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- ItemAerosol Particle and Black Carbon Emission Factors of Vehicular Fleet in Manila, Philippines(Basel, Switzerland : MDPI AG, 2019) MadueƱo, Leizel; Kecorius, Simonas; Birmili, Wolfram; MĆ¼ller, Thomas; Simpas, James; Vallar, Edgar; Galvez, Maria Cecilia; Cayetano, Mylene; Wiedensohler, AlfredPoor air quality has been identified as one of the main risks to human health, especially in developing regions, where the information on physical chemical properties of air pollutants is lacking. To bridge this gap, we conducted an intensive measurement campaign in Manila, Philippines to determine the emission factors (EFs) of particle number (PN) and equivalent black carbon (BC). The focus was on public utility jeepneys (PUJ), equipped with old technology diesel engines, widely used for public transportation. The EFs were determined by aerosol physical measurements, fleet information, and modeled dilution using the Operational Street Pollution Model (OSPM). The results show that average vehicle EFs of PN and BC in Manila is up to two orders of magnitude higher than European emission standards. Furthermore, a PUJ emits up to seven times more than a light-duty vehicles (LDVs) and contribute to more than 60% of BC emission in Manila. Unfortunately, traffic restrictions for heavy-duty vehicles do not apply to PUJs. The results presented in this work provide a framework to help support targeted traffic interventions to improve urban air quality not only in Manila, but also in other countries with a similar fleet composed of old-technology vehicles. Ā© 2019 by the authors.
- ItemTerrestrial or marine ā indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7Ā°āN(Katlenburg-Lindau : European Geosciences Union, 2021) Hartmann, Markus; Gong, Xianda; Kecorius, Simonas; van Pinxteren, Manuela; Vogl, Teresa; Welti, AndrĆ©; Wex, Heike; Zeppenfeld, Sebastian; Herrmann, Hartmut; Wiedensohler, Alfred; Stratmann, FrankIce-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. -38gC and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above -10gC and below -32gC, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95gC for 1Äā¬ĀÆh, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2Äā¬ĀÆĪ¼m syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2Äā¬ĀÆĪ¼m. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with -3.47gC, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above -10gC. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source. Ā© Author(s) 2021.
- ItemExposure and Respiratory Tract Deposition Dose of Equivalent Black Carbon in High Altitudes(Basel, Switzerland : MDPI AG, 2020) MadueƱo, Leizel; Kecorius, Simonas; Andrade, Marcos; Wiedensohler, AlfredThe traffic microenvironment accounts for a significant fraction of the total daily dose of inhaled air pollutants. The adverse effects of air pollution may be intensified in high altitudes (HA) due to increased minute ventilation (MV), which may result in higher deposition doses compared to that at sea level. Despite this, air quality studies in regions with combined high pollution levels and enhanced inhalation are limited. The main goals of this study are to investigate how the choice of travel mode (walking, microbus, and cable car ride) determines (i) the personal exposure to equivalent black carbon (eBC) and (ii) the corresponding potential respiratory deposited dose (RDD) in HA. For this investigation, we chose La Paz and El Alto in Bolivia as HA representative cities. The highest eBC exposure occurred in microbus commutes (13 Ī¼g m-3), while the highest RDD per trip was recorded while walking (6.3 Ī¼g) due to increased MV. On the other hand, the lowest eBC exposure and RDD were observed in cable car commute. Compared with similar studies done at sea level, our results revealed that a HA city should reduce exposure by 1.4 to 1.8-fold to achieve similar RDD at sea level, implying that HA cities require doubly aggressive and stringent road emission policies compared to those at sea level. Ā© 2020 by the authors.
