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- ItemA new method to measure real-world respiratory tract deposition of inhaled ambient black carbon(Amsterdam [u.a.] : Elsevier Science, 2019) Madueño, Leizel; Kecorius, Simonas; Löndahl, Jakob; Müller, Thomas; Pfeifer, Sascha; Haudek, Andrea; Mardoñez, Valeria; Wiedensohler, AlfredIn this study, we present the development of a mobile system to measure real-world total respiratory tract deposition of inhaled ambient black carbon (BC). Such information can be used to supplement the existing knowledge on air pollution-related health effects, especially in the regions where the use of standard methods and intricate instrumentation is limited. The study is divided in two parts. Firstly, we present the design of portable system and methodology to evaluate the exhaled air BC content. We demonstrate that under real-world conditions, the proposed system exhibit negligible particle losses, and can additionally be used to determine the minute ventilation. Secondly, exemplary experimental data from the system is presented. A feasibility study was conducted in the city of La Paz, Bolivia. In a pilot experiment, we found that the cumulative total respiratory tract deposition dose over 1-h commuting trip would result in approximately 2.6 μg of BC. This is up to 5 times lower than the values obtained from conjectural approach (e.g. using physical parameters from previously reported worksheets). Measured total respiratory tract deposited BC fraction varied from 39% to 48% during walking and commuting inside a micro-bus, respectively. To the best of our knowledge, no studies focusing on experimental determination of real-world deposition dose of BC have been performed in developing regions. This can be especially important because the BC mass concentration is significant and determines a large fraction of particle mass concentration. In this work, we propose a potential method, recommendations, as well as the limitations in establishing an easy and relatively cheap way to estimate the respiratory tract deposition of BC. In this study we present a novel method to measure real-world respiratory tract deposition dose of Black Carbon. Results from a pilot study in La Paz, Bolivia, are presented. © 2019 The Authors
- ItemPreventing airborne transmission of SARS-CoV-2 in hospitals and nursing homes(Basel : MDPI AG, 2020) Ahlawat, Ajit; Mishra, Sumit Kumar; Birks, John W.; Costabile, Francesca; Wiedensohler, Alfred[No abstract available]
- ItemPhysico-Chemical Properties and Deposition Potential of PM2.5 during Severe Smog Event in Delhi, India(Basel : MDPI AG, 2022) Fatima, Sadaf; Mishra, Sumit Kumar; Ahlawat, Ajit; Dimri, Ashok PriyadarshanThe present work studies a severe smog event that occurred in Delhi (India) in 2017, targeting the characterization of PM2.5 and its deposition potential in human respiratory tract of different population groups in which the PM2.5 levels raised from 124.0 µg/m3 (pre-smog period) to 717.2 µg/m3 (during smog period). Higher concentration of elements such as C, N, O, Na, Mg, Al, Si, S, Fe, Cl, Ca, Ti, Cr, Pb, Fe, K, Cu, Cl, P, and F were observed during the smog along with dominant organic functional groups (aldehyde, ketones, alkyl halides (R-F; R-Br; R-Cl), ether, etc.), which supported potential contribution from transboundary biomass-burning activities along with local pollution sources and favorable meteorological conditions. The morphology of individual particles were found mostly as non-spherical, including carbon fractals, aggregates, sharp-edged, rod-shaped, and flaky structures. A multiple path particle dosimetry (MPPD) model showed significant deposition potential of PM2.5 in terms of deposition fraction, mass rate, and mass flux during smog conditions in all age groups. The highest PM2.5 deposition fraction and mass rate were found for the head region followed by the alveolar region of the human respiratory tract. The highest mass flux was reported for 21-month-old (4.7 × 102 µg/min/m2), followed by 3-month-old (49.2 µg/min/m2) children, whereas it was lowest for 21-year-old adults (6.8 µg/min/m2), indicating babies and children were more vulnerable to PM2.5 pollution than adults during smog. Deposition doses of toxic elements such as Cr, Fe, Zn, Pb, Cu, Mn, and Ni were also found to be higher (up to 1 × 10−7 µg/kg/day) for children than adults.
