Browsing by Subject "PARTICULATE MATTER"

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  • Du, Wei; Dada, Lubna; Zhao, Jian; Chen, Xueshun; Dällenbach, Kaspar; Xie, Conghui; Wang, Weigang; He, Yao; Cai, Jing; Yao, Lei; Zhang, Yingjie; Wang, Qingqing; Xu, Weiqi; Wang, Yuying; Tang, Guiqian; Cheng, Xueling; Kokkonen, Tom V.; Zhou, Wei; Yan, Chao; Chu, Biwu; Zha, Qiaozhi; Hakala, Simo; Kurppa, Mona; Jarvi, Leena; Liu, Yongchun; Li, Zhanqing; Ge, Maofa; Fu, Pingqing; Nie, Wei; Bianchi, Federico; Petäjä, Tuukka; Paasonen, Pauli; Wang, Zifa; Worsnop, Douglas R.; Kerminen, Veli-Matti; Kulmala, Markku; Sun, Yele (2021)
    The role of new particle formation (NPF) events and their contribution to haze formation through subsequent growth in polluted megacities is still controversial. To improve the understanding of the sources, meteorological conditions, and chemistry behind air pollution, we performed simultaneous measurements of aerosol composition and particle number size distributions at ground level and at 260 m in central Beijing, China, during a total of 4 months in 2015-2017. Our measurements show a pronounced decoupling of gas-to-particle conversion between the two heights, leading to different haze processes in terms of particle size distributions and chemical compositions. The development of haze was initiated by the growth of freshly formed particles at both heights, whereas the more severe haze at ground level was connected directly to local primary particles and gaseous precursors leading to higher particle growth rates. The particle growth creates a feedback loop, in which a further development of haze increases the atmospheric stability, which in turn strengthens the persisting apparent decoupling between the two heights and increases the severity of haze at ground level. Moreover, we complemented our field observations with model analyses, which suggest that the growth of NPF-originated particles accounted up to similar to 60% of the accumulation mode particles in the Beijing-Tianjin-Hebei area during haze conditions. The results suggest that a reduction in anthropogenic gaseous precursors, suppressing particle growth, is a critical step for alleviating haze although the number concentration of freshly formed particles (3-40 nm) via NPF does not reduce after emission controls.
  • Cavalli, F.; Alastuey, A.; Areskoug, H.; Ceburnis, D.; Cech, J.; Genberg, J.; Harrison, R. M.; Jaffrezo, J. L.; Kiss, G.; Laj, P.; Mihalopoulos, N.; Perez, N.; Quincey, P.; Schwarz, J.; Sellegri, K.; Spindler, G.; Swietlicki, E.; Theodosi, C.; Yttri, K. E.; Aas, W.; Putaud, J. P. (2016)
    Although particulate organic and elemental carbon (OC and EC) are important constituents of the suspended atmospheric particulate matter (PM), measurements of OC and EC are much less common and More uncertain than measurements of e.g. the ionic components of PM. In the framework of atmospheric research infrastructures supported by the European Union, actions have been undertaken to determine and mitigate sampling artefacts, and assess the comparability of OC and EC data obtained in a network of 10 atmospheric observatories across Europe. Positive sampling artefacts (from 0:4 to 2.8 mu g C/m(3)) and analytical discrepancies (between -50% and +40% for the EC/TC ratio) have been taken into account to generate a robust data set, from which we established the phenomenology of carbonaceous aerosols at regional background sites in Europe. Across the network, TC and EC annual average concentrations range from 0.4 to 9 mu g C/m(3), and from 0.1 to 2 mu g C/m(3), respectively. TC/PM10 annual mean ratios range from 0.11 at a Mediterranean site to 0.34 at the most polluted continental site, and TC/PM2.5 ratios are slightly greater at all sites (0.15-0.42). EC/TC annual mean ratios range from 0.10 to 0.22, and do not depend much on PM concentration levels, especially in winter. Seasonal variations in PM and TC concentrations, and in TC/PM and EC/TC ratios, differ across the network, which can be explained by seasonal changes in PM source contributions at some sites. (C) 2016 The Authors. Published by Elsevier Ltd.
