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    Diurnal variations of ambient particulate wood burning emissions and their contribution to the concentration of Polycyclic Aromatic Hydrocarbons (PAHs) in Seiffen, Germany
    (München : European Geopyhsical Union, 2011) Poulain, L.; Iinuma, Y.; Müller, K.; Birmili, W.; Weinhold, K.; Brüggemann, E.; Gnauk, T.; Hausmann, A.; Löschau, G.; Wiedensohler, A.; Herrmann, H.
    Residential wood burning is becoming an increasingly important cause of air quality problems since it has become a popular source of alternative energy to fossil fuel. In order to characterize the contribution of residential wood burning to local particle pollution, a field campaign was organized at the village of Seiffen (Saxony, Germany). During this campaign, an Aerosol Mass Spectrometer (AMS) was deployed in parallel to a PM1 high volume filter sampler. The AMS mass spectra were analyzed using Positive Matrix Factorization (PMF) to obtain detailed information about the organic aerosol (OA). Biomass-burning organic aerosol (BBOA), Hydrocarbon-like organic aerosol (HOA), and Oxygenated Organic Aerosol (OOA) were identified and represented 20%, 17% and 62% of total OA, respectively. Additionally, Polycyclic Aromatic Hydrocarbons (PAH) were measured by the AMS with an average concentration of 10 ng m−3 and short term events of extremely high PAH concentration (up to 500 ng m−3) compared to the mean PAH value were observed during the whole measurement period. A comparison with the results from PM1 filter samples showed that the BBOA factor and the AMS PAH are good indicators of the total concentration of the different monosaccharide anhydrides and PAH measured on the filter samples. Based on its low correlation with CO and the low car traffic, the HOA factor was considered to be related to residential heating using liquid fuel. An influence of the time of the week (week vs. weekend) on the diurnal profiles of the different OA components was observed. The weekdays were characterized by two maxima; a first one early in the morning and a stronger one in the evening. During the weekend days, the different OA components principally reached only one maximum in the afternoon. Finally, the PAH emitted directly from residential wood combustion was estimated to represent 1.5% of the total mass of the BBOA factor and around 62% of the total PAH concentration measured at Seiffen. This result highlights the important contribution of residential wood combustion to air quality and PAH emissions at the sampling place, which might have a significant impact on human health. Moreover, it also emphasizes the need for a better time resolution of the chemical characterization of toxic particulate compounds in order to provide more information on variations of the different sources through the days as well as to better estimate the real human exposure.
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    Identification and source attribution of organic compounds in ultrafine particles near Frankfurt International Airport
    (Katlenburg-Lindau : European Geosciences Union, 2021) Ungeheuer, Florian; van Pinxteren, Dominik; Vogel, Alexander L.
    Analysing the composition of ambient ultrafine particles (UFPs) is a challenging task due to the low mass and chemical complexity of small particles, yet it is a prerequisite for the identification of particle sources and the assessment of potential health risks. Here, we show the molecular characterization of UFPs, based on cascade impactor (Nano-MOUDI) samples that were collected at an air quality monitoring station near one of Europe's largest airports, in Frankfurt, Germany. At this station, particle-size-distribution measurements show an enhanced number concentration of particles smaller than 50 nm during airport operating hours. We sampled the lower UFP fraction (0.010-0.018, 0.018-0.032, 0.032-0.056 classCombining double low lineinline-formula/m) when the air masses arrived from the airport. We developed an optimized filter extraction procedure using ultra-high-performance liquid chromatography (UHPLC) for compound separation and a heated electrospray ionization (HESI) source with an Orbitrap high-resolution mass spectrometer (HRMS) as a detector for organic compounds. A non-Target screening detected classCombining double low lineinline-formulag1/4200/ organic compounds in the UFP fraction with sample-To-blank ratios larger than 5. We identified the largest signals as homologous series of pentaerythritol esters (PEEs) and trimethylolpropane esters (TMPEs), which are base stocks of aircraft lubrication oils. We unambiguously attribute the majority of detected compounds to jet engine lubrication oils by matching retention times, high-resolution and accurate mass measurements, and comparing tandem mass spectrometry (MS classCombining double low lineinline-formula2/) fragmentation patterns between both ambient samples and commercially available jet oils. For each UFP stage, we created molecular fingerprints to visualize the complex chemical composition of the organic fraction and their average carbon oxidation state. These graphs underline the presence of the homologous series of PEEs and TMPEs and the appearance of jet oil additives (e.g.Tricresyl phosphate, TCP). Targeted screening of TCP confirmed the absence of the harmful tri-iortho/i isomer, while we identified a thermal transformation product of TMPE-based lubrication oil (trimethylolpropane phosphate, TMP-P). Even though a quantitative determination of the identified compounds is limited, the presented method enables the qualitative detection of molecular markers for jet engine lubricants in UFPs and thus strongly improves the source apportionment of UFPs near airports./p. © 2021 BMJ Publishing Group. All rights reserved.
