7 results
Search Results
Now showing 1 - 7 of 7
- ItemLong-term measurements of aerosol and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian taiga(München : European Geopyhsical Union, 2013) Chi, X.; Winderlich, J.; Mayer, J.-C.; Panov, A.V.; Heimann, M.; Birmili, W.; Heintzenberg, J.; Cheng, Y.; Andreae, M.O.Siberia is one of few continental regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine background conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September 2006 and December 2011 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, such as equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted from near-pristine air masses, providing quantitative characteristics for each type. Depending on the season, 23–36% of the sampling time at ZOTTO was found to be representative of a clean atmosphere. The summer pristine data indicate that primary biogenic and secondary organic aerosol formation are quite strong particle sources in the Siberian taiga. The summer seasons 2007–2008 were dominated by an Aitken mode around 80 nm size, whereas the summer 2009 with prevailing easterly winds produced particles in the accumulation mode around 200 nm size. We found these differences to be mainly related to air temperature, through its effect on the production rates of biogenic volatile organic compounds (VOC) precursor gases. In winter, the particle size distribution peaked at 160 nm, and the footprint of clean background air was characteristic for aged particles from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from domestic heating. The wintertime polluted air originates mainly from large cities south and southwest of the site; these particles have a dominant mode around 100 nm, and the ΔBCe / ΔCO ratio of 7–11 ng m−3 ppb−1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution particles at ZOTTO, while only 12% of the polluted events are classified as biomass-burning-dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different ΔBCe / ΔCO ratios from different fire types, with the agricultural fires in April~2008 yielding a very high ratio of 21 ng m−3 ppb−1. Overall, we find that anthropogenic sources dominate the aerosol population at ZOTTO most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only in the growing season and then only episodically.
- ItemCloud condensation nuclei in polluted air and biomass burning smoke near the mega-city Guangzhou, China – Part 2: Size-resolved aerosol chemical composition, diurnal cycles, and externally mixed weakly CCN-active soot particles(München : European Geopyhsical Union, 2011) Rose, D.; Gunthe, S.S.; Su, H.; Garland, R.M.; Yang, H.; Berghof, M.; Cheng, Y.F.; Wehner, B.; Achtert, P.; Nowak, A.; Wiedensohler, A.; Takegawa, N.; Kondo, Y.; Hu, M.; Zhang, Y.; Andreae, M.O.; Pöschl, U.Size-resolved chemical composition, mixing state, and cloud condensation nucleus (CCN) activity of aerosol particles in polluted mega-city air and biomass burning smoke were measured during the PRIDE-PRD2006 campaign near Guangzhou, China, using an aerosol mass spectrometer (AMS), a volatility tandem differential mobility analyzer (VTDMA), and a continuous-flow CCN counter (DMT-CCNC). The size-dependence and temporal variations of the effective average hygroscopicity parameter for CCN-active particles (κa) could be parameterized as a function of organic and inorganic mass fractions (forg, finorg) determined by the AMS: κa,p=κorg·forg + κinorg·finorg. The characteristic κ values of organic and inorganic components were similar to those observed in other continental regions of the world: κorg≈0.1 and κinorg≈0.6. The campaign average κa values increased with particle size from ~0.25 at ~50 nm to ~0.4 at ~200 nm, while forg decreased with particle size. At ~50 nm, forg was on average 60% and increased to almost 100% during a biomass burning event. The VTDMA results and complementary aerosol optical data suggest that the large fractions of CCN-inactive particles observed at low supersaturations (up to 60% at S≤0.27%) were externally mixed weakly CCN-active soot particles with low volatility (diameter reduction <5% at 300 °C) and effective hygroscopicity parameters around κLV≈0.01. A proxy for the effective average hygroscopicity of the total ensemble of CCN-active particles including weakly CCN-active particles (κt) could be parameterized as a function of κa,p and the number fraction of low volatility particles determined by VTDMA (φLV): κt,p=κa,p−φLV·(κa,p−κLV). Based on κ values derived from AMS and VTDMA data, the observed CCN number concentrations (NCCN,S≈102–104 cm−3 at S = 0.068–0.47%) could be efficiently predicted from the measured particle number size distribution. The mean relative deviations between observed and predicted CCN concentrations were ~10% when using κt,p, and they increased to ~20% when using only κa,p. The mean relative deviations were not higher (~20%) when using an approximate continental average value of κ≈0.3, although the constant κ value cannot account for the observed temporal variations in particle composition and mixing state (diurnal cycles and biomass burning events). Overall, the results confirm that on a global and climate modeling scale an average value of κ≈0.3 can be used for approximate predictions of CCN number concentrations in continental boundary layer air when aerosol size distribution data are available without information about chemical composition. Bulk or size-resolved data on aerosol chemical composition enable improved CCN predictions resolving regional and temporal variations, but the composition data need to be highly accurate and complemented by information about particle mixing state to achieve high precision (relative deviations <20%).