- ItemNew particle formation and its effect on cloud condensation nuclei abundance in the summer Arctic: A case study in the Fram Strait and Barents Sea(Katlenburg-Lindau : EGU, 2019) Kecorius, Simonas; Vogl, Teresa; Paasonen, Pauli; Lampilahti, Janne; Rothenberg, Daniel; Wex, Heike; Zeppenfeld, Sebastian; van Pinxteren, Manuela; Hartmann, Markus; Henning, Silvia; Gong, Xianda; Welti, Andre; Kulmala, Markku; Stratmann, Frank; Herrmann, Hartmut; Wiedensohler, AlfredIn a warming Arctic the increased occurrence of new particle formation (NPF) is believed to originate from the declining ice coverage during summertime. Understanding the physico-chemical properties of newly formed particles, as well as mechanisms that control both particle formation and growth in this pristine environment, is important for interpreting aerosol-cloud interactions, to which the Arctic climate can be highly sensitive. In this investigation, we present the analysis of NPF and growth in the high summer Arctic. The measurements were made on-board research vessel Polarstern during the PS106 Arctic expedition. Four distinctive NPF and subsequent particle growth events were observed, during which particle (diameter in a range 10-50ānm) number concentrations increased from background values of approx. 40 up to 4000ācm-3. Based on particle formation and growth rates, as well as hygroscopicity of nucleation and the Aitken mode particles, we distinguished two different types of NPF events. First, some NPF events were favored by negative ions, resulting in more-hygroscopic nucleation mode particles and suggesting sulfuric acid as a precursor gas. Second, other NPF events resulted in less-hygroscopic particles, indicating the influence of organic vapors on particle formation and growth. To test the climatic relevance of NPF and its influence on the cloud condensation nuclei (CCN) budget in the Arctic, we applied a zero-dimensional, adiabatic cloud parcel model. At an updraft velocity of 0.1āmās-1, the particle number size distribution (PNSD) generated during nucleation processes resulted in an increase in the CCN number concentration by a factor of 2 to 5 compared to the background CCN concentrations. This result was confirmed by the directly measured CCN number concentrations. Although particles did not grow beyond 50ānm in diameter and the activated fraction of 15-50ānm particles was on average below 10ā%, it could be shown that the sheer number of particles produced by the nucleation process is enough to significantly influence the background CCN number concentration. This implies that NPF can be an important source of CCN in the Arctic. However, more studies should be conducted in the future to understand mechanisms of NPF, sources of precursor gases and condensable vapors, as well as the role of the aged nucleation mode particles in Arctic cloud formation. Ā© Author(s) 2019. This work is distributed under the Creative Commons Attribution 4.0 License.
- ItemInfluence of biomass burning on mixing state of sub-micron aerosol particles in the North China Plain(Oxford [u.a.] : Elsevier, 2017) Kecorius, Simonas; Ma, Nan; Teich, Monique; van Pinxteren, Dominik; Zhang, Shenglan; GrƶĪ², Johannes; Spindler, Gerald; MĆ¼ller, Konrad; Iinuma, Yoshiteru; Hu, Min; Herrmann, Hartmut; Wiedensohler, AlfredParticulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6Ā°N, 115.2Ā°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP.
- ItemAerosol particle mixing state, refractory particle number size distributions and emission factors in a polluted urban environment: Case study of Metro Manila, Philippines(Oxford [u.a.] : Elsevier, 2017) Kecorius, Simonas; MadueƱo, Leizel; Vallar, Edgar; Alas, Honey; Betito, Grace; Birmili, Wolfram; Cambaliza, Maria Obiminda; Catipay, Grethyl; Gonzaga-Cayetano, Mylene; Galvez, Maria Cecilia; Lorenzo, Genie; MĆ¼ller, Thomas; Simpas, James B.; Tamayo, Everlyn Gayle; Wiedensohler, AlfredUltrafine soot particles (black carbon, BC) in urban environments are related to adverse respiratory and cardiovascular effects, increased cases of asthma and premature deaths. These problems are especially pronounced in developing megacities in South-East Asia, Latin America, and Africa, where unsustainable urbanization ant outdated environmental protection legislation resulted in severe degradation of urban air quality in terms of black carbon emission. Since ultrafine soot particles do often not lead to enhanced