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    Hydroxymethanesulfonic acid in size-segregated aerosol particles at nine sites in Germany
    (München : European Geopyhsical Union, 2014) Scheinhardt, S.; van Pinxteren, D.; Müller, K.; Spindler, G.; Herrmann, H.
    In the course of two field campaigns, size-segregated particle samples were collected at nine sites in Germany, including traffic, urban, rural, marine and mountain sites. During the chemical characterisation of the samples some of them were found to contain an unknown substance that was later identified as hydroxymethanesulfonic acid (HMSA). HMSA is known to be formed during the reaction of S(IV) (HSO3− or SO32−) with formaldehyde in the aqueous phase. Due to its stability, HMSA can act as a reservoir species for S(IV) in the atmosphere and is therefore of interest for the understanding of atmospheric sulfur chemistry. However, no HMSA data are available for atmospheric particles from central Europe, and even on a worldwide scale data are scarce. Thus, the present study now provides a representative data set with detailed information on HMSA concentrations in size-segregated central European aerosol particles. HMSA mass concentrations in this data set were highly variable: HMSA was found in 224 out of 738 samples (30%), sometimes in high mass concentrations exceeding those of oxalic acid. On average over all 154 impactor runs, 31.5 ng m−3 HMSA was found in PM10, contributing 0.21% to the total mass. The results show that the particle diameter, the sampling location, the sampling season and the air mass origin impact the HMSA mass concentration. Highest concentrations were found in the particle fraction 0.42–1.2 μm, at urban sites, in winter and with eastern (continental) air masses, respectively. The results suggest that HMSA is formed during aging of pollution plumes. A positive correlation of HMSA with sulfate, oxalate and PM is found (R2 > 0.4). The results furthermore suggest that the fraction of HMSA in PM slightly decreases with increasing pH.
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    Profiling of fine and coarse particle mass: Case studies of Saharan dust and Eyjafjallajökull/Grimsvötn volcanic plumes
    (München : European Geopyhsical Union, 2012) Ansmann, A.; Seifert, P.; Tesche, M.; Wandinger, U.
    The polarization lidar photometer networking (POLIPHON) method introduced to separate coarse-mode and fine-mode particle properties of Eyjafjallajökull volcanic aerosols in 2010 is extended to cover Saharan dust events as well. Furthermore, new volcanic dust observations performed after the Grimsvötn volcanic eruptions in 2011 are presented. The retrieval of particle mass concentrations requires mass-specific extinction coefficients. Therefore, a review of recently published mass-specific extinction coefficients for Saharan dust and volcanic dust is given. Case studies of four different scenarios corroborate the applicability of the profiling technique: (a) Saharan dust outbreak to central Europe, (b) Saharan dust plume mixed with biomass-burning smoke over Cape Verde, and volcanic aerosol layers originating from (c) the Eyjafjallajökull eruptions in 2010 and (d) the Grimsvötn eruptions in 2011. Strong differences in the vertical aerosol layering, aerosol mixing, and optical properties are observed for the different volcanic events.
