first case, marine conditions were observed near South Africa on the autumn cruise PS95. Values of optical properties (depolarisation ratios close to zero, lidar ratios of 23 sr at 355 and 532 nm) within the MBL indicate pure marine aerosol. A layer of dried marine aerosol, indicated by an increase of the particle depolarisation ratio to about 10% at 355 nm (9% at 532 nm) and thus confirming the non-sphericity of these particles, could be detected on top of the MBL. On the same cruise, an almost pure Saharan dust plume was observed near the Canary Islands, presented in the second case. The third case deals with several layers of Saharan dust partly mixed with biomass-burning smoke measured on PS98 near the Cabo Verde islands. While the MBL was partly mixed with dust in the pure Saharan dust case, an almost marine MBL was observed in the third case. A statistical analysis showed latitudinal differences in the optical properties within the MBL, caused by the downmixing of dust in the tropics and anthropogenic influences in the northern latitudes, whereas the optical properties of the MBL in the Southern Hemisphere correlate with typical marine values. The particle depolarisation ratio of dried marine layers ranged between 4 and 9% at 532 nm. Night measurements from PS95 and PS98 were used to illustrate the potential of aerosol classification using lidar ratio, particle depolarisation ratio at 355 and 532 nm, and Angström exponent. Lidar ratio and particle depolarisation ratio have been found to be the main indicator for particle type, whereas the Ångström exponent is rather variable.
- 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.
- 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
- ItemRetrieving horizontally resolved wind fields using multi-static meteor radar observations(Göttingen : Copernicus GmbH, 2018) Stober, G.; Chau, J.L.; Vierinen, J.; Jacobi, C.; Wilhelm, S.Recently, the MMARIA (Multi-static, Multi-frequency Agile Radar for Investigations of the Atmosphere) concept of a multi-static VHF meteor radar network to derive horizontally resolved wind fields in the mesosphere-lower thermosphere was introduced. Here we present preliminary results of the MMARIA network above Eastern Germany using two transmitters located at Juliusruh and Collm, and five receiving links: two monostatic and three multi-static. The observations are complemented during a one-week campaign, with a couple of addition continuous-wave coded transmitters, making a total of seven multi-static links. In order to access the kinematic properties of non-homogenous wind fields, we developed a wind retrieval algorithm that applies regularization to determine the non-linear wind field in the altitude range of 82-98 km. The potential of such observations and the new retrieval to investigate gravity waves with horizontal scales between 50-200 km is presented and discussed. In particular, it is demonstrated that horizonal wavelength spectra of gravity waves can be obtained from the new data set. © Author(s) 2018.
- ItemDerivation of gravity wave intrinsic parameters and vertical wavelength using a single scanning OH(3-1) airglow spectrometer(Katlenburg-Lindau : Copernicus, 2018-5-18) Wüst, Sabine; Offenwanger, Thomas; Schmidt, Carsten; Bittner, Michael; Jacobi, Christoph; Stober, Gunter; Yee, Jeng-Hwa; Mlynczak, Martin G.; Russell III, James M.For the first time, we present an approach to derive zonal, meridional, and vertical wavelengths as well as periods of gravity waves based on only one OH* spectrometer, addressing one vibrational-rotational transition. Knowledge of these parameters is a precondition for the calculation of further information, such as the wave group velocity vector. OH(3-1) spectrometer measurements allow the analysis of gravity wave ground-based periods but spatial information cannot necessarily be deduced. We use a scanning spectrometer and harmonic analysis to derive horizontal wavelengths at the mesopause altitude above Oberpfaffenhofen (48.09∘ N, 11.28∘ E), Germany for 22 nights in 2015. Based on the approximation of the dispersion relation for gravity waves of low and medium frequencies and additional horizontal wind information, we calculate vertical wavelengths. The mesopause wind measurements nearest to Oberpfaffenhofen are conducted at Collm (51.30∘ N, 13.02∘ E), Germany, ca. 380 km northeast of Oberpfaffenhofen, by a meteor radar. In order to compare our results, vertical temperature profiles of TIMED-SABER (thermosphere ionosphere mesosphere energetics dynamics, sounding of the atmosphere using broadband emission radiometry) overpasses are analysed with respect to the dominating vertical wavelength.
