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- ItemConcentration and variability of ice nuclei in the subtropical maritime boundary layer(Katlenburg-Lindau : EGU, 2018) Welti, André; Müller, Konrad; Fleming, Zoë L.; Stratmann, FrankMeasurements of the concentration and variability of ice nucleating particles in the subtropical maritime boundary layer are reported. Filter samples collected in Cabo Verde over the period 2009-2013 are analyzed with a drop freezing experiment with sensitivity to detect the few rare ice nuclei active at low supercooling. The data set is augmented with continuous flow diffusion chamber measurements at temperatures below -24 °C from a 2-month field campaign in Cabo Verde in 2016. The data set is used to address the following questions: what are typical concentrations of ice nucleating particles active at a certain temperature? What affects their concentration and where are their sources? Concentration of ice nucleating particles is found to increase exponentially by 7 orders of magnitude from -5 to -38 °C. Sample-to-sample variation in the steepness of the increase indicates that particles of different origin, with different ice nucleation properties (size, composition), contribute to the ice nuclei concentration at different temperatures. The concentration of ice nuclei active at a specific temperature varies over a range of up to 4 orders of magnitude. The frequency with which a certain ice nuclei concentration is measured within this range is found to follow a lognormal distribution, which can be explained by random dilution during transport. To investigate the geographic origin of ice nuclei, source attribution of air masses from dispersion modeling is used to classify the data into seven typical conditions. While no source could be attributed to the ice nuclei active at temperatures higher than -12 °C, concentrations at lower temperatures tend to be elevated in air masses originating from the Sahara.
- ItemInfluence of biomass burning on mixing state of sub-micron aerosol particles in the North China Plain(Oxford [u.a.] : Elsevier, 2017) Kecorius, Simonas; Ma, Nan; Teich, Monique; van Pinxteren, Dominik; Zhang, Shenglan; Gröβ, Johannes; Spindler, Gerald; Müller, Konrad; Iinuma, Yoshiteru; Hu, Min; Herrmann, Hartmut; Wiedensohler, AlfredParticulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6°N, 115.2°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP.
- ItemLong-term profiling of mineral dust and pollution aerosol with multiwavelength polarization Raman lidar at the Central Asian site of Dushanbe, Tajikistan: Case studies(München : European Geopyhsical Union, 2017) Hofer, Julian; Althausen, Dietrich; Abdullaev, Sabur F.; Makhmudov, Abduvosit N.; Nazarov, Bakhron I.; Schettler, Georg; Engelmann, Ronny; Baars, Holger; Fomba, K.Wadinga; Müller, Konrad; Heinold, Bernd; Kandler, Konrad; Ansmann, AlbertFor the first time, continuous vertically resolved aerosol measurements were performed by lidar in Tajikistan, Central Asia. Observations with the multiwavelength polarization Raman lidar PollyXT were conducted during CADEX (Central Asian Dust EXperiment) in Dushanbe, Tajikistan, from March 2015 to August 2016. Co-located with the lidar, a sun photometer was also operated. The goal of CADEX is to provide an unprecedented data set on vertically resolved aerosol optical properties in Central Asia, an area highly affected by climate change but largely missing vertically resolved aerosol measurements. During the 18-month measurement campaign, mineral dust was detected frequently from ground to the cirrus level height. In this study, an overview of the measurement period is given and four typical but different example measurement cases are discussed in detail. Three of them are dust cases and one is a contrasting pollution aerosol case. Vertical profiles of the measured optical properties and the calculated dust and non-dust mass concentrations are presented. Dust source regions were identified by means of backward trajectory analyses. A lofted layer of Middle Eastern dust with an aerosol optical thickness (AOT) of 0.4 and an extinction-related Ångström exponent of 0.41 was measured. In comparison, two near-ground dust cases have Central Asian sources. One is an extreme dust event with an AOT of 1.5 and Ångström exponent of 0.12 and the other one is a most extreme dust event with an AOT of above 4 (measured by sun photometer) and an Ångström exponent of −0.08. The observed lidar ratios (and particle linear depolarization ratios) in the presented dust cases range from 40.3 to 46.9sr (and 0.18–0.29) at 355nm and from 35.7 to 42.9sr (0.31–0.35) at 532nm wavelength. The particle linear depolarization ratios indicate almost unpolluted dust in the case of a lofted dust layer and pure dust in the near-ground dust cases. The lidar ratio values are lower than typical lidar ratio values for Saharan dust (50–60sr) and comparable to Middle Eastern or west-Asian dust lidar ratios (35–45sr). In contrast, the presented case of pollution aerosol of local origin has an Ångström exponent of 2.07 and a lidar ratio (particle linear depolarization ratio) of 55.8sr (0.03) at 355nm and 32.8sr (0.08) at 532nm wavelength.