- ItemLong-term trends of black carbon and particle number concentration in the lower free troposphere in Central Europe(Berlin ; Heidelberg : Springer, 2021) Sun, Jia; Hermann, Markus; Yuan, Ye; Birmili, Wolfram; Collaud Coen, Martine; Weinhold, Kay; Madueño, Leizel; Poulain, Laurent; Tuch, Thomas; Ries, Ludwig; Sohmer, Ralf; Couret, Cedric; Frank, Gabriele; Brem, Benjamin Tobias; Gysel-Beer, Martin; Ma, Nan; Wiedensohler, AlfredBackground: The implementation of emission mitigation policies in Europe over the last two decades has generally improved the air quality, which resulted in lower aerosol particle mass, particle number, and black carbon mass concentration. However, little is known whether the decreasing particle concentrations at a lower-altitude level can be observed in the free troposphere (FT), an important layer of the atmosphere, where aerosol particles have a longer lifetime and may affect climate dynamics. In this study, we used data from two high-Alpine observatories, Zugspitze-Schneefernerhaus (ZSF) and Jungfraujoch (JFJ), to assess the long-term trends on size-resolved particle number concentrations (PNCs) and equivalent black carbon (eBC) mass concentration separated for undisturbed lower FT conditions and under the influence of air from the planetary boundary layer (PBL) from 2009 to 2018. Results: The FT and PBL-influenced conditions were segregated for both sites. We found that the FT conditions in cold months were more prevalent than in warm months, while the measured aerosol parameters showed different seasonal patterns for the FT and PBL-influenced conditions. The pollutants in the PBL-influenced condition have a higher chance to be transported to high-altitudes due to the mountainous topography, leading to a higher concentration and more distinct seasonal variation, and vice versa. The long-term trends of the measured aerosol parameters were evaluated and the decreased aerosol concentrations were observed for both FT and PBL-influenced conditions. The observed decreasing trends in eBC concentration in the PBL-influenced condition are well consistent with the reported trends in total BC emission in Germany and Switzerland. The decreased concentrations in the FT condition suggest that the background aerosol concentration in the lower FT over Central Europe has correspondingly decreased. The change of back trajectories in the FT condition at ZSF and JFJ was further evaluated to investigate the other possible drivers for the decreasing trends. Conclusions: The background aerosol concentration in the lower FT over Central Europe has significantly decreased during 2009–2018. The implementation of emission mitigation policies is the most decisive factor and the decrease of the regional airmass occurrence over Central Europe also has contributed to the decreasing trends. © 2021, The Author(s).
- ItemThe impact of COVID-19 lockdown measures on the Indian summer monsoon(Bristol : IOP Publ., 2021-7-16) Fadnavis, Suvarna; Sabin, T. P.; Rap, Alexandru; Müller, Rolf; Kubin, Anne; Heinold, BerndAerosol concentrations over Asia play a key role in modulating the Indian summer monsoon (ISM) rainfall. Lockdown measures imposed to prevent the spread of the COVID-19 pandemic led to substantial reductions in observed Asian aerosol loadings. Here, we use bottom-up estimates of anthropogenic emissions based on national mobility data from Google and Apple, along with simulations from the ECHAM6-HAMMOZ state-of-the-art aerosol-chemistry-climate model to investigate the impact of the reduced aerosol and gases pollution loadings on the ISM. We show that the decrease in anthropogenic emissions led to a 4 W m−2 increase in surface solar radiation over parts of South Asia, which resulted in a strengthening of the ISM. Simultaneously, while natural emission parameterizations are kept the same in all our simulations, the anthropogenic emission reduction led to changes in the atmospheric circulation, causing accumulation of dust over the Tibetan plateau (TP) during the pre-monsoon and monsoon seasons. This accumulated dust has intensified the warm core over the TP that reinforced the intensification of the Hadley circulation. The associated cross-equatorial moisture influx over the Indian landmass led to an enhanced amount of rainfall by 4% (0.2 mm d−1) over the Indian landmass and 5%–15% (0.8–3 mm d−1) over central India. These estimates may vary under the influence of large-scale coupled atmosphere–ocean oscillations (e.g. El Nino Southern Oscillation, Indian Ocean Dipole). Our study indicates that the reduced anthropogenic emissions caused by the unprecedented COVID-19 restrictions had a favourable effect on the hydrological cycle over South Asia, which has been facing water scarcity during the past decades. This emphasizes the need for stringent measures to limit future anthropogenic emissions in South Asia for protecting one of the world's most densely populated regions.