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    Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China
    (Katlenburg-Lindau : EGU, 2018) Chen, Jie; Wu, Zhijun; Augustin-Bauditz, Stefanie; Grawe, Sarah; Hartmann, Markus; Pei, Xiangyu; Liu, Zirui; Ji, Dongsheng; Wex, Heike
    Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
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    Analysis of exceedances in the daily PM10 mass concentration (50 μg m−3) at a roadside station in Leipzig, Germany
    (München : European Geopyhsical Union, 2012) Engler, C.; Birmili, W.; Spindler, G.; Wiedensohler, A.
    Five years of PM10 and PM2.5 ambient air measurements at a roadside, an urban, and a regional background site in Leipzig (Germany) were analyzed for violations of the legal PM10 limit value (EC, 1999). The annual mean PM10 concentrations at the three sites were well below the legal threshold of 40 μg m−3 (32.6, 22.0 and 21.7 μg m−3, respectively). At roadside, the daily maximum value of 50 μg m−3 was exceeded on 232 days (13% of all days) in 2005–2009, which led to a violation of the EC directive in three out of five years. We analysed the meteorological factors and local source contributions that eventually led to the exceedances of the daily limit value. As noted in other urban environments before, most exceedance days were observed in the cold season. Exceedance days were most probable under synoptic situations characterised by stagnant winds, low temperatures and strong temperature inversions in winter time. However, these extreme situations accounted for only less than half of the exeedance days. We also noticed a significant number of exceedance days that occurred in the cold season under south-westerly winds, and in the warm season in the presence of easterly winds. Our analysis suggests that local as well as regional sources of PM are equally responsible for exceedances days at the roadside site. The conclusion is that a combined effort of local, national and international reduction measures appears most likely to avoid systematic exceedances of the daily limit value in the future.
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    Aerosol hygroscopicity derived from size-segregated chemical composition and its parameterization in the North China Plain
    (München : European Geopyhsical Union, 2014) Liu, H.J.; Zhao, C.S.; Nekat, B.; Ma, N.; Wiedensohler, A.; van Pinxteren, D.; Spindler, G.; Müller, K.; Herrmann, H.
    Hygroscopic growth of aerosol particles is of significant importance in quantifying the aerosol radiative effect in the atmosphere. In this study, hygroscopic properties of ambient particles are investigated based on particle chemical composition at a suburban site in the North China Plain during the HaChi campaign (Haze in China) in summer 2009. The size-segregated aerosol particulate mass concentration as well as the particle components such as inorganic ions, organic carbon and water-soluble organic carbon (WSOC) are identified from aerosol particle samples collected with a ten-stage impactor. An iterative algorithm is developed to evaluate the hygroscopicity parameter κ from the measured chemical composition of particles. During the HaChi summer campaign, almost half of the mass concentration of particles between 150 nm and 1 μm is contributed by inorganic species. Organic matter (OM) is abundant in ultrafine particles, and 77% of the particulate mass with diameter (Dp) of around 30 nm is composed of OM. A large fraction of coarse particle mass is undetermined and is assumed to be insoluble mineral dust and liquid water. The campaign's average size distribution of κ values shows three distinct modes: a less hygroscopic mode (Dp < 150 nm) with κ slightly above 0.2, a highly hygroscopic mode (150 nm < Dp < 1 μm) with κ greater than 0.3 and a nearly hydrophobic mode (Dp > 1 μm) with κ of about 0.1. The peak of the κ curve appears around 450 nm with a maximum value of 0.35. The derived κ values are consistent with results measured with a high humidity tandem differential mobility analyzer within the size range of 50–250 nm. Inorganics are the predominant species contributing to particle hygroscopicity, especially for particles between 150 nm and 1 μm. For example, NH4NO3, H2SO4, NH4HSO4 and (NH4)2SO4 account for nearly 90% of κ for particles of around 900 nm. For ultrafine particles, WSOC plays a critical role in particle hygroscopicity due to the predominant mass fraction of OM in ultrafine particles. WSOC for particles of around 30 nm contribute 52% of κ. Aerosol hygroscopicity is related to synoptic transport patterns. When southerly wind dominates, particles are more hygroscopic; when northerly wind dominates, particles are less hygroscopic. Aerosol hygroscopicity also has a diurnal variation, which can be explained by the diurnal evolution of planetary boundary layer, photochemical aging processes during daytime and enhanced black carbon emission at night. κ is highly correlated with mass fractions of SO42−, NO3− and NH4+ for all sampled particles as well as with the mass fraction of WSOC for particles of less than 100 nm. A parameterization scheme for κ is developed using mass fractions of SO42−, NO3−, NH4+ and WSOC due to their high correlations with κ, and κ calculated from the parameterization agrees well with κ derived from the particle's chemical composition. Further analysis shows that the parameterization scheme is applicable to other aerosol studies in China.