- ItemCloud water composition during HCCT-2010: Scavenging efficiencies, solute concentrations, and droplet size dependence of inorganic ions and dissolved organic carbon(München : European Geopyhsical Union, 2016) van Pinxteren, Dominik; Fomba, Khanneh Wadinga; Mertes, Stephan; Müller, Konrad; Spindler, Gerald; Schneider, Johannes; Lee, Taehyoung; Collett, Jeffrey L.; Herrmann, HartmutCloud water samples were taken in September/October 2010 at Mt. Schmücke in a rural, forested area in Germany during the Lagrange-type Hill Cap Cloud Thuringia 2010 (HCCT-2010) cloud experiment. Besides bulk collectors, a three-stage and a five-stage collector were applied and samples were analysed for inorganic ions (SO42−,NO3−, NH4+, Cl−, Na+, Mg2+, Ca2+, K+), H2O2 (aq), S(IV), and dissolved organic carbon (DOC). Campaign volume-weighted mean concentrations were 191, 142, and 39 µmol L−1 for ammonium, nitrate, and sulfate respectively, between 4 and 27 µmol L−1 for minor ions, 5.4 µmol L−1 for H2O2 (aq), 1.9 µmol L−1 for S(IV), and 3.9 mgC L−1 for DOC. The concentrations compare well to more recent European cloud water data from similar sites. On a mass basis, organic material (as DOC × 1.8) contributed 20–40 % (event means) to total solute concentrations and was found to have non-negligible impact on cloud water acidity. Relative standard deviations of major ions were 60–66 % for solute concentrations and 52–80 % for cloud water loadings (CWLs). The similar variability of solute concentrations and CWLs together with the results of back-trajectory analysis and principal component analysis, suggests that concentrations in incoming air masses (i.e. air mass history), rather than cloud liquid water content (LWC), were the main factor controlling bulk solute concentrations for the cloud studied. Droplet effective radius was found to be a somewhat better predictor for cloud water total ionic content (TIC) than LWC, even though no single explanatory variable can fully describe TIC (or solute concentration) variations in a simple functional relation due to the complex processes involved. Bulk concentrations typically agreed within a factor of 2 with co-located measurements of residual particle concentrations sampled by a counterflow virtual impactor (CVI) and analysed by an aerosol mass spectrometer (AMS), with the deviations being mainly caused by systematic differences and limitations of the approaches (such as outgassing of dissolved gases during residual particle sampling). Scavenging efficiencies (SEs) of aerosol constituents were 0.56–0.94, 0.79–0.99, 0.71–98, and 0.67–0.92 for SO42−, NO3−, NH4+, and DOC respectively when calculated as event means with in-cloud data only. SEs estimated using data from an upwind site were substantially different in many cases, revealing the impact of gas-phase uptake (for volatile constituents) and mass losses across Mt. Schmücke likely due to physical processes such as droplet scavenging by trees and/or entrainment. Drop size-resolved cloud water concentrations of major ions SO42−, NO3−, and NH4+ revealed two main profiles: decreasing concentrations with increasing droplet size and “U” shapes. In contrast, profiles of typical coarse particle mode minor ions were often increasing with increasing drop size, highlighting the importance of a species' particle concentration size distribution for the development of size-resolved solute concentration patterns. Concentration differences between droplet size classes were typically < 2 for major ions from the three-stage collector and somewhat more pronounced from the five-stage collector, while they were much larger for minor ions. Due to a better separation of droplet populations, the five-stage collector was capable of resolving some features of solute size dependencies not seen in the three-stage data, especially sharp concentration increases (up to a factor of 5–10) in the smallest droplets for many solutes.