- ItemParticle number emission rates of aerosol sources in 40 German households and their contributions to ultrafine and fine particle exposure(Oxford : Wiley-Blackwell, 2020) Zhao, Jiangyue; Birmili, Wolfram; Hussein, Tareq; Wehner, Birgit; Wiedensohler, AlfredMore representative data on source-specific particle number emission rates and associated exposure in European households are needed. In this study, indoor and outdoor particle number size distributions (10–800 nm) were measured in 40 German households under real-use conditions in over 500 days. Particle number emission rates were derived for around 800 reported indoor source events. The highest emission rate was caused by burning candles (5.3 × 1013 h−1). Data were analyzed by the single-parameter approach (SPA) and the indoor aerosol dynamics model approach (IAM). Due to the consideration of particle deposition, coagulation, and time-dependent ventilation rates, the emission rates of the IAM approach were about twice as high as those of the SPA. Correction factors are proposed to convert the emission rates obtained from the SPA approach into more realistic values. Overall, indoor sources contributed ~ 56% of the daily-integrated particle number exposure in households under study. Burning candles and opening the window leads to seasonal differences in the contributions of indoor sources to residential exposure (70% and 40% in the cold and warm season, respectively). Application of the IAM approach allowed to attribute the contributions of outdoor particles to the penetration through building shell and entry through open windows (26% and 15%, respectively). © 2020 John Wiley & Sons A/S. Published by John Wiley & Sons Ltd
- ItemInfrequent new particle formation over the remote boreal forest of Siberia(Amsterdam [u.a.] : Elsevier Science, 2018) Wiedensohler, A.; Ma, N.; Birmili, W.; Heintzenberg, J.; Ditas, F.; Andreae, M.O.; Panov, A.Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Ltd
- ItemDetection of RO2 radicals and other products from cyclohexene ozonolysis with NH4+ and acetate chemical ionization mass spectrometry(Oxford [u.a.] : Elsevier, 2018) Hansel, Armin; Scholz, Wiebke; Mentler, Bernhard; Fischer, Lukas; Berndt, TorstenThe performance of the novel ammonium chemical ionization time of flight mass spectrometer (NH4+-CI3–TOF) utilizing NH4+ adduct ion chemistry to measure first generation oxidized product molecules (OMs) as well as highly oxidized organic molecules (HOMs) was investigated for the first time. The gas-phase ozonolysis of cyclohexene served as a first test system. Experiments have been carried out in the TROPOS free-jet flow system at close to atmospheric conditions. Product ion signals were simultaneously observed by the NH4+-CI3-TOF and the acetate chemical ionization atmospheric pressure interface time of flight mass spectrometer (acetate-CI-API-TOF). Both instruments are in remarkable good agreement within a factor of two for HOMs. For OMs not containing an OOH group the acetate technique can considerably underestimate OM concentrations by 2–3 orders of magnitude. First steps of cyclohexene ozonolysis generate ten different main products, detected with the ammonium-CI3-TOF, comprising 93% of observed OMs. The remaining 7% are distributed over several minor products that can be attributed to HOMs, predominately to highly oxidized RO2 radicals. Summing up, observed ammonium-CI3-TOF products yield 5.6 × 109 molecules cm−³ in excellent agreement with the amount of reacted cyclohexene of 4.5 × 109 molecules cm−³ for reactant concentrations of [O3] = 2.25 × 1012 molecules cm−³ and [cyclohexene] = 2.0 × 1012 molecules cm−³ and a reaction time of 7.9 s. NH4+ adduct ion chemistry is a promising CIMS technology for achieving carbon-closure due to the unique opportunity for complete detection of the whole product distribution including also peroxy radicals, and consequently, for a much better understanding of oxidation processes.
