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Iinuma Y.,Leibniz Institute For Tropospharenforschung Tropos | Keywood M.,CSIRO | Herrmann H.,Leibniz Institute For Tropospharenforschung Tropos
Atmospheric Environment | Year: 2016

Detailed chemical characterisation was performed for wintertime and summertime PM10 samples collected in Melbourne, Australia. The samples were analysed for marker compounds of biomass burning and biogenic secondary organic aerosol (SOA). The chemical analysis showed that the site was significantly influenced by the emissions from wintertime domestic wood combustion and summertime bushfires. Monosaccharide anhydrides were major primary biomass burning marker compounds found in the samples with the average concentrations of 439, 191, 57 and 3630 ngm-3 for winter 2004, winter 2005, summer 2005 and summer 2006, respectively. The highest concentration was determined during the summer 2006 bushfire season with the concentration of 15,400 ngm-3. Biomass burning originating SOA compounds detected in the samples include substituted nitrophenols, mainly 4-nitrocatechol (Mr 155), methyl-nitrocatechols (Mr 169) and dimethyl-nitrocatechols (Mr 183) with the sum concentrations as high as 115 ngm-3 for the wintertime samples and 770 ngm-3 for the bushfire influenced samples. In addition to this, elevated levels of biogenic SOA marker compounds were determined in the summertime samples influence by bushfire smoke. These marker compounds can be categorised into carboxylic acid marker compounds and heteroatomic organic acids containing nitrogen and sulfur. Carboxylic acid marker compounds can be largely attributed to oxidation products originating from 1,8-cineole, α-pinene and β-pinene that are main constituents of eucalyptus VOC emissions. Among those, diaterpenylic acid, terpenylic acid and daterebic acid were found at elevated levels in the bushfire influenced samples. Heteroatomic monoterpene SOA marker compounds (Mr 295, C10H17NO7S) were detected during both winter and summer periods. Especially high levels of these compounds were determined in the severe bushfire samples from summer 2006. Based on the results obtained from the chemical analysis and a macro tracer method, we estimated that 1,8-cineole SOA alone contributed up to 3.5% of secondary organic carbon mass during the bushfire period in 2006. It is likely that biogenic VOC oxidation can be an important source of biomass burning organic aerosol mass. © 2015 Elsevier Ltd. Source


Van Pinxteren D.,Leibniz Institute For Tropospharenforschung Tropos | Neususs C.,Aalen University of Applied Sciences | Herrmann H.,Leibniz Institute For Tropospharenforschung Tropos
Atmospheric Chemistry and Physics | Year: 2014

Dicarboxylic acids (DCAs) are among the most abundant organic compounds observed in atmospheric aerosol particles and have been extensively studied at many places around the world. The importance of the various primary sources and secondary formation pathways discussed in the literature is often difficult to assess from field studies, though. In the present study, a large data set of size-resolved DCA concentrations from several inland sites in Germany is combined with results from a recently developed approach of statistical back-trajectory analysis and additional data. Principal component analysis is then used to reveal the most important factors governing the abundance of DCAs in different particle size ranges. The two most important sources revealed are (i) photochemical formation during intense radiation days in polluted air masses, likely occurring in the gas phase on short timescales (gasSOA), and (ii) secondary reactions in anthropogenically influenced air masses, likely occurring in the aqueous phase on longer timescales (aqSOA). While the first source strongly impacts DCA concentrations mainly in small and large particles, the second one enhances accumulation mode DCAs and is responsible for the bulk of the observed concentrations. Primary sources were found to be minor (sea salt, soil resuspension) or non-existent (biomass burning, traffic). The results can be regarded as representative for typical central European continental conditions. © Author(s) 2014. Source


Gross S.,German Aerospace Center | Freudenthaler V.,Ludwig Maximilians University of Munich | Schepanski K.,Leibniz Institute For Tropospharenforschung Tropos | Toledano C.,University of Valladolid | And 4 more authors.
Atmospheric Chemistry and Physics | Year: 2015

Dual-wavelength Raman and depolarization lidar observations were performed during the Saharan Aerosol Long-range Transport and Aerosol-Cloud interaction Experiment in Barbados in June and July 2013 to characterize the optical properties and vertical distribution of long-range transported Saharan dust after transport across the Atlantic Ocean. Four major dust events were studied during the measurements from 15 June to 13 July 2013 with aerosol optical depths at 532 nm of up to 0.6. The vertical aerosol distribution was characterized by a three-layer structure consisting of the boundary layer, the entrainment or mixing layer and the pure Saharan dust layer. The upper boundary of the pure dust layer reached up to 4.5 km in height. The contribution of the pure dust layer was about half of the total aerosol optical depth at 532 nm. The total dust contribution was about 50-70 % of the total aerosol optical depth at 532 nm. The lidar ratio within the pure dust layer was found to be wavelength independent with mean values of 53 ± 5 sr at 355 nm and 56 ± 7 sr at 532 nm. For the particle linear depolarization ratio, wavelength-independent mean values of 0.26 ± 0.03 at 355 nm and 0.27 ± 0.01 at 532 nm have been found. Source


