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- ItemMeasurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240ma.s.l.) in the Bolivian Andes(Katlenburg-Lindau : EGU, 2023) Scholz, Wiebke; Shen, Jiali; Aliaga, Diego; Wu, Cheng; Carbone, Samara; Moreno, Isabel; Zha, Qiaozhi; Huang, Wei; Heikkinen, Liine; Jaffrezo, Jean Luc; Uzu, Gaelle; Partoll, Eva; Leiminger, Markus; Velarde, Fernando; Laj, Paolo; Ginot, Patrick; Artaxo, Paolo; Wiedensohler, Alfred; Kulmala, Markku; Mohr, Claudia; Andrade, Marcos; Sinclair, Victoria; Bianchi, Federico; Hansel, ArminDimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)2OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000-8000ma.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS-) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance >330km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.
- ItemMutual promotion between aerosol particle liquid water and particulate nitrate enhancement leads to severe nitrate-dominated particulate matter pollution and low visibility(Katlenburg-Lindau : EGU, 2020) Wang, Yu; Chen, Ying; Wu, Zhijun; Shang, Dongjie; Bian, Yuxuan; Du, Zhuofei; Schmitt, Sebastian H.; Su, Rong; Gkatzelis, Georgios I.; Schlag, Patrick; Hohaus, Thorsten; Voliotis, Aristeidis; Lu, Keding; Zeng, Limin; Zhao, Chunsheng; Alfarra, M. Rami; McFiggans, Gordon; Wiedensohler, Alfred; Kiendler-Scharr, Astrid; Zhang, Yuanhang; Hu, MinAs has been the case in North America and western Europe, the SO2 emissions have substantially reduced in the North China Plain (NCP) in recent years. Differential rates of reduction in SO2 and NOx concentrations result in the frequent occurrence of particulate matter pollution dominated by nitrate (pNO−3) over the NCP. In this study, we observed a polluted episode with the particulate nitrate mass fraction in nonrefractory PM1 (NR-PM1) being up to 44 % during wintertime in Beijing. Based on this typical pNO−3-dominated haze event, the linkage between aerosol water uptake and pNO−3 enhancement, further impacting on visibility degradation, has been investigated based on field observations and theoretical calculations. During haze development, as ambient relative humidity (RH) increased from ∼10 % to 70 %, the aerosol particle liquid water increased from ∼1 µg m−3 at the beginning to ∼75 µg m−3 in the fully developed haze period. The aerosol liquid water further increased the aerosol surface area and volume, enhancing the condensational loss of N2O5 over particles. From the beginning to the fully developed haze, the condensational loss of N2O5 increased by a factor of 20 when only considering aerosol surface area and volume of dry particles, while increasing by a factor of 25 when considering extra surface area and volume due to water uptake. Furthermore, aerosol liquid water favored the thermodynamic equilibrium of HNO3 in the particle phase under the supersaturated HNO3 and NH3 in the atmosphere. All the above results demonstrated that pNO−3 is enhanced by aerosol water uptake with elevated ambient RH during haze development, in turn facilitating the aerosol take-up of water due to the hygroscopicity of particulate nitrate salt. Such mutual promotion between aerosol particle liquid water and particulate nitrate enhancement can rapidly degrade air quality and halve visibility within 1 d. Reduction of nitrogen-containing gaseous precursors, e.g., by control of traffic emissions, is essential in mitigating severe haze events in the NCP.