- ItemLong-term in situ observations of biomass burning aerosol at a high altitude station in Venezuela – Sources, impacts and interannual variability(München : European Geopyhsical Union, 2013) Hamburger, T.; Matisāns, M.; Tunved, P.; Ström, J.; Calderon, S.; Hoffmann, P.; Hochschild, G.; Gross, J.; Schmeissner, T.; Wiedensohler, A.; Krejci, R.First long-term observations of South American biomass burning aerosol within the tropical lower free troposphere are presented. The observations were conducted between 2007 and 2009 at a high altitude station (4765 m a.s.l.) on the Pico Espejo, Venezuela. Sub-micron particle volume, number concentrations of primary particles and particle absorption were observed. Orographic lifting and shallow convection leads to a distinct diurnal cycle at the station. It enables measurements within the lower free troposphere during night-time and observations of boundary layer air masses during daytime and at their transitional regions. The seasonal cycle is defined by a wet rainy season and a dry biomass burning season. The particle load of biomass burning aerosol is dominated by fires in the Venezuelan savannah. Increases of aerosol concentrations could not be linked to long-range transport of biomass burning plumes from the Amazon basin or Africa due to effective wet scavenging of particles. Highest particle concentrations were observed within boundary layer air masses during the dry season. Ambient sub-micron particle volume reached 1.4±1.3 μm3 cm−3, refractory particle number concentrations (at 300 °C) 510±420 cm−3 and the absorption coefficient 0.91±1.2 Mm−1. The respective concentrations were lowest within the lower free troposphere during the wet season and averaged at 0.19±0.25 μm3 cm−3, 150±94 cm−3 and 0.15±0.26 Mm−1. A decrease of particle concentrations during the dry seasons from 2007–2009 could be connected to a decrease in fire activity in the wider region of Venezuela using MODIS satellite observations. The variability of biomass burning is most likely linked to the El Niño–Southern Oscillation (ENSO). Low biomass burning activity in the Venezuelan savannah was observed to follow La Niña conditions, high biomass burning activity followed El Niño conditions.
- ItemWater uptake by biomass burning aerosol at sub- and supersaturated conditions: closure studies and implications for the role of organics(München : European Geopyhsical Union, 2011) Dusek, U.; Frank, G.P.; Massling, A.; Zeromskiene, K.; Iinuma, Y.; Schmid, O.; Helas, G.; Hennig, T.; Wiedensohler, A.; Andreae, M.O.We investigate the CCN activity of freshly emitted biomass burning particles and their hygroscopic growth at a relative humidity (RH) of 85%. The particles were produced in the Mainz combustion laboratory by controlled burning of various wood types. The water uptake at sub- and supersaturations is parameterized by the hygroscopicity parameter, κ (c.f. Petters and Kreidenweis, 2007). For the wood burns, κ is low, generally around 0.06. The main emphasis of this study is a comparison of κ derived from measurements at sub- and supersaturated conditions (κG and κCCN), in order to see whether the water uptake at 85% RH can predict the CCN properties of the biomass burning particles. Differences in κGand κCCN can arise through solution non-idealities, the presence of slightly soluble or surface active compounds, or non-spherical particle shape. We find that κG and κCCN agree within experimental uncertainties (of around 30%) for particle sizes of 100 and 150 nm; only for 50 nm particles is κCCN larger than κG by a factor of 2. The magnitude of this difference and its dependence on particle size is consistent with the presence of surface active organic compounds. These compounds mainly facilitate the CCN activation of small particles, which form the most concentrated solution droplets at the point of activation. The 50 nm particles, however, are only activated at supersaturations higher than 1% and are therefore of minor importance as CCN in ambient clouds. By comparison with the actual chemical composition of the biomass burning particles, we estimate that the hygroscopicity of the water-soluble organic carbon (WSOC) fraction can be represented by a κWSOC value of approximately 0.2. The effective hygroscopicity of a typical wood burning particle can therefore be represented by a linear mixture of an inorganic component with κ ≅ 0.6, a WSOC component with κ ≅ 0.2, and an insoluble component with κ = 0.