Van Pinxteren M.,Leibniz Institute For Tropospharenforschung Tropos | Herrmann H.,Leibniz Institute For Tropospharenforschung Tropos
Atmospheric Chemistry and Physics | Year: 2013

An analytical method for the determination of the alpha dicarbonyls glyoxal (GLY) and methylglyoxal (MGLY) from seawater and marine aerosol particles is presented. The method is based on derivatization with o-(2,3,4,5,6- Pentafluorobenzyl)-hydroxylamine (PFBHA) reagent, solvent extraction and GC-MS (SIM) analysis. The method showed good precision (RSD < 10%), sensitivity (detection limits in the low ng L-1 range), and accuracy (good agreement between external calibration and standard addition). The method was applied to determine GLY and MGLY in oceanic water sampled during the Polarstern cruise ANT XXVII/4 from Capetown to Bremerhaven in spring 2011. GLY and MGLY were determined in the sea surface microlayer (SML) of the ocean and corresponding bulk water (BW) with average concentrations of 228 ng L -1 (GLY) and 196 ng L-1 (MGLY). The results show a significant enrichment (factor of 4) of GLY and MGLY in the SML. Furthermore, marine aerosol particles (PM1) were sampled during the cruise and analyzed for GLY (average concentration 0.19 ng m-3) and MGLY (average concentration 0.15 ng m-3). On aerosol particles, both carbonyls show a very good correlation with oxalate, supporting the idea of a secondary formation of oxalic acid via GLY and MGLY. Concentrations of GLY and MGLY in seawater and on aerosol particles were correlated to environmental parameters such as global radiation, temperature, distance to the coastline and biological activity. There are slight hints for a photochemical production of GLY and MGLY in the SML (significant enrichment in the SML, higher enrichment at higher temperature). However, a clear connection of GLY and MGLY to global radiation as well as to biological activity cannot be concluded from the data. A slight correlation between GLY and MGLY in the SML and in aerosol particles could be a hint for interactions, in particular of GLY, between seawater and the atmosphere. © 2013 Author(s). Source


Spindler G.,Leibniz Institute For Tropospharenforschung Tropos | Gruner A.,Leibniz Institute For Tropospharenforschung Tropos | Muller K.,Leibniz Institute For Tropospharenforschung Tropos | Schlimper S.,Deutsche WetterSchutz GmbH | Herrmann H.,Leibniz Institute For Tropospharenforschung Tropos
Journal of Atmospheric Chemistry | Year: 2013

Size-segregated high-volume (HV) quartz filter samples were collected daily at the Melpitz rural site in Germany for PM10 (November 1992 until April 2012), and for PM2.5 and PM1 (January 2003 until April 2012, PM1 sampled every sixth day). The samples were analysed for mass concentration (gravimetrically), water-soluble ions (ion-chromatography) and since 2003 for organic carbon (OC) and elemental carbon (EC) (thermography). The long-term measurements first show a decreasing trend for PM10 (1993-2000) followed by a second period (2001-2011) with a mean mass concentration of about 22.4 μgm-3 and an inter-annual variation of about ± 2.9 μgm-3 (13% fluctuation margin). The absolute sulphate and calcium concentration (for the full period), as well as the EC concentration (time after 2003) decrease by about 50, 75 and 30% for PM10, respectively. The nitrate concentration remains constant all the time. For the daily objective weather type classification (OWTC, 1993-2002) the highest PM10 concentration was found for South-East (SE) and the lowest for North-West (NW) wind direction with 44 and 24 μgm-3, respectively. These concentrations decrease for 2003-2011 in comparison to 1993-2002 by about 21% and 26%, respectively. The highest PM10, PM2.5 and PM1 concentrations (2003-2011) were found for SE and the lowest for NW wind direction with about 34 and 17 μgm-3 (PM10), 28 and 19 μgm-3 (PM2.5) and 22 and 11 μgm-3 (PM1), respectively. The relative content of sulphate, OC and EC was the highest for SE wind direction. A differentiation into four categories for winter (Wi) and summer (Su) and air mass inflow from West (W) and East (E) was carried out. The highest PM concentrations were observed for WiE with the highest inter-annual fluctuation. In this category sulphate contents are largest. The lowest concentrations where found for SuW. The means for WiE show the strongest relative decreases, e.g. in PM10 sulphate (1993-2011) and EC (2003-2011) by about 60% and 40%, respectively. Nitrate is an indicator for NOx motor-car emissions. It shows a typical variation with maximum values in the middle of the week, especially for air mass inflow from West. In contrast, chloride mostly originating from sea spray doesn't show such a concentration pattern. The PM2.5/PM10 as well the PM1/PM 10-ratio have the highest median (0.878 and 0.654) during WiE and the lowest (0.718 and 0.578) during SuW, respectively. For the ratio PM 2.5/PM10 a slightly increasing trend was found (about 0.71 and 0.83 for 1995 and 2011, respectively). The increase is stronger in summer than in winter. © 2013 Springer Science+Business Media Dordrecht. Source

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