- ItemNo Evidence for a Significant Impact of Heterogeneous Chemistry on Radical Concentrations in the North China Plain in Summer 2014(Columbus, Ohio : American Chemical Society, 2020) Tan, Zhaofeng; Hofzumahaus, Andreas; Lu, Keding; Brown, Steven S.; Holland, Frank; Huey, Lewis Gregory; Kiendler-Scharr, Astrid; Li, Xin; Liu, Xiaoxi; Ma, Nan; Min, Kyung-Eun; Rohrer, Franz; Shao, Min; Wahner, Andreas; Wang, Yuhang; Wiedensohler, Alfred; Wu, Yusheng; Wu, Zhijun; Zeng, Limin; Zhang, Yuanhang; Fuchs, HendrikThe oxidation of nitric oxide to nitrogen dioxide by hydroperoxy (HO2) and organic peroxy radicals (RO2) is responsible for the chemical net ozone production in the troposphere and for the regeneration of hydroxyl radicals, the most important oxidant in the atmosphere. In Summer 2014, a field campaign was conducted in the North China Plain, where increasingly severe ozone pollution has been experienced in the last years. Chemical conditions in the campaign were representative for this area. Radical and trace gas concentrations were measured, allowing for calculating the turnover rates of gas-phase radical reactions. Therefore, the importance of heterogeneous HO2 uptake on aerosol could be experimentally determined. HO2 uptake could have suppressed ozone formation at that time because of the competition with gas-phase reactions that produce ozone. The successful reduction of the aerosol load in the North China Plain in the last years could have led to a significant decrease of HO2 loss on particles, so that ozone-forming reactions could have gained importance in the last years. However, the analysis of the measured radical budget in this campaign shows that HO2 aerosol uptake did not impact radical chemistry for chemical conditions in 2014. Therefore, reduced HO2 uptake on aerosol since then is likely not the reason for the increasing number of ozone pollution events in the North China Plain, contradicting conclusions made from model calculations reported in the literature. © 2020 American Chemical Society.
- 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.
- ItemDecreasing trends of particle number and black carbon mass concentrations at 16 observational sites in Germany from 2009 to 2018(Katlenburg-Lindau : EGU, 2020) Sun, Jia; Birmili, Wolfram; Hermann, Markus; Tuch, Thomas; Weinhold, Kay; Merkel, Maik; Rasch, Fabian; Müller, Thomas; Schladitz, Alexander; Bastian, Susanne; Löschau, Gunter; Cyrys, Josef; Gu, Jianwei; Flentje, Harald; Briel, Björn; Asbach, Christoph; Kaminski, Heinz; Ries, Ludwig; Sohmer, Ralf; Gerwig, Holger; Wirtz, Klaus; Meinhardt, Frank; Schwerin, Andreas; Bath, Olaf; Ma, Nan; Wiedensohler, AlfredAnthropogenic emissions are dominant contributors to air pollution. Consequently, mitigation policies have been attempted since the 1990s in Europe to reduce pollution by anthropogenic emissions. To evaluate the effectiveness of these mitigation policies, the German Ultrafine Aerosol Network (GUAN) was established in 2008, focusing on black carbon (BC) and sub-micrometre aerosol particles. In this study, long-term trends of atmospheric particle number concentrations (PNCs) and equivalent BC (eBC) mass concentration over a 10-year period (2009-2018) were determined for 16 GUAN sites ranging from roadside to high Alpine environments. Overall, statistically significant decreasing trends are found for most of these parameters and environments in Germany. The annual relative slope of eBC mass concentration varies between-13.1% and-1.7% per year. The slopes of the PNCs vary from-17.2% to-1.7 %,-7.8% to-1.1 %, and-11.1% to-1.2% per year for 10-30, 30-200, and 200-800 nm size ranges, respectively. The reductions in various anthropogenic emissions are found to be the dominant factors responsible for the decreasing trends of eBC mass concentration and PNCs. The diurnal and seasonal variations in the trends clearly show the effects of the mitigation policies for road transport and residential emissions. The influences of other factors such as air masses, precipitation, and temperature were also examined and found to be less important or negligible. This study proves that a combination of emission mitigation policies can effectively improve the air quality on large spatial scales. It also suggests that a long-term aerosol measurement network at multi-type sites is an efficient and necessary tool for evaluating emission mitigation policies. © 2020 Author(s).