- ItemVariation of CCN activity during new particle formation events in the North China Plain(München : European Geopyhsical Union, 2016) Ma, Nan; Zhao, Chunsheng; Tao, Jiangchuan; Wu, Zhijun; Kecorius, Simonas; Wang, Zhibin; Größ, Johannes; Liu, Hongjian; Bian, Yuxuan; Kuang, Ye; Teich, Monique; Spindler, Gerald; Müller, Konrad; van Pinxteren, Dominik; Herrmann, Hartmut; Hu, Min; Wiedensohler, AlfredThe aim of this investigation was to obtain a better understanding of the variability of the cloud condensation nuclei (CCN) activity during new particle formation (NPF) events in an anthropogenically polluted atmosphere of the North China Plain (NCP). We investigated the size-resolved activation ratio as well as particle number size distribution, hygroscopicity, and volatility during a 4-week intensive field experiment in summertime at a regional atmospheric observatory in Xianghe. Interestingly, based on a case study, two types of NPF events were found, in which the newly formed particles exhibited either a higher or a lower hygroscopicity. Therefore, the CCN activity of newly formed particles in different NPF events was largely different, indicating that a simple parameterization of particle CCN activity during NPF events over the NCP might lead to poor estimates of CCN number concentration (NCCN). For a more accurate estimation of the potential NCCN during NPF events, the variation of CCN activity has to be taken into account. Considering that a fixed activation ratio curve or critical diameter are usually used to calculate NCCN, the influence of the variation of particle CCN activity on the calculation of NCCN during NPF events was evaluated based on the two parameterizations. It was found that NCCN might be underestimated by up to 30 % if a single activation ratio curve (representative of the region and season) were to be used in the calculation; and might be underestimated by up to 50 % if a fixed critical diameter (representative of the region and season) were used. Therefore, we suggest not using a fixed critical diameter in the prediction of NCCN in NPF. If real-time CCN activity data are not available, using a proper fixed activation ratio curve can be an alternative but compromised choice.
- ItemSea salt emission, transport and influence on size-segregated nitrate simulation: A case study in northwestern Europe by WRF-Chem(München : European Geopyhsical Union, 2016) Chen, Ying; Cheng, Yafang; Ma, Nan; Wolke, Ralf; Nordmann, Stephan; Schüttauf, Stephanie; Ran, Liang; Wehner, Birgit; Birmili, Wolfram; van der Gon, Hugo A.C. Denier; Mu, Qing; Barthel, Stefan; Spindler, Gerald; Stieger, Bastian; Müller, Konrad; Zheng, Guang-Jie; Pöschl, Ulrich; Su, Hang; Wiedensohler, AlfredSea salt aerosol (SSA) is one of the major components of primary aerosols and has significant impact on the formation of secondary inorganic particles mass on a global scale. In this study, the fully online coupled WRF-Chem model was utilized to evaluate the SSA emission scheme and its influence on the nitrate simulation in a case study in Europe during 10–20 September 2013. Meteorological conditions near the surface, wind pattern and thermal stratification structure were well reproduced by the model. Nonetheless, the coarse-mode (PM1 − 10) particle mass concentration was substantially overestimated due to the overestimation of SSA and nitrate. Compared to filter measurements at four EMEP stations (coastal stations: Bilthoven, Kollumerwaard and Vredepeel; inland station: Melpitz), the model overestimated SSA concentrations by a factor of 8–20. We found that this overestimation was mainly caused by overestimated SSA emissions over the North Sea during 16–20 September. Over the coastal regions, SSA was injected into the continental free troposphere through an “aloft bridge” (about 500 to 1000 m above the ground), a result of the different thermodynamic properties and planetary boundary layer (PBL) structure between continental and marine regions. The injected SSA was further transported inland and mixed downward to the surface through downdraft and PBL turbulence. This process extended the influence of SSA to a larger downwind region, leading, for example, to an overestimation of SSA at Melpitz, Germany, by a factor of ∼ 20. As a result, the nitrate partitioning fraction (ratio between particulate nitrate and the summation of particulate nitrate and gas-phase nitric acid) increased by about 20 % for the coarse-mode nitrate due to the overestimation of SSA at Melpitz. However, no significant difference in the partitioning fraction for the fine-mode nitrate was found. About 140 % overestimation of the coarse-mode nitrate resulted from the influence of SSA at Melpitz. In contrast, the overestimation of SSA inhibited the nitrate particle formation in the fine mode by about 20 % because of the increased consumption of precursor by coarse-mode nitrate formation.