Browsing by Subject "BLACK CARBON"

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  • 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.
  • Grythe, Henrik; Kristiansen, Nina I.; Zwaaftink, Christine D. Groot; Eckhardt, Sabine; Strom, Johan; Tunved, Peter; Krejci, Radovan; Stohl, Andreas (2017)
    A new, more physically based wet removal scheme for aerosols has been implemented in the Lagrangian particle dispersion model FLEXPART. It uses three-dimensional cloud water fields from the European Centre for MediumRange Weather Forecasts (ECMWF) to determine cloud extent and distinguishes between in-cloud and below-cloud scavenging. The new in-cloud nucleation scavenging depends on cloud water phase (liquid, ice or mixed-phase), based on the aerosol's prescribed efficiency to serve as ice crystal nuclei and liquid water nuclei, respectively. The impaction scavenging scheme now parameterizes below-cloud removal as a function of aerosol particle size and precipitation type (snow or rain) and intensity. Sensitivity tests with the new scavenging scheme and comparisons with observational data were conducted for three distinct types of primary aerosols, which pose different challenges for modeling wet scavenging due to their differences in solubility, volatility and size distribution: (1) Cs-137 released during the Fukushima nuclear accident attached mainly to highly soluble sulphate aerosol particles, (2) black carbon (BC) aerosol particles, and (3) mineral dust. Calculated e-folding lifetimes of accumulation mode aerosols for these three aerosol types were 11.7, 16.0, and 31.6 days respectively, when well mixed in the atmosphere. These are longer lifetimes than those obtained by the previous removal schem, and, for mineral dust in particular, primarily result from very slow in-cloud removal, which globally is the primary removal mechanism for these accumulation mode particles. Calculated e-folding lifetimes in FLEXPART also have a strong size dependence, with the longest lifetimes found for the accumulation-mode aerosols. For example, for dust particles emitted at the surface the lifetimes were 13.8 days for particles with 1 aem diameter and a few hours for 10 aem particles. A strong size dependence in below-cloud scavenging, combined with increased dry removal, is the primary reason for the shorter lifetimes of the larger particles. The most frequent removal is in-cloud scavenging (85% of all scavenging events) but it occurs primarily in the free troposphere, while below-cloud removal is more frequent below 1000m (52% of all events) and can be important for the initial fate of species emitted at the surface, such as those examined here. For assumed realistic in-cloud removal efficiencies, both BC and sulphate have a slight overestimation of observed atmospheric concentrations (a factor of 1.6 and 1.2 respectively). However, this overestimation is largest close to the sources and thus appears more related to overestimated emissions rather than underestimated removal. The new aerosol wet removal scheme of FLEXPART incorporates more realistic information about clouds and aerosol properties and it compares better with both observed lifetimes and concentration than the old scheme.