- ItemAssociations between air temperature and cardio-respiratory mortality in the urban area of Beijing, China: a time-series analysis(London : BioMed Central, 2011) Liu, Liqun; Breitner, Susanne; Pan, Xiaochuan; Franck, Ulrich; Leitte, Arne Marian; Wiedensohler, Alfred; von Klot, Stephanie; Wichmann, H-Erich; Peters, Annette; Schneider, AlexandraBackground: Associations between air temperature and mortality have been consistently observed in Europe and the United States; however, there is a lack of studies for Asian countries. Our study investigated the association between air temperature and cardio-respiratory mortality in the urban area of Beijing, China. Methods: Death counts for cardiovascular and respiratory diseases for adult residents (≥15 years), meteorological parameters and concentrations of particulate air pollution were obtained from January 2003 to August 2005. The effects of two-day and 15-day average temperatures were estimated by Poisson regression models, controlling for time trend, relative humidity and other confounders if necessary. Effects were explored for warm (April to September) and cold periods (October to March) separately. The lagged effects of daily temperature were investigated by polynomial distributed lag (PDL) models. Results: We observed a J-shaped exposure-response function only for 15-day average temperature and respiratory mortality in the warm period, with 21.3°C as the threshold temperature. All other exposure-response functions could be considered as linear. In the warm period, a 5°C increase of two-day average temperature was associated with a RR of 1.098 (95% confidence interval (95%CI): 1.057-1.140) for cardiovascular and 1.134 (95%CI: 1.050-1.224) for respiratory mortality; a 5°C decrease of 15-day average temperature was associated with a RR of 1.040 (95%CI: 0.990-1.093) for cardiovascular mortality. In the cold period, a 5°C increase of two-day average temperature was associated with a RR of 1.149 (95%CI: 1.078-1.224) for respiratory mortality; a 5°C decrease of 15-day average temperature was associated with a RR of 1.057 (95%CI: 1.022-1.094) for cardiovascular mortality. The effects remained robust after considering particles as additional confounders. Conclusions: Both increases and decreases in air temperature are associated with an increased risk of cardiovascular mortality. The effects of heat were immediate while the ones of cold became predominant with longer time lags. Increases in air temperature are also associated with an immediate increased risk of respiratory mortality.
- ItemCloud condensation nuclei spectra derived from size distributions and hygroscopic properties of the aerosol in coastal south-west Portugal during ACE-2(Milton Park : Taylor & Francis, 2016) Dusek, Ulrike; Covert, David S.; Wiedensohler, Alfred; Neusüss, Christian; Weise, Diana; Cantrell, WillIn this work we propose and test a method to calculate cloud condensation nuclei (CCN) spectra basedon aerosol number size distributions and hygroscopic growth factors. Sensitivity studies show thatthis method can be used in a wide variety of conditions except when the aerosol consist mainly oforganic compounds. One crucial step in the calculations, estimating soluble ions in an aerosol particlebased on hygroscopic growth factors, is tested in an internal hygroscopic consistency study. The resultsshow that during the second Aerosol Characterization Experiment (ACE-2) the number concentrationof inorganic ions analyzed in impactor samples could be reproduced from measured growth factorswithin the measurement uncertainties at the measurement site in Sagres, Portugal. CCN spectra were calculated based on data from the ACE-2 field experiment at the Sagres site.The calculations overestimate measured CCN spectra on average by approximately 30%, which iscomparable to the uncertainties in measurements and calculations at supersaturations below 0.5%. Thecalculated CCN spectra were averaged over time periods when Sagres received clean air masses and airmasses influenced by aged and recent pollution. Pollution outbreaks enhance the CCN concentrationsat supersaturations near 0.2% by a factor of 3 (aged pollution) to 5 (recent pollution) compared to theclean marine background concentrations. In polluted air masses, the shape of the CCN spectra changes.The clean spectra can be approximated by a power function, whereas the polluted spectra are betterapproximated by an error function.