  • Zanatta, M.; Gysel, M.; Bukowiecki, N.; Mueller, T.; Weingartner, E.; Areskoug, H.; Fiebig, M.; Yttri, K. E.; Mihalopoulos, N.; Kouvarakis, G.; Beddows, D.; Harrison, R. M.; Cavalli, F.; Putaud, J. P.; Spindler, G.; Wiedensohler, A.; Alastuey, A.; Pandolfi, M.; Sellegri, K.; Swietlicki, E.; Jaffrezo, J. L.; Baltensperger, U.; Laj, P. (2016)
    A reliable assessment of the optical properties of atmospheric black carbon is of crucial importance for an accurate estimation of radiative forcing. In this study we investigated the spatio-temporal variability of the mass absorption cross-section (MAC) of atmospheric black carbon, defined as light absorption coefficient (sigma(ap)) divided by elemental carbon mass concentration (m(EC)). sigma(ap) and m(EC) have been monitored at supersites of the ACTRIS network for a minimum period of one year. The 9 rural background sites considered in this study cover southern Scandinavia, central Europe and the Mediterranean. sigma(ap) was determined using filter based absorption photometers and m(EC) using a thermal-optical technique. Homogeneity of the data-set was ensured by harmonization of all involved methods and instruments during extensive intercomparison exercises at the European Center for Aerosol Calibration (ECAC). Annual mean values of sigma(ap) at a wavelength of 637 nm vary between 0.66 and 1.3 Mm(-1) in southern Scandinavia, 3.7-11 Mm(-1) in Central Europe and the British Isles, and 2.3-2.8 Mm(-1) in the Mediterranean. Annual mean values of mEC vary between 0.084 and 0.23 mu g m(-3) in southern Scandinavia, 0.28 -1.1 in Central Europe and the British Isles, and 0.22-0.26 in the Mediterranean. Both sigma(ap) and mEC in southern Scandinavia and Central Europe have a distinct seasonality with maxima during the cold season and minima during summer, whereas at the Mediterranean sites an opposite trend was observed. Annual mean MAC values were quite similar across all sites and the seasonal variability was small at most sites. Consequently, a MAC value of 10.0 m(2) g(-1) (geometric standard deviation = 133) at a wavelength of 637 nm can be considered to be representative of the mixed boundary layer at European background sites, where BC is expected to be internally mixed to a large extent. The observed spatial variability is rather small compared to the variability of values in previous literature, indicating that the harmonization efforts resulted in substantially increased precision of the reported MAC. However, absolute uncertainties of the reported MAC values remain as high as +/- 30-70% due to the lack of appropriate reference methods and calibration materials. The mass ratio between elemental carbon and non-light-absorbing matter was used as a proxy for the thickness of coatings around the BC cores, in order to assess the influence of the mixing state on the MAC of BC. Indeed, the MAC was found to increase with increasing values of the coating thickness proxy. This provides evidence that coatings do increase the MAC of atmospheric BC to some extent, which is commonly referred to as lensing effect. (C) 2016 The Authors. Published by Elsevier Ltd.
  • Pandolfi, Marco; Alados-Arboledas, Lucas; Alastuey, Andres; Andrade, Marcos; Angelov, Christo; Artinano, Begona; Backman, John; Baltensperger, Urs; Bonasoni, Paolo; Bukowiecki, Nicolas; Coen, Martine Collaud; Conil, Sebastien; Coz, Esther; Crenn, Vincent; Dudoitis, Vadimas; Ealo, Marina; Eleftheriadis, Kostas; Favez, Olivier; Fetfatzis, Prodromos; Fiebig, Markus; Flentje, Harald; Ginot, Patrick; Gysel, Martin; Henzing, Bas; Hoffer, Andras; Smejkalova, Adela Holubova; Kalapov, Ivo; Kalivitis, Nikos; Kouvarakis, Giorgos; Kristensson, Adam; Kulmala, Markku; Lihavainen, Heikki; Lunder, Chris; Luoma, Krista; Lyamani, Hassan; Marinoni, Angela; Mihalopoulos, Nikos; Moerman, Marcel; Nicolas, Jose; O'Dowd, Colin; Petäjä, Tuukka; Petit, Jean-Eudes; Pichon, Jean Marc; Prokopciuk, Nina; Putaud, Jean-Philippe; Rodriguez, Sergio; Sciare, Jean; Sellegri, Karine; Swietlicki, Erik; Titos, Gloria; Tuch, Thomas; Tunved, Peter; Ulevicius, Vidmantas; Vaishya, Aditya; Vana, Milan; Virkkula, Aki; Vratolis, Stergios; Weingartner, Ernest; Wiedensohler, Alfred; Laj, Paolo (2018)
    This paper presents the light-scattering properties of atmospheric aerosol particles measured over the past decade at 28 ACTRIS observatories, which are located mainly in Europe. The data include particle light scattering (sigma(sp)) and hemispheric backscattering (sigma(bsp)) coefficients, scattering Angstrom exponent (SAE), backscatter fraction (BF) and asymmetry parameter (g). An increasing gradient of sigma(sp) is observed when moving from remote environments (arctic/mountain) to regional and to urban environments. At a regional level in Europe, sigma(sp) also increases when moving from Nordic and Baltic countries and from western Europe to central/eastern Europe, whereas no clear spatial gradient is observed for other station environments. The SAE does not show a clear gradient as a function of the placement of the station. However, a west-to-east-increasing gradient is observed for both regional and mountain placements, suggesting a lower fraction of fine-mode particle in western/south-western Europe compared to central and eastern Europe, where the fine-mode particles dominate the scattering. The g does not show any clear gradient by station placement or geographical location reflecting the complex relationship of this parameter with the physical properties of the aerosol particles. Both the station placement and the geographical location are important factors affecting the intraannual variability. At mountain sites, higher sigma(sp) and SAE values are measured in the summer due to the enhanced boundary layer influence and/or new particle-formation episodes. Conversely, the lower horizontal and vertical dispersion during winter leads to higher sigma(sp) values at all low-altitude sites in central and eastern Europe compared to summer. These sites also show SAE maxima in the summer (with corresponding g minima). At all sites, both SAE and g show a strong variation with aerosol particle loading. The lowest values of g are always observed together with low sigma(sp) values, indicating a larger contribution from particles in the smaller accumulation mode. During periods of high sigma(sp) values, the variation of g is less pronounced, whereas the SAE increases or decreases, suggesting changes mostly in the coarse aerosol particle mode rather than in the fine mode. Statistically significant decreasing trends of sigma(sp) are observed at 5 out of the 13 stations included in the trend analyses. The total reductions of sigma(sp) are consistent with those reported for PM2.5 and PM10 mass concentrations over similar periods across Europe.