PM10 and PM2.5 mass concentration, the risks related to ultrafine particle pollution may therefore be significantly underestimated compared to the contribution of secondary aerosol constituents. To increase the awareness of the potential toxicological relevant problems of ultrafine black carbon particles, we conducted a case study in Metro Manila, the capital of the Philippines. Here, we present a part of the results from a detailed field campaign, called Manila Aerosol Characterization Experiment (MACE, 2015). Measurements took place from May to June 2015 with the focus on the state of mixing of aerosol particles. The results were alarming, showing the abundance of externally mixed refractory particles (soot proxy) at street site with a maximum daily number concentration of approximately 15000 #/cm3. That is up to 10 times higher than in cities of Western countries. We also found that the soot particle mass contributed from 55 to 75% of total street site PM2.5. The retrieved refractory particle number size distribution appeared to be a superposition of 2 ultrafine modes at 20 and 80 nm with a corresponding contribution to the total refractory particle number of 45 and 55%, respectively. The particles in the 20 nm mode were most likely ash from metallic additives in lubricating oil, tiny carbonaceous particles and/or nucleated and oxidized organic polymers, while bigger ones (80 nm) were soot agglomerates. To the best of the authorsā knowledge, no other studies reported such high number concentration of ultrafine refractory particles under ambient conditions. Inverse modeling of emission factors of refractory particle number size distributions revealed that diesel-fed public utility Jeepneys, commonly used for public transportation, are responsible for 94% of total roadside emitted refractory particle mass. The observed results showed that the majority of urban pollution in Metro Manila is dominated by carbonaceous aerosol. This suggests that PM10 or PM2.5 metrics do not fully describe possible health related effects in this kind of urban environments. Extremely high concentrations of ultrafine particles have been and will continue to induce adverse health related effects, because of their potential toxicity. We imply that in megacities, where the major fraction of particulates originates from the transport sector, PM10 or PM2.5 mass concentration should be complemented by legislative measurements of equivalent black carbon mass concentration.
- ItemThe Arctic Cloud Puzzle: Using ACLOUD/PASCAL Multiplatform Observations to Unravel the Role of Clouds and Aerosol Particles in Arctic Amplification(Boston, Mass. : ASM, 2019) Wendisch, Manfred; Macke, Andreas; Ehrlich, AndrĆ©; LĆ¼pkes, Christof; Mech, Mario; Chechin, Dmitry; Dethloff, Klaus; Velasco, Carola Barrientos; Bozem, Heiko; BrĆ¼ckner, Marlen; Clemen, Hans-Christian; Crewell, Susanne; Donth, Tobias; Dupuy, Regis; Ebell, Kerstin; Egerer, Ulrike; Engelmann, Ronny; Engler, Christa; Eppers, Oliver; Gehrmann, Martin; Gong, Xianda; Gottschalk, Matthias; Gourbeyre, Christophe; Griesche, Hannes; Hartmann, Jƶrg; Hartmann, Markus; Heinold, Bernd; Herber, Andreas; Herrmann, Hartmut; Heygster, Georg; Hoor, Peter; Jafariserajehlou, Soheila; JƤkel, Evelyn; JƤrvinen, Emma; Jourdan, Olivier; KƤstner, Udo; Kecorius, Simonas; Knudsen, Erlend M.; Kƶllner, Franziska; Kretzschmar, Jan; Lelli, Luca; Leroy, Delphine; Maturilli, Marion; Mei, Linlu; Mertes, Stephan; Mioche, Guillaume; Neuber, Roland; Nicolaus, Marcel; Nomokonova, Tatiana; Notholt, Justus; Palm, Mathias; van Pinxteren, Manuela; Quaas, Johannes; Richter, Philipp; Ruiz-Donoso, Elena; SchƤfer, Michael; Schmieder, Katja; Schnaiter, Martin; Schneider, Johannes; Schwarzenbƶck, Alfons; Seifert, Patric; Shupe, Matthew D.; Siebert, Holger; Spreen, Gunnar; Stapf, Johannes; Stratmann, Frank; Vogl, Teresa; Welti, AndrĆ©; Wex, Heike; Wiedensohler, Alfred; Zanatta, Marco; Zeppenfeld, SebastianClouds play an important role in Arctic amplification. This term represents the recently observed enhanced warming of the Arctic relative to the global increase of near-surface air temperature. However, there are still important knowledge gaps regarding the interplay between Arctic clouds and aerosol particles, and surface properties, as well as turbulent and radiative fluxes that inhibit accurate model simulations of clouds in the Arctic climate system. In an attempt to resolve this so-called Arctic cloud