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    Ion-particle interactions during particle formation and growth at a coniferous forest site in central Europe
    (München : European Geopyhsical Union, 2014) Gonser, S.G.; Klein, F.; Birmili, W.; Größ, J.; Kulmala, M.; Manninen, H.E.; Wiedensohler, A.; Held, A.
    In this work, we examined the interaction of ions and neutral particles during atmospheric new particle formation (NPF) events. The analysis is based on simultaneous field measurements of atmospheric ions and total particles using a neutral cluster and air ion spectrometer (NAIS) across the diameter range 2–25 nm. The Waldstein research site is located in a spruce forest in NE Bavaria, Southern Germany, known for enhanced radon concentrations, presumably leading to elevated ionization rates. Our observations show that the occurrence of the ion nucleation mode preceded that of the total particle nucleation mode during all analyzed NPF events. The time difference between the appearance of 2 nm ions and 2 nm total particles was typically about 20 to 30 min. A cross correlation analysis showed a rapid decrease of the time difference between the ion and total modes during the growth process. Eventually, this time delay vanished when both ions and total particles did grow to larger diameters. Considering the growth rates of ions and total particles separately, total particles exhibited enhanced growth rates at diameters below 15 nm. This observation cannot be explained by condensation or coagulation, because these processes would act more efficiently on charged particles compared to neutral particles. To explain our observations, we propose a mechanism including recombination and attachment of continuously present cluster ions with the ion nucleation mode and the neutral nucleation mode, respectively.
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    Annual variability of ice-nucleating particle concentrations at different Arctic locations
    (Göttingen : Copernicus GmbH, 2019) Wex, H.; Huang, L.; Zhang, W.; Hung, H.; Traversi, R.; Becagli, S.; Sheesley, R.J.; Moffett, C.E.; Barrett, T.E.; Bossi, R.; Skov, H.; Hünerbein, A.; Lubitz, J.; Löffler, M.; Linke, O.; Hartmann, M.; Herenz, P.; Stratmann, F.
    Number concentrations of ice-nucleating particles (NINP) in the Arctic were derived from ground-based filter samples. Examined samples had been collected in Alert (Nunavut, northern Canadian archipelago on Ellesmere Island), Utqiagvik, formerly known as Barrow (Alaska), Nyalesund (Svalbard), and at the Villum Research Station (VRS; northern Greenland). For the former two stations, examined filters span a full yearly cycle. For VRS, 10 weekly samples, mostly from different months of one year, were included. Samples from Ny-Alesund were collected during the months from March until September of one year. At all four stations, highest concentrations were found in the summer months from roughly June to September. For those stations with sufficient data coverage, an annual cycle can be seen. The spectra of NINP observed at the highest temperatures, i.e., those obtained for summer months, showed the presence of INPs that nucleate ice up to-5 °C. Although the nature of these highly ice-active INPs could not be determined in this study, it often has been described in the literature that ice activity observed at such high temperatures originates from the presence of ice-active material of biogenic origin. Spectra observed at the lowest temperatures, i.e., those derived for winter months, were on the lower end of the respective values from the literature on Arctic INPs or INPs from midlatitude continental sites, to which a comparison is presented herein. An analysis concerning the origin of INPs that were ice active at high temperatures was carried out using back trajectories and satellite information. Both terrestrial locations in the Arctic and the adjacent sea were found to be possible source areas for highly active INPs.
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    Atmospheric 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, Wolfram
    This 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.