- ItemA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: Improvement of particulate nitrate prediction(Katlenburg-Lindau : EGU, 2018) Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, AlfredThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R Combining double low line 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-Muscat, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.
- ItemSimultaneous observations of NLCs and MSEs at midlatitudes: Implications for formation and advection of ice particles(Göttingen : Copernicus GmbH, 2018) Gerding, M.; Zöllner, J.; Zecha, M.; Baumgarten, K.; Höffner, J.; Stober, G.; Lübken, F.-J.We combined ground-based lidar observations of noctilucent clouds (NLCs) with collocated, simultaneous radar observations of mesospheric summer echoes (MSEs) in order to compare ice cloud altitudes at a midlatitude site (Kühlungsborn, Germany, 54° N, 12° E). Lidar observations are limited to larger particles ( > 10 nm), while radars are also sensitive to small particles ( < 10 nm), but require sufficient ionization and turbulence at the ice cloud altitudes. The combined lidar and radar data set thus includes some information on the size distribution within the cloud and through this on the of the cloud. The soundings for this study are carried out by the IAP Rayleigh-Mie-Raman (RMR) lidar and the OSWIN VHF radar. On average, there is no difference between the lower edges (lowNLC and lowMSE). The mean difference of the upper edges upNLC and upMSE is g1/4 500 m, which is much less than expected from observations at higher latitudes. In contrast to high latitudes, the MSEs above our location typically do not reach much higher than the NLCs. In addition to earlier studies from our site, this gives additional evidence for the supposition that clouds containing large enough particles to be observed by lidar are not formed locally but are advected from higher latitudes. During the advection process, the smaller particles in the upper part of the cloud either grow and sediment, or they sublimate. Both processes result in a thinning of the layer. High-altitude MSEs, usually indicating nucleation of ice particles, are rarely observed in conjunction with lidar observations of NLCs at Kühlungsborn. © Author(s) 2018.
- ItemThe impact of mineral dust on cloud formation during the Saharan dust event in April 2014 over Europe(Göttingen : Copernicus GmbH, 2018) Weger, M.; Heinold, B.; Engler, C.; Schumann, U.; Seifert, A.; Fößig, R.; Voigt, C.; Baars, H.; Blahak, U.; Borrmann, S.; Hoose, C.; Kaufmann, S.; Krämer, M.; Seifert, P.; Senf, F.; Schneider, J.; Tegen, I.A regional modeling study on the impact of desert dust on cloud formation is presented for a major Saharan dust outbreak over Europe from 2 to 5 April 2014. The dust event coincided with an extensive and dense cirrus cloud layer, suggesting an influence of dust on atmospheric ice nucleation. Using interactive simulation with the regional dust model COSMO-MUSCAT, we investigate cloud and precipitation representation in the model and test the sensitivity of cloud parameters to dust-cloud and dust-radiation interactions of the simulated dust plume. We evaluate model results with ground-based and spaceborne remote sensing measurements of aerosol and cloud properties, as well as the in situ measurements obtained during the ML-CIRRUS aircraft campaign. A run of the model with single-moment bulk microphysics without online dust feedback considerably underestimated cirrus cloud cover over Germany in the comparison with infrared satellite imagery. This was also reflected in simulated upper-Tropospheric ice water content (IWC), which accounted for only 20 % of the observed values. The interactive dust simulation with COSMO-MUSCAT, including a two-moment bulk microphysics scheme and dust-cloud as well as dust-radiation feedback, in contrast, led to significant improvements. The modeled cirrus cloud cover and IWC were by at least a factor of 2 higher in the relevant altitudes compared to the noninteractive model run. We attributed these improvements mainly to enhanced deposition freezing in response to the high mineral dust concentrations. This was corroborated further in a significant decrease in ice particle radii towards more realistic values, compared to in situ measurements from the ML-CIRRUS aircraft campaign. By testing different empirical ice nucleation parameterizations, we further demonstrate that remaining uncertainties in the ice-nucleating properties of mineral dust affect the model performance at least as significantly as including the online representation of the mineral dust distribution. Dust-radiation interactions played a secondary role for cirrus cloud formation, but contributed to a more realistic representation of precipitation by suppressing moist convection in southern Germany. In addition, a too-low specific humidity in the 7 to 10 km altitude range in the boundary conditions was identified as one of the main reasons for misrepresentation of cirrus clouds in this model study.