puzzle, two comprehensive and closely coordinated field studies were conducted: the Arctic Cloud Observations Using Airborne Measurements during Polar Day (ACLOUD) aircraft campaign and the Physical Feedbacks of Arctic Boundary Layer, Sea Ice, Cloud and Aerosol (PASCAL) ice breaker expedition. Both observational studies were performed in the framework of the German Arctic Amplification: Climate Relevant Atmospheric and Surface Processes, and Feedback Mechanisms (AC) project. They took place in the vicinity of Svalbard, Norway, in May and June 2017. ACLOUD and PASCAL explored four pieces of the Arctic cloud puzzle: cloud properties, aerosol impact on clouds, atmospheric radiation, and turbulent dynamical processes. The two instrumented Polar 5 and Polar 6 aircraft; the icebreaker Research Vessel (R/V) Polarstern; an ice floe camp including an instrumented tethered balloon; and the permanent ground-based measurement station at Ny-Ć lesund, Svalbard, were employed to observe Arctic low- and mid-level mixed-phase clouds and to investigate related atmospheric and surface processes. The Polar 5 aircraft served as a remote sensing observatory examining the clouds from above by downward-looking sensors; the Polar 6 aircraft operated as a flying in situ measurement laboratory sampling inside and below the clouds. Most of the collocated Polar 5/6 flights were conducted either above the R/V Polarstern or over the Ny-Ć lesund station, both of which monitored the clouds from below using similar but upward-looking remote sensing techniques as the Polar 5 aircraft. Several of the flights were carried out underneath collocated satellite tracks. The paper motivates the scientific objectives of the ACLOUD/PASCAL observations and describes the measured quantities, retrieved parameters, and the applied complementary instrumentation. Furthermore, it discusses selected measurement results and poses critical research questions to be answered in future papers analyzing the data from the two field campaigns.
- ItemHeterogeneous N2O5 uptake coefficient and production yield of ClNO2 in polluted northern China: Roles of aerosol water content and chemical composition(Katlenburg-Lindau : EGU, 2018) Tham, Yee Jun; Wang, Zhe; Li, Qinyi; Wang, Weihao; Wang, Xinfeng; Lu, Keding; Ma, Nan; Yan, Chao; Kecorius, Simonas; Wiedensohler, Alfred; Zhang, Yuanhang; Wang, TaoHeterogeneous uptake of dinitrogen pentoxide (N2O5) and production of nitryl chloride (ClNO2) are important nocturnal atmospheric processes that have significant implications for the production of secondary pollutants. However, the understanding of N2O5 uptake processes and ClNO2 production remains limited, especially in China. This study presents a field investigation of the N2O5 heterogeneous uptake coefficient (Ī³(N2O5)) and ClNO2 production yield (Ļ) in a polluted area of northern China during the summer of 2014. The N2O5 uptake coefficient and ClNO2 yield were estimated by using the simultaneously measured ClNO2 and total nitrate in 10 selected cases, which have concurrent increases in the ClNO2 and nitrate concentrations and relatively stable environmental conditions. The determined Ī³(N2O5) and Ļ values varied greatly, with an average of 0.022 for Ī³(N2O5) (Ā±0.012, standard deviation) and 0.34 for Ļ (Ā±0.28, standard deviation). The variations in Ī³(N2O5) could not be fully explained by the previously derived parameterizations of N2O5 uptake that consider nitrate, chloride, and the organic coating. Heterogeneous uptake of N2O5 was found to have a strong positive dependence on the relative humidity and aerosol water content. This result suggests that the heterogeneous uptake of N2O5 in Wangdu is governed mainly by the amount of water in the aerosol, and is strongly water limited, which is different from most of the field observations in the US and Europe. The ClNO2 yield estimated from the parameterization was also overestimated comparing to that derived from the observation. The observation-derived Ļ showed a decreasing trend with an increasing ratio of acetonitrile to carbon monoxide, an indicator of biomass burning emissions, which suggests a possible suppressive effect on the production yield of ClNO2 in the plumes influenced by biomass burning in this region. The findings of this study illustrate the need to improve our understanding and to parameterize the key factors for Ī³(N2O5) and Ļ to accurately assess photochemical and haze pollution.