  • Laj, Paolo; Bigi, Alessandro; Rose, Clemence; Andrews, Elisabeth; Myhre, Cathrine Lund; Coen, Martine Collaud; Lin, Yong; Wiedensohler, Alfred; Schulz, Michael; Ogren, John A.; Fiebig, Markus; Gliss, Jonas; Mortier, Augustin; Pandolfi, Marco; Petäjä, Tuukka; Kim, Sang-Woo; Aas, Wenche; Putaud, Jean-Philippe; Mayol-Bracero, Olga; Keywood, Melita; Labrador, Lorenzo; Aalto, Pasi; Ahlberg, Erik; Alados Arboledas, Lucas; Alastuey, Andres; Andrade, Marcos; Artinano, Begona; Ausmeel, Stina; Arsov, Todor; Asmi, Eija; Backman, John; Baltensperger, Urs; Bastian, Susanne; Bath, Olaf; Beukes, Johan Paul; Brem, Benjamin T.; Bukowiecki, Nicolas; Conil, Sebastien; Couret, Cedric; Day, Derek; Dayantolis, Wan; Degorska, Anna; Eleftheriadis, Konstantinos; Fetfatzis, Prodromos; Favez, Olivier; Flentje, Harald; Gini, Maria I.; Gregoric, Asta; Gysel-Beer, Martin; Hallar, A. Gannet; Hand, Jenny; Hoffer, Andras; Hueglin, Christoph; Hooda, Rakesh K.; Hyvärinen, Antti; Kalapov, Ivo; Kalivitis, Nikos; Kasper-Giebl, Anne; Kim, Jeong Eun; Kouvarakis, Giorgos; Kranjc, Irena; Krejci, Radovan; Kulmala, Markku; Labuschagne, Casper; Lee, Hae-Jung; Lihavainen, Heikki; Lin, Neng-Huei; Loeschau, Gunter; Luoma, Krista; Marinoni, Angela; Dos Santos, Sebastiao Martins; Meinhardt, Frank; Merkel, Maik; Metzger, Jean-Marc; Mihalopoulos, Nikolaos; Nhat Anh Nguyen; Ondracek, Jakub; Perez, Noemi; Perrone, Maria Rita; Petit, Jean-Eudes; Picard, David; Pichon, Jean-Marc; Pont, Veronique; Prats, Natalia; Prenni, Anthony; Reisen, Fabienne; Romano, Salvatore; Sellegri, Karine; Sharma, Sangeeta; Schauer, Gerhard; Sheridan, Patrick; Sherman, James Patrick; Schuetze, Maik; Schwerin, Andreas; Sohmer, Ralf; Sorribas, Mar; Steinbacher, Martin; Sun, Junying; Titos, Gloria; Toczko, Barbara; Tuch, Thomas; Tulet, Pierre; Tunved, Peter; Vakkari, Ville; Velarde, Fernando; Velasquez, Patricio; Villani, Paolo; Vratolis, Sterios; Wang, Sheng-Hsiang; Weinhold, Kay; Weller, Rolf; Yela, Margarita; Yus-Diez, Jesus; Zdimal, Vladimir; Zieger, Paul; Zikova, Nadezda (2020)
    Aerosol particles are essential constituents of the Earth's atmosphere, impacting the earth radiation balance directly by scattering and absorbing solar radiation, and indirectly by acting as cloud condensation nuclei. In contrast to most greenhouse gases, aerosol particles have short atmospheric residence times, resulting in a highly heterogeneous distribution in space and time. There is a clear need to document this variability at regional scale through observations involving, in particular, the in situ near-surface segment of the atmospheric observation system. This paper will provide the widest effort so far to document variability of climate-relevant in situ aerosol properties (namely wavelength dependent particle light scattering and absorption coefficients, particle number concentration and particle number size distribution) from all sites connected to the Global Atmosphere Watch network. High-quality data from almost 90 stations worldwide have been collected and controlled for quality and are reported for a reference year in 2017, providing a very extended and robust view of the variability of these variables worldwide. The range of variability observed worldwide for light scattering and absorption coefficients, single-scattering albedo, and particle number concentration are presented together with preliminary information on their long-term trends and comparison with model simulation for the different stations. The scope of the present paper is also to provide the necessary suite of information, including data provision procedures, quality control and analysis, data policy, and usage of the ground-based aerosol measurement network. It delivers to users of the World Data Centre on Aerosol, the required confidence in data products in the form of a fully characterized value chain, including uncertainty estimation and requirements for contributing to the global climate monitoring system.