  • Kirkevag, Alf; Grini, Alf; Olivie, Dirk; Seland, Oyvind; Alterskjaer, Kari; Hummel, Matthias; Karset, Inger H. H.; Lewinschal, Anna; Liu, Xiaohong; Makkonen, Risto; Bethke, Ingo; Griesfeller, Jan; Schulz, Michael; Iversen, Trond (2018)
    We document model updates and present and discuss modeling and validation results from a further developed production-tagged aerosol module, OsloAero5.3, for use in Earth system models. The aerosol module has in this study been implemented and applied in CAM5.3-Oslo. This model is based on CAM5.3-CESM1.2 and its own predecessor model version CAM4-Oslo. OsloAero5.3 has improved treatment of emissions, aerosol chemistry, particle life cycle, and aerosol-cloud interactions compared to its predecessor OsloAero4.0 in CAM4-Oslo. The main new features consist of improved aerosol sources; the module now explicitly accounts for aerosol particle nucleation and secondary organic aerosol production, with new emissions schemes also for sea salt, dimethyl sulfide (DMS), and marine primary organics. Mineral dust emissions are updated as well, adopting the formulation of CESM1.2. The improved model representation of aerosol-cloud interactions now resolves heterogeneous ice nucleation based on black carbon (BC) and mineral dust calculated by the model and treats the activation of cloud condensation nuclei (CCN) as in CAM5.3. Compared to OsloAero4.0 in CAM4-Oslo, the black carbon (BC) mass concentrations are less excessive aloft, with a better fit to observations. Near-surface mass concentrations of BC and sea salt aerosols are also less biased, while sulfate and mineral dust are slightly more biased. Although appearing quite similar for CAM5.3-Oslo and CAM4-Oslo, the validation results for organic matter (OM) are inconclusive, since both of the respective versions of OsloAero are equipped with a limited number of OM tracers for the sake of computational efficiency. Any information about the assumed mass ratios of OM to organic carbon (OC) for different types of OM sources is lost in the transport module. Assuming that observed OC concentrations scaled by 1.4 are representative for the modeled OM concentrations, CAM5.3-Oslo with OsloAero5.3 is slightly inferior for the very sparsely available observation data. Comparing clear-sky column-integrated optical properties with data from ground-based remote sensing, we find a negative bias in optical depth globally; however, it is not as strong as in CAM4-Oslo, but has positive biases in some areas typically dominated by mineral dust emissions. Aerosol absorption has a larger negative bias than the optical depth globally. This is reflected in a lower positive bias in areas where mineral dust is the main contributor to absorption. Globally, the low bias in absorption is smaller than in CAM4-Oslo. The Angstrom parameter exhibits small biases both globally and regionally, suggesting that the aerosol particle sizes are reasonably well represented. Cloud-top droplet number concentrations over oceans are generally underestimated compared to satellite retrievals, but seem to be overestimated downwind of major emissions of dust and biomass burning sources. Finally, we find small changes in direct radiative forcing at the top of the atmosphere, while the cloud radiative forcing due to anthropogenic aerosols is now more negative than in CAM4-Oslo, being on the strong side compared to the multi-model estimate in IPCC AR5. Although not all validation results in this study show improvement for the present CAM5.3-Oslo version, the extended and updated aerosol module OsloAero5.3 is more advanced and applicable than its predecessor OsloAero4.0, as it includes new parameterizations that more readily facilitate sensitivity and process studies and use in climate and Earth system model studies in general.
  • 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.
  • Xausa, Filippo; Paasonen, Pauli; Makkonen, Risto; Arshinov, Mikhail; Ding, Aijun; Van Der Gon, Hugo Denier; Kerminen, Veli-Matti; Kulmala, Markku (2018)
    Climate models are important tools that are used for generating climate change projections, in which aerosol-climate interactions are one of the main sources of uncertainties. In order to quantify aerosol-radiation and aerosolcloud interactions, detailed input of anthropogenic aerosol number emissions is necessary. However, the anthropogenic aerosol number emissions are usually converted from the corresponding mass emissions in pre-compiled emission inventories through a very simplistic method depending uniquely on chemical composition, particle size and density, which are defined for a few, very wide main source sectors. In this work, the anthropogenic particle number emissions converted from the AeroCom mass in the ECHAM-HAM climate model were replaced with the recently formulated number emissions from the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS) model. In the GAINS model the emission number size distributions vary, for example, with respect to the fuel and technology. Special attention was paid to accumulation mode particles (particle diameter d(p) > 100 nm) because of (i) their capability of acting as cloud condensation nuclei (CCN), thus forming cloud droplets and affecting Earth's radiation budget, and (ii) their dominant role in forming the coagulation sink and thus limiting the concentration of sub-100 nm particles. In addition, the estimates of anthropogenic CCN formation, and thus the forcing from aerosol-climate interactions, are expected to be affected. Analysis of global particle number concentrations and size distributions reveals that GAINS implementation increases CCN concentration compared with AeroCom, with regional enhancement factors reaching values as high as 10. A comparison between modeled and observed concentrations shows that the increase in number concentration for accumulation mode particles agrees well with measurements, but it leads to a consistent underestimation of both nucleation mode and Aitken mode (d(p) <100 nm) particle number concentrations. This suggests that revisions are needed in the new particle formation and growth schemes currently applied in global modeling frameworks.