- ItemBlack carbon emission and transport mechanisms to the free troposphere at the La Paz/El Alto (Bolivia) metropolitan area based on the Day of Census (2012)(Oxford [u.a.] : Elsevier, 2018) Wiedensohler, A.; Andrade, M.; Weinhold, K.; Müller, T.; Birmili, W.; Velarde, F.; Moreno, I.; Forno, R.; Sanchez, M.F.; Laj, P.; Ginot, P.; Whiteman, D.N.; Krejci, R.; Sellegri, K.; Reichler, T.Urban development, growing industrialization, and increasing demand for mobility have led to elevated levels of air pollution in many large cities in Latin America, where air quality standards and WHO guidelines are frequently exceeded. The conurbation of the metropolitan area of La Paz/El Alto is one of the fastest growing urban settlements in South America with the particularity of being located in a very complex terrain at a high altitude. As many large cities or metropolitan areas, the metropolitan area of La Paz/El Alto and the Altiplano region are facing air quality deterioration. Long-term measurement data of the equivalent black carbon (eBC) mass concentrations and particle number size distributions (PNSD) from the Global Atmosphere Watch Observatory Chacaltaya (CHC; 5240 m a.s.l., above sea level) indicated a systematic transport of particle matter from the metropolitan area of La Paz/El Alto to this high altitude station and subsequently to the lower free troposphere. To better understand the sources and the transport mechanisms, we conducted eBC and PNSDs measurements during an intensive campaign at two locations in the urban area of La Paz/El Alto from September to November 2012. While the airport of El Alto site (4040 m a.s.l.) can be seen as representative of the urban and Altiplano background, the road site located in Central La Paz (3590 m a.s.l.) is representative for heavy traffic-dominated conditions. Peaks of eBC mass concentrations up to 5 μg m−3 were observed at the El Alto background site in the early morning and evening, while minimum values were detected in the early afternoon, mainly due to thermal convection and change of the planetary boundary layer height. The traffic-related eBC mass concentrations at the road site reached maximum values of 10–20 μg m−3. A complete traffic ban on the specific Bolivian Day of Census (November 21, 2012) led to a decrease of eBC below 1 μg m−3 at the road site for the entire day. Compared to the day before and after, particle number concentrations decreased by a factor between 5 and 25 over the particle size range from 10 to 800 nm, while the submicrometer particle mass concentration dropped by approximately 80%. These results indicate that traffic is the dominating source of BC and particulate air pollution in the metropolitan area of La Paz/El Alto. In general, the diurnal cycle of eBC mass concentration at the Chacaltaya observatory is anti-correlated to the observations at the El Alto background site. This pattern indicates that the traffic-related particulate matter, including BC, is transported to higher altitudes with the developing of the boundary layer during daytime. The metropolitan area of La Paz/El Alto seems to be a significant source for BC of the regional lower free troposphere. From there, BC can be transported over long distances and exert impact on climate and composition of remote southern hemisphere.
- ItemThe influence of impactor size cut-off shift caused by hygroscopic growth on particulate matter loading and composition measurements(Oxford [u.a.] : Elsevier, 2018) Chen, Ying; Wild, Oliver; Wang, Yu; Ran, Liang; Teich, Monique; Größ, Johannes; Wang, Lina; Spindler, Gerald; Herrmann, Hartmut; van Pinxteren, Dominik; McFiggans, Gordon; Wiedensohler, AlfredThe mass loading and composition of atmospheric particles are important in determining their climate and health effects, and are typically measured by filter sampling. However, particle sampling under ambient conditions can lead to a shift in the size cut-off threshold induced by hygroscopic growth, and the influence of this on measurement of particle loading and composition has not been adequately quantified. Here, we propose a method to assess this influence based on κ-Köhler theory. A global perspective is presented based on previously reported annual climatological values of hygroscopic properties, meteorological parameters and particle volume size distributions. Measurements at background sites in Europe may be more greatly influenced by the cut-off shift than those from other continents, with a median influence of 10–20% on the total mass of sampled particles. However, the influence is generally much smaller (<7%) at urban sites, and is negligible for dust and particles in the Arctic. Sea-salt particles experience the largest influence (median value ∼50%), resulting from their large size, high hygroscopicity and the high relative humidity (RH) in marine air-masses. We estimate a difference of ∼30% in this influence of sea-salt particle sampling between relatively dry (RH = 60%) and humid (RH = 90%) conditions. Given the variation in the cut-off shift in different locations and at different times, a consistent consideration of this influence using the approach we introduce here is critical for observational studies of the long-term and spatial distribution of particle loading and composition, and crucial for robust validation of aerosol modules in modelling studies.