  • Belis, C. A.; Karagulian, F.; Amato, F.; Almeida, M.; Artaxo, P.; Beddows, D. C. S.; Bernardoni, V.; Bove, M. C.; Carbone, S.; Cesari, D.; Contini, D.; Cuccia, E.; Diapouli, E.; Eleftheriadis, K.; Favez, O.; El Haddad, I.; Harrison, R. M.; Hellebust, S.; Hovorka, J.; Jang, E.; Jorquera, H.; Kammermeier, T.; Karl, M.; Lucarelli, F.; Mooibroek, D.; Nava, S.; Nojgaard, J. K.; Paatero, P.; Pandolfi, M.; Perrone, M. G.; Petit, J. E.; Pietrodangelo, A.; Pokorna, P.; Prati, P.; Prevot, A. S. H.; Quass, U.; Querol, X.; Saraga, D.; Sciare, J.; Sfetsos, A.; Valli, G.; Vecchi, R.; Vestenius, M.; Yubero, E.; Hopke, P. K. (2015)
    The performance and the uncertainty of receptor models (RMs) were assessed in intercomparison exercises employing real-world and synthetic input datasets. To that end, the results obtained by different practitioners using ten different RMs were compared with a reference. In order to explain the differences in the performances and uncertainties of the different approaches, the apportioned mass, the number of sources, the chemical profiles, the contribution-to-species and the time trends of the sources were all evaluated using the methodology described in Bells et al. (2015). In this study, 87% of the 344 source contribution estimates (SCEs) reported by participants in 47 different source apportionment model results met the 50% standard uncertainty quality objective established for the performance test. In addition, 68% of the SCE uncertainties reported in the results were coherent with the analytical uncertainties in the input data. The most used models, EPA-PMF v.3, PMF2 and EPA-CMB 8.2, presented quite satisfactory performances in the estimation of SCEs while unconstrained models, that do not account for the uncertainty in the input data (e.g. APCS and FA-MLRA), showed below average performance. Sources with well-defined chemical profiles and seasonal time trends, that make appreciable contributions (>10%), were those better quantified by the models while those with contributions to the PM mass close to 1% represented a challenge. The results of the assessment indicate that RMs are capable of estimating the contribution of the major pollution source categories over a given time window with a level of accuracy that is in line with the needs of air quality management. (C) 2015 The Authors. Published by Elsevier Ltd.
  • Zhang, Yanjun; Peräkylä, Otso; Yan, Chao; Heikkinen, Liine; Äijälä, Mikko; Dällenbach, Kaspar; Zha, Qiaozhi; Riva, Matthieu; Garmash, Olga; Junninen, Heikki; Paatero, Pentti; Worsnop, Douglas; Ehn, Mikael (2019)
    Recent advancements in atmospheric mass spectrometry provide huge amounts of new information but at the same time present considerable challenges for the data analysts. High-resolution (HR) peak identification and separation can be effort- and time-consuming yet still tricky and inaccurate due to the complexity of overlapping peaks, especially at larger mass-to-charge ratios. This study presents a simple and novel method, mass spectral binning combined with positive matrix factorization (binPMF), to address these problems. Different from unit mass resolution (UMR) analysis or HR peak fitting, which represent the routine data analysis approaches for mass spectrometry datasets, binPMF divides the mass spectra into small bins and takes advantage of the positive matrix factorization's (PMF) strength in separating different sources or processes based on different temporal patterns. In this study, we applied the novel approach to both ambient and synthetic datasets to evaluate its performance. It not only succeeded in separating overlapping ions but was found to be sensitive to subtle variations as well. Being fast and reliable, binPMF has no requirement for a priori peak information and can save much time and effort from conventional HR peak fitting, while still utilizing nearly the full potential of HR mass spectra. In addition, we identify several future improvements and applications for binPMF and believe it will become a powerful approach in the data analysis of mass spectra.