  • Lihavainen, H.; Alghamdi, M. A.; Hyvärinen, A.; Hussein, T.; Neitola, Kimmo; Khoder, M.; Abdelmaksoud, A. S.; Al-Jeelani, H.; Shabbaj, I. I.; Almehmadi, F. M. (2017)
    To derive the comprehensive aerosol in situ characteristics at a rural background area in Saudi Arabia, an aerosol measurements station was established to Hada Al Sham, 60 km east from the Red Sea and the city of Jeddah. The present sturdy describes the observational data from February 2013 to February 2015 of scattering and absorption coefficients, Angstrom exponents and single scattering albedo over the measurement period. The average scattering and absorption coefficients at wavelength 525 nm were 109 +/- 71 Min(-1) (mean +/- SD, at STP conditions) and 15 +/- 17 Mm(-1) (at STP conditions), respectively. As expected, the scattering coefficient was dominated by large desert dust particles with low Angstrom scattering exponent, 0.49 +/- 0.62. Especially from February to June the Angstrom scattering exponent was clearly lower (0.23) and scattering coefficients higher (124 Mm(-1)) than total averages because of the dust outbreak season. Aerosol optical properties had clear diurnal cycle. The lowest scattering and absorption coefficients and aerosol optical depths were observed around noon. The observed diurnal variation is caused by wind direction and speed, during night time very calm easterly winds are dominating whereas during daytime the stronger westerly winds are dominating (sea breeze). Positive Matrix Factorization mathematical tool was applied to the scattering and absorption coefficients and PM2.5 and coarse mode (PM10-PM2.5) mass concentrations to identify source characteristics. Three different factors with clearly different properties were found; anthropogenic, BC source and desert dust. Mass absorption efficiencies for BC source and desert dust factors were, 6.0 m(2) g(-1) and 0.4 m(2) g(-1), respectively, and mass scattering efficiencies for anthropogenic (sulphate) and desert dust, 2.5 m(2) g(-1) and 0.8 m(2) g(-1), respectively.
  • COST action TD1107 (2017)
    Key priorities in biochar research for future guidance of sustainable policy development have been identified by expert assessment within the COST Action TD1107. The current level of scientific understanding (LOSU) regarding the consequences of biochar application to soil were explored. Five broad thematic areas of biochar research were addressed: soil biodiversity and ecotoxicology, soil organic matter and greenhouse gas (GHG) emissions, soil physical properties, nutrient cycles and crop production, and soil remediation. The highest future research priorities regarding biochar's effects in soils were: functional redundancy within soil microbial communities, bioavailability of biochar's contaminants to soil biota, soil organic matter stability, GHG emissions, soil formation, soil hydrology, nutrient cycling due to microbial priming as well as altered rhizosphere ecology, and soil pH buffering capacity. Methodological and other constraints to achieve the required LOSU are discussed and options for efficient progress of biochar research and sustainable application to soil are presented.