- ItemSize distributions of polycyclic aromatic hydrocarbons in urban atmosphere: Sorption mechanism and source contributions to respiratory deposition(München : European Geopyhsical Union, 2016) Lv, Yan; Li, Xiang; Xu, Ting Ting; Cheng, Tian Tao; Yang, Xin; Chen, Jian Min; Iinuma, Yoshiteru; Herrmann, HartmutIn order to better understand the particle size distribution of polycyclic aromatic hydrocarbons (PAHs) and their source contribution to human respiratory system, size-resolved PAHs have been studied in ambient aerosols at a megacity Shanghai site during a 1-year period (2012–2013). The results showed the PAHs had a bimodal distribution with one mode peak in the fine-particle size range (0.4–2.1 µm) and another mode peak in the coarse-particle size range (3.3–9.0 µm). Along with the increase in ring number of PAHs, the intensity of the fine-mode peak increased, while the coarse-mode peak decreased. Plotting of log(PAH / PM) against log(Dp) showed that all slope values were above −1, suggesting that multiple mechanisms (adsorption and absorption) controlled the particle size distribution of PAHs. The total deposition flux of PAHs in the respiratory tract was calculated as being 8.8 ± 2.0 ng h−1. The highest lifetime cancer risk (LCR) was estimated at 1.5 × 10−6, which exceeded the unit risk of 10−6. The LCR values presented here were mainly influenced by accumulation mode PAHs which came from biomass burning (24 %), coal combustion (25 %), and vehicular emission (27 %). The present study provides us with a mechanistic understanding of the particle size distribution of PAHs and their transport in the human respiratory system, which can help develop better source control strategies.
- ItemOptical and microphysical properties of smoke over Cape Verde inferred from multiwavelength lidar measurements(Milton Park : Taylor & Francis, 2017) Tesche, Matthias; Müller, Detlef; Gross, Silke; Ansmann, Albert; Althausen, Dietrich; Freudenthaler, Volker; Weinzierl, Bernadett; Veira, Andreas; Petzold, AndreasLidar measurements of mixed dust/smoke plumes over the tropical Atlantic ocean were carried out during the winter campaign of SAMUM-2 at Cape Verde. Profiles of backscatter and extinction coefficients, lidar ratios, and Ångstr¨om exponents related to pure biomass-burning aerosol from southern West Africa were extracted from these observations. Furthermore, these findings were used as input for an inversion algorithm to retrieve microphysical properties of pure smoke. Seven measurement days were found suitable for the procedure of aerosol-type separation and successive inversion of optical data that describe biomass-burning smoke. We inferred high smoke lidar ratios of 87 ± 17 sr at 355 nm and 79 ± 17 sr at 532 nm. Smoke lidar ratios and Ångstr¨om exponents are higher compared to the ones for the dust/smoke mixture. These numbers indicate higher absorption and smaller sizes for pure smoke particles compared to the dust/smoke mixture. Inversion of the smoke data set results in mean effective radii of 0.22 ± 0.08 μm with individual results varying between 0.10 and 0.36 μm. The single-scattering albedo for pure biomass-burning smoke was found to vary between 0.63 and 0.89 with a very low mean value of 0.75 ± 0.07. This is in good agreement with findings of airborne in situ measurements which showed values of 0.77 ± 0.03. Effective radii from the inversion were similar to the ones found for the fine mode of the in situ size distributions.
- ItemSaharan Mineral Dust Experiments SAMUM-1 and SAMUM-2: What have we learned?(Milton Park : Taylor & Francis, 2011) Ansmann, Albert; Petzold, Andreas; Kandler, Konrad; Tegen, Ina; Wendisch, Manfred; Müller, Detlef; Weinzierl, Bernadett; Müller, Thomas; Heintzenberg, JostTwo comprehensive field campaigns were conducted in 2006 and 2008 in the framework of the Saharan Mineral Dust Experiment (SAMUM) project. The relationship between chemical composition, shape morphology, size distribution and optical effects of the dust particles was investigated. The impact of Saharan dust on radiative transfer and the feedback of radiative effects upon dust emission and aerosol transport were studied. Field observations (ground-based, airborne and remote sensing) and modelling results were compared within a variety of dust closure experiments with a strong focus on vertical profiling. For the first time, multiwavelength Raman/polarization lidars and an airborne high spectral resolution lidar were involved in major dust field campaigns and provided profiles of the volume extinction coefficient of the particles at ambient conditions (for the full dust size distribution), of particle-shape-sensitive optical properties at several wavelengths, and a clear separation of dust and smoke profiles allowing for an estimation of the single-scattering albedo of the biomass-burning aerosol. SAMUM–1 took place in southern Morocco close to the Saharan desert in the summer of 2006, whereas SAMUM–2 was conducted in Cape Verde in the outflow region of desert dust and biomass-burning smoke from western Africa in the winter of 2008. This paper gives an overview of the SAMUM concept, strategy and goals, provides snapshots (highlights) of SAMUM–2 observations and modelling efforts, summarizes main findings of SAMUM–1 and SAMUM–2 and finally presents a list of remaining problems and unsolved questions.