  • Demmler, Joanne C.; Gosztonyi, Ákos; Du, Yaxing; Leinonen, Matti; Ruotsalainen, Laura; Järvi , Leena; Ala-Mantila, Sanna (2021)
    Background Air pollution is one of the major environmental challenges cities worldwide face today. Planning healthy environments for all future populations, whilst considering the ongoing demand for urbanisation and provisions needed to combat climate change, remains a difficult task. Objective To combine artificial intelligence (AI), atmospheric and social sciences to provide urban planning solutions that optimise local air quality by applying novel methods and taking into consideration population structures and traffic flows. Methods We will use high-resolution spatial data and linked electronic population cohort for Helsinki Metropolitan Area (Finland) to model (a) population dynamics and urban inequality related to air pollution; (b) detailed aerosol dynamics, aerosol and gas-phase chemistry together with detailed flow characteristics; (c) high-resolution traffic flow addressing dynamical changes at the city environment, such as accidents, construction work and unexpected congestion. Finally, we will fuse the information resulting from these models into an optimal city planning model balancing air quality, comfort, accessibility and travelling efficiency.
  • Hussein, Tareq; Juwhari, Hassan; Al Kuisi, Mustafa; Alkattan, Hamza; Lahlouh, Bashar; Al-Hunaiti, Afnan (2018)
    In this study, we analyzed the concentrations of accumulation and coarse modes measured during November 2013–July 2017 at an urban background site in Amman, Jordan. The concentrations showed distinct seasonal variations with high concentrations with a monthly average higher than 100 cm−3 and 1.5 cm−3, respectively, for accumulation and coarse modes during the winter and low concentrations with a monthly average less than 40 cm−3 and 1–1.5 cm−3, respectively, for accumulation and coarse modes during the summer. Sand and dust storms (SDS) affected the coarse mode during the early spring whereas local dust re-suspension affected them during the autumn. The gravimetric analysis confirmed the seasonal variation of the calculated particulate mass concentration but suggested that the assumption of spherical particles and unit density is not always proper. The ATR-FTIR analysis of selected filters revealed that aerosols in the background atmosphere of Amman are a mixture of locally emitted (fossil fuel combustion) and local/regional dust. Based on the 24-h average of the calculated PM10, the pollution standard index (PSI) revealed that about 81% of the days were either good or moderate air quality conditions. About 71% of the days were below the 24-h PM10 limit value according to the Jordanian air quality standards (120 μg m−3).
  • Crenn, V.; Sciare, J.; Croteau, P. L.; Verlhac, S.; Froehlich, R.; Belis, C. A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artinano, B.; Baisnee, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillon, M. C.; Mocnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petit, J. -E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Esteve, R.; Slowik, J. G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prevot, A. S. H.; Jayne, J. T.; Favez, O. (2015)
    As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for 3 weeks during the late-fall-early-winter period (November-December 2013). The first week was dedicated to the tuning and calibration of each instrument, whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical, and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium, and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r(2) > 0.9) were observed systematically for each individual Q-ACSM across all chemical families except for chloride for which three Q-ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025, 1999) and were found to be 9, 15, 19, 28, and 36% for NR-PM1, nitrate, organic matter, sulfate, and ammonium, respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of Q-ACSMs, detailed intercomparison results are presented, along with a discussion of some recommendations about best calibration practices, standardized data processing, and data treatment.