  • Nielsen, Ingeborg E.; Skov, Henrik; Massling, Andreas; Eriksson, Axel C.; Dall'Osto, Manuel; Junninen, Heikki; Sarnela, Nina; Lange, Robert; Collier, Sonya; Zhang, Qi; Cappa, Christopher D.; Nøjgaard, Jacob K. (2019)
    There are limited measurements of the chemical composition, abundance and sources of atmospheric particles in the High Arctic To address this, we report 93 d of soot particle aerosol mass spectrometer (SP-AMS) data collected from 20 February to 23 May 2015 at Villum Research Station (VRS) in northern Greenland (81 degrees 36' N). During this period, we observed the Arctic haze phenomenon with elevated PM1 concentrations ranging from an average of 2.3, 2.3 and 3.3 mu g m(-3) in February, March and April, respectively, to 1.2 mu g m(-3) in May. Particulate sulfate (SO42-) accounted for 66 % of the non-refractory PM1 with the highest concentration until the end of April and decreasing in May. The second most abundant species was organic aerosol (OA) (24 %). Both OA and PM1, estimated from the sum of all collected species, showed a marked decrease throughout May in accordance with the polar front moving north, together with changes in aerosol removal processes. The highest refractory black carbon (rBC) concentrations were found in the first month of the campaign, averaging 0.2 mu g m(-3). In March and April, rBC averaged 0.1 mu g m(-3) while decreasing to 0.02 mu g m(-3) in May. Positive matrix factorization (PMF) of the OA mass spectra yielded three factors: (1) a hydrocarbon-like organic aerosol (HOA) factor, which was dominated by primary aerosols and accounted for 12 % of OA mass, (2) an Arctic haze organic aerosol (AOA) factor and (3) a more oxygenated marine organic aerosol (MOA) factor. AOA dominated until mid-April (64 %-81 % of OA), while being nearly absent from the end of May and correlated significantly with SO42-, suggesting the main part of that factor is secondary OA. The MOA emerged late at the end of March, where it increased with solar radiation and reduced sea ice extent and dominated OA for the rest of the campaign until the end of May (24 %-74 % of OA), while AOA was nearly absent. The highest O/C ratio (0.95) and S/C ratio (0.011) was found for MOA. Our data support the current understanding that Arctic aerosols are highly influenced by secondary aerosol formation and receives an important contribution from marine emissions during Arctic spring in remote High Arctic areas. In view of a changing Arctic climate with changing sea-ice extent, biogenic processes and corresponding source strengths, highly time-resolved data are needed in order to elucidate the components dominating aerosol concentrations and enhance the understanding of the processes taking place.
  • Chauvigné, Aurélien; Aliaga, Diego; Sellegri, Karine; Montoux, Nadège; Krejci, Radovan; Močnik, Griša; Moreno, Isabel; Müller, Thomas; Pandolfi, Marco; Velarde, Fernando; Weinhold, Kay; Ginot, Patrick; Wiedensohler, Alfred; Andrade, Marcos; Laj, Paolo (2019)
    This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multiyear record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm(-1) respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm(-1) respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm(-1) respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.
  • 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.
  • Wang, Yonghong; Gao, Wenkang; Wang, Shuai; Song, Tao; Gong, Zhengyu; Ji, Dongsheng; Wang, Lili; Liu, Zirui; Tang, Guiqian; Huo, Yanfeng; Tian, Shili; Li, Jiayun; Li, Mingge; Yang, Yuan; Chu, Biwu; Petäjä, Tuukka; Kerminen, Veli-Matti; He, Hong; Hao, Jiming; Kulmala, Markku; Wang, Yuesi; Zhang, Yuanhang (2020)
    Although much attention has been paid to investigating and controlling air pollution in China, the trends of air-pollutant concentrations on a national scale have remained unclear. Here, we quantitatively investigated the variation of air pollutants in China using long-term comprehensive data sets from 2013 to 2017, during which Chinese government made major efforts to reduce anthropogenic emission in polluted regions. Our results show a significant decreasing trend in the PM2.5 concentration in heavily polluted regions of eastern China, with an annual decrease of similar to 7% compared with measurements in 2013. The measured decreased concentrations of SO2, NO2 and CO (a proxy for anthropogenic volatile organic compounds) could explain a large fraction of the decreased PM2.5 concentrations in different regions. As a consequence, the heavily polluted days decreased significantly in corresponding regions. Concentrations of organic aerosol, nitrate, sulfate, ammonium and chloride measured in urban Beijing revealed a remarkable reduction from 2013 to 2017, connecting the decreases in aerosol precursors with corresponding chemical components closely. However, surface-ozone concentrations showed increasing trends in most urban stations from 2013 to 2017, which indicates stronger photochemical pollution. The boundary-layer height in capital cities of eastern China showed no significant trends over the Beijing-Tianjin-Hebei, Yangtze River Delta and Pearl River Delta regions from 2013 to 2017, which confirmed the reduction in anthropogenic emissions. Our results demonstrated that the Chinese government was successful in the reduction of particulate matter in urban areas from 2013 to 2017, although the ozone concentration has increased significantly, suggesting a more complex mechanism of improving Chinese air quality in the future.