  • Petäjä, Tuukka; Ovaska, Aino; Fung, Pak Lun; Poutanen, Pyry; Yli-Ojanperä, Jaakko; Suikkola, Jari; Laakso, Mikko; Mäkelä, Taneli; Niemi, Jarkko V.; Keskinen, Jorma; Järvinen, Anssi; Kuula, Joel; Kurppa, Mona; Hussein, Tareq; Tarkoma, Sasu; Kulmala, Markku; Karppinen, Ari; Manninen, Hanna E.; Timonen, Hilkka (2021)
    Poor air quality influences the quality of life in the urban environment. The regulatory observation stations provide the backbone for the city administration to monitor urban air quality. Recently a suite of cost-effective air quality sensors has emerged to provide novel insights into the spatio-temporal variability of aerosol particles and trace gases. Particularly in low concentrations these sensors might suffer from issues related e.g., to high detection limits, concentration drifts and interdependency between the observed trace gases and environmental parameters. In this study we characterize the optical particle detector used in AQT530 (Vaisala Ltd.) air quality sensor in the laboratory. We perform a measurement campaign with a network of AQT530 sensors in Helsinki, Finland in 2020-2021 and present a long-term performance evaluation of five sensors for particulate (PM10, PM2.5) and gaseous (NO2, NO, CO, O-3) components during a half-year co-location study with reference instruments at an urban traffic site. Furthermore, short-term (3-5 weeks) co-location tests were performed for 25 sensors to provide sensor-specific correction equations for the fine-tuning of selected pollutants in the sensor network. We showcase the added value of the verified network of 25 sensor units to address the spatial variability of trace gases and aerosol mass concentrations in an urban environment. The analysis assesses road and harbor traffic monitoring, local construction dust monitoring, aerosol concentrations from fireworks, impact of sub-urban small scale wood combustion and detection of long-range transport episodes on a city scale. Our analysis illustrates that the calibrated network of Vaisala AQT530 air quality sensors provide new insights into the spatio-temporal variability of air pollution within the city. This information is beneficial to, for example, optimization of road dust and construction dust emission control as well as provides data to tackle air quality problems arising from traffic exhaust and localized wood combustion emissions in the residential areas.
  • Maragkidou, Androniki; Jaghbeir, Omar; Hämeri, Kaarle; Hussein, Tareq (2018)
    In this study, we measured the concentrations of accumulation and coarse particles inside an educational workshop (March 31–April 6, 2015), calculated particle emission and losses rates, and estimated inhaled deposited dose. We used an Optical Particle Sizer (TSI OPS 3330) that measures the particle number size distribution (diameter 0.3–10 μm) and we converted that into particle mass size distribution (assuming spherical particles and unit density). We focused on two particle size fractions: 0.3–1 μm (referred as PN0.3−1 and PM0.3−1) and 1–10 μm (referred as PN1−10 and PM1−10). The occupants' activities included coffee brewing, lecturing, tobacco smoking, welding, scrubbing, and sorting/drilling iron. The highest concentrations were observed during welding with PN0.3−1 (PM0.3−1) was ∼1866 cm−3 (55 μg/m3) and PN1−10 (PM1−10) was ∼7 cm−3 (103 μg/m3). The lowest concentrations were observed during coffee brewing and metal turning with PN0.3−1 (PM0.3−1) was ∼22 cm−3 (0.7 μg/m3) and PN1−10 (PM1−10) was ∼0.5 cm−3 (4 μg/m3). The emissions rate of coarse particles was 85–1010 particles/hour × cm3 whereas that for submicron particle in the diameter range 0.3–1 μm was 5.7 × 104–9.3 × 104 particles/hour × cm3 depending on the activity and the ventilation rate. The coarse particles losses rate was 0.35–2.1 h−1 and the ventilation rate was 0.24–2.1 h−1. The alveolar received the majority and particles below 1 μm with a fraction of about 53% of the total inhaled deposited dose whereas the head/throat region received about 18%. This study is important for better understanding the health effects at educational workshops.
  • Hemmilä, Marja; Hellén, Heidi; Virkkula, Aki; Makkonen, Ulla; Praplan, Arnaud P.; Kontkanen, Jenni; Ahonen, Lauri; Kulmala, Markku; Hakola, Hannele (2018)
    We measured amines in boreal forest air in Finland both in gas and particle phases with 1 h time resolution using an online ion chromatograph (instrument for Measuring AeRosols and Gases in Ambient Air - MARGA) connected to an electrospray ionization quadrupole mass spectrometer (MS). The developed MARGA-MS method was able to separate and detect seven different amines: monomethylamine (MMA), dimethylamine (DMA), trimethylamine (TMA), ethylamine (EA), diethylamine (DEA), propylamine (PA), and butylamine (BA). The detection limits of the method for amines were low (0.2-3.1 ng m(-3)), the accuracy of ICMS analysis was 11-37 %, and the precision 10-15 %. The proper measurements in the boreal forest covered about 8 weeks between March and December 2015. The amines were found to be an inhomogeneous group of compounds, showing different seasonal and diurnal variability. Total MMA (MMA(tot)) peaked together with the sum of ammonia and ammonium ions already in March. In March, monthly means for MMA were 90 %, gas-phase DMA correlated well with 1.1-2 nm particle number concentration (R-2 = 0.63) suggesting that it participates in atmospheric clustering. EA concentrations were low all the time. Its July means were <0.36 and 0.4 +/- 0.4 ng m(-3) in gas and aerosol phases, respectively, but individual concentration data correlated well with monoterpene concentrations in July. Monthly means of PA and BA were below detection limits at all times.
  • Helin, Aku; Sietiö, Outi-Maaria; Heinonsalo, Jussi; Bäck, Jaana; Riekkola, Marja-Liisa; Parshintsev, Jevgeni (2017)
    Primary biological aerosol particles (PBAPs) are ubiquitous in the atmosphere and constitute similar to 30% of atmospheric aerosol particle mass in sizes > 1 mu m. PBAP components, such as bacteria, fungi and pollen, may affect the climate by acting as cloud-active particles, thus having an effect on cloud and precipitation formation processes. In this study, size-segregated aerosol samples (<1.0, 1-2.5, 2.5-10 and > 10 mu m) were collected in boreal forest (Hyytiala, Finland) during a 9-month period covering all seasons and analysed for free amino acids (FAAs), DNA concentration and microorganism (bacteria, Pseudomonas and fungi). Measurements were performed using tandem mass spectrometry, spectrophotometry and qPCR, respectively. Meteorological parameters and statistical analysis were used to study their atmospheric implication for results. Distinct annual patterns of PBAP components were observed, late spring and autumn being seasons of dominant occurrence. Elevated abundances of FAAs and bacteria were observed during the local pollen season, whereas fungi were observed at the highest level during autumn. Meteorological parameters such as air and soil temperature, radiation and rainfall were observed to possess a close relationship with PBAP abundances on an annual scale.
  • Carbone, S.; Onasch, T.; Saarikoski, S.; Timonen, H.; Saarnio, K.; Sueper, D.; Ronkko, T.; Pirjola, L.; Häyrinen, A.; Worsnop, D.; Hillamo, R. (2015)
    A method to detect and quantify mass concentrations of trace metals on soot particles by the Aerodyne soot-particle aerosol mass spectrometer (SP-AMS) was developed and evaluated in this study. The generation of monodisperse Regal black (RB) test particles with trace amounts of 13 different metals (Na, Al, Ca, V, Cr, Mn, Fe, Ni, Cu, Zn, Rb, Sr and Ba) allowed for the determination of the relative ionization efficiency of each metal relative to black carbon (RIEmeas). The observed RIEmeas/RIEtheory values were larger than unity for Na, Rb, Ca, Sr and Ba due to thermal surface ionization (TSI) on the surface of the laser-heated RB particles. Values closer to unity were obtained for the transition metals Zn, Cu, V and Cr. Mn, Fe, and Ni presented the lowest RIEmeas/RIEtheory ratios and highest deviation from unity. The latter discrepancy is unexplained; however it may be related to problems with our calibration method and/or the formation of metal complexes that were not successfully quantified. The response of the metals to the laser power was investigated and the results indicated that a minimum pump laser current of 0.6 A was needed in order to vaporize the metals and the refractory black carbon (rBC). Isotopic patterns of metals were resolved from high-resolution mass spectra, and the mass-weighted size distributions for each individual metal ion were obtained using the high-resolution particle time-of-flight (HR-PToF) method. The RIEmeas values obtained in this study were applied to the data of emission measurements in a heavy-fuel-oil-fired heating station. Emission measurements revealed a large number of trace metals, including evidence for metal oxides and metallic salts, such as vanadium sulfate, calcium sulfate, iron sulfate and barium sulfate, which were identified in the SP-AMS high-resolution mass spectra. SP-AMS measurements of Ba, Fe, and V agreed with ICP-MS analyzed filter samples within a factor of 2 when emitted rBC mass loadings were elevated.
  • Enroth, Joonas; Saarikoski, Sanna; Niemi, Jarkko; Kousa, Anu; Jezek, Irena; Mocnik, Grisa; Carbone, Samara; Kuuluvainen, Heino; Rönkkö, Topi; Hillamo, Risto; Pirjola, Liisa (2016)
    Traffic-related pollution is a major concern in urban areas due to its deleterious effects on human health. The characteristics of the traffic emissions on four highway environments in the Helsinki metropolitan area were measured with a mobile laboratory, equipped with state-of-the-art instrumentation. Concentration gradients were observed for all traffic-related pollutants, particle number (CN), particulate mass (PM1), black carbon (BC), organics, and nitrogen oxides (NO and NO2). Flow dynamics in different environments appeared to be an important factor for the dilution of the pollutants. For example, the half-decay distances for the traffic-related CN concentrations varied from 8 to 83aEuro-m at different sites. The PM1 emissions from traffic mostly consisted of organics and BC. At the most open site, the ratio of organics to BC increased with distance to the highway, indicating condensation of volatile and semi-volatile organics on BC particles. These condensed organics were shown to be hydrocarbons as the fraction of hydrocarbon fragments in organics increased. Regarding the CN size distributions, particle growth during the dilution was not observed; however the mass size distributions measured with a soot particle aerosol mass spectrometer (SP-AMS), showed a visible shift of the mode, detected at aEuro-100aEuro-nm at the roadside, to a larger size when the distance to the roadside increased. The fleet average emission factors appeared to be lower for the CN and higher for the NO2 than ten years ago. The reason is likely to be the increased fraction of light-duty (LD) diesel vehicles in the past ten years. The fraction of heavy-duty (HD) traffic, although constituting less than 10aEuro-% of the total traffic flow, was found to have a large impact on the emissions.