  • 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)
  • Eriksson, A. C.; Wittbom, C.; Roldin, P.; Sporre, M.; Str M, E.; Nilsson, P.; Martinsson, J.; Rissler, J.; Nordin, E. Z.; Svenningsson, B.; Pagels, J.; Swietlicki, E. (2017)
    Fresh and aged diesel soot particles have different impacts on climate and human health. While fresh diesel soot particles are highly aspherical and non-hygroscopic, aged particles are spherical and hygroscopic. Aging and its effect on water uptake also controls the dispersion of diesel soot in the atmosphere. Understanding the timescales on which diesel soot ages in the atmosphere is thus important, yet knowledge thereof is lacking. We show that under cold, dark and humid conditions the atmospheric transformation from fresh to aged soot occurs on a timescale of less than five hours. Under dry conditions in the laboratory, diesel soot transformation is much less efficient. While photochemistry drives soot aging, our data show it is not always a limiting factor. Field observations together with aerosol process model simulations show that the rapid ambient diesel soot aging in urban plumes is caused by coupled ammonium nitrate formation and water uptake.
  • Ruppel, Meri M.; Soares, Joana; Gallet, Jean-Charles; Isaksson, Elisabeth; Martma, Tonu; Svensson, Jonas; Kohler, Jack; Pedersen, Christina A.; Manninen, Sirkku; Korhola, Atte; Strom, Johan (2017)
    The climate impact of black carbon (BC) is notably amplified in the Arctic by its deposition, which causes albedo decrease and subsequent earlier snow and ice spring melt. To comprehensively assess the climate impact of BC in the Arctic, information on both atmospheric BC concentrations and deposition is essential. Currently, Arctic BC deposition data are very scarce, while atmospheric BC concentrations have been shown to generally decrease since the 1990s. However, a 300-year Svalbard ice core showed a distinct increase in EC (elemental carbon, proxy for BC) deposition from 1970 to 2004 contradicting atmospheric measurements and modelling studies. Here, our objective was to decipher whether this increase has continued in the 21st century and to investigate the drivers of the observed EC deposition trends. For this, a shallow firn core was collected from the same Svalbard glacier, and a regional-to-meso-scale chemical transport model (SILAM) was run from 1980 to 2015. The ice and firn core data indicate peaking EC deposition values at the end of the 1990s and lower values thereafter. The modelled BC deposition results generally support the observed glacier EC variations. However, the ice and firn core results clearly deviate from both measured and modelled atmospheric BC concentration trends, and the modelled BC deposition trend shows variations seemingly independent from BC emission or atmospheric BC concentration trends. wet-deposited at this Svalbard glacier, indicating that meteorological processes such as precipitation and scavenging efficiency have most likely a stronger influence on the BC deposition trend than BC emission or atmospheric concentration trends. BC emission source sectors contribute differently to the modelled atmospheric BC concentrations and BC deposition, which further supports our conclusion that different processes affect atmospheric BC concentration and deposition trends. Consequently, Arctic BC deposition trends should not directly be inferred based on atmospheric BC measurements, and more observational BC deposition data are required to assess the climate impact of BC in Arctic snow.
  • Räisänen, Petri; Makkonen, Risto; Kirkevag, Alf; Debernard, Jens B. (2017)
    Snow consists of non-spherical grains of various shapes and sizes. Still, in radiative transfer calculations, snow grains are often treated as spherical. This also applies to the computation of snow albedo in the Snow, Ice, and Aerosol Radiation (