  • Hirvonen, Viivi; Myllys, Nanna; Kurtén, Theo; Elm, Jonas (2018)
    The role of covalently bound dimer formation is studied using highlevel quantum chemical methods. Reaction free energy profiles for dimer formation between common oxygen-containing functional groups are calculated, and based on the Gibbs free energy differences between transition states and reactants, we show that none of the studied two-component gas-phase reactions are kinetically feasible at 298.15 K and 1 atm. Therefore, the catalyzing effect of water, base, or acid molecules is calculated, and sulfuric acid is identified to lower the activation free energies significantly. We find that the reactions yielding hemiacetal, peroxyhemiacetal, alpha-hydroxyester, and geminal diol products occur with activation free energies of less than 10 kcal/mol with sulfuric acid as a catalyst, indicating that these reactions could potentially take place on the surface of sulfuric acid clusters. Additionally, the formed dimer products bind stronger onto the pre-existing cluster than the corresponding reagent monomers do. This implies that covalent dimerization reactions stabilize the existing cluster thermodynamically and make it less likely to evaporate. However, the studied small organic compounds, which contain only one functional group, not able to form dimer are products that are stable against evaporation at atmospheric conditions. Calculations of dimer formation onto a cluster surface and the clustering ability of dimer products should be extended to large terpene oxidation products in order to estimate the real atmospheric significance.
  • Keshavarz, Fatemeh; Shcherbacheva, Anna; Kubecka, Jakub; Vehkamäki, Hanna; Kurten, Theo (2019)
    The effect of dust aerosols on accretion reactions of water, formaldehyde, and formic acid was studied in the conditions of earth's troposphere at the DLPNO-CCSD(T)/aug-cc-pVTZ//omega B97X-D/6-31++G** level of theory. A detailed analysis of the reaction mechanisms in the gas phase and on the surface of mineral dust, represented by mono- and trisilicic acid, revealed that mineral dust has the potential of decreasing reaction barrier heights. Specifically, at 0 K, mineral dust can lower the apparent energy barrier of the reaction of formaldehyde with formic acid to zero. However, when the entropic contributions to the reaction free energies were accounted for, mineral dust was found to selectively enhance the reaction of water with formaldehyde, while inhibiting the reaction of formaldehyde and formic acid, in the lower parts of the troposphere (with temperatures around 298 K). In the upper troposphere (with temperatures closer to 198 K), mineral dust catalyzes both reactions and also the reaction of methanol with formic acid. Despite the intrinsic potential of mineral dust, calculation of the catalytic enhancement parameter for a likely range of dust aerosol concentrations suggested that dust aerosols will not contribute to secondary organic aerosol formation via dimerization of closed-shell organic compounds. The main reason for this is the relatively low absolute concentratign of tropospheric dust aerosol and its inefficiency in increasing the effective reaction rate coefficients.
  • Al Bawab, Abeer; Al-Hunaiti, Afnan; Abu Mallouh, Saida; Bozeya, Ayat; Abu-Zurayk, Rund; Hussein, Tareq (2020)
    Some cultural heritage sites in Jordan are in urban areas being exposed to anthropogenic pollution. Therefore, it is important to evaluate the contamination at these sites to protect them. Here, we considered a Roman archeological site (Nymphaeum) situated in Amman. The contamination in soil, plants, and building stones did not show spatial distribution within the site. The contamination was the highest in soil (heavy metals 10(4) -10(7) ppb and sulfur similar to 3.5x10(6) ppb) whereas in plants was the least for Cr (similar to 400 ppb) and in building stones it was the least for Cu (similar to 860 ppb). The highest contamination in plants and building stones was found for Al (similar to 5x10(4) and similar to 6.2x10(5) ppb respectively). The sulfur content in plants (similar to 7.6x10(5) ppb) was higher than that in the building stones (similar to 2.3x10(5) ppb). The heavy metals and sulfur contamination in the building stones were lower than what was reported elsewhere outside Jordan.
  • Mohr, Claudia; Lopez-Hilfiker, Felipe D.; Zotter, Peter; Prevot, Andre S. H.; Xu, Lu; Ng, Nga L.; Herndon, Scott C.; Williams, Leah R.; Franklin, Jonathan P.; Zahniser, Mark S.; Worsnop, Douglas R.; Knighton, W. Berk; Aiken, Allison C.; Gorkowski, Kyle J.; Dubey, Manvendra K.; Allan, James D.; Thornton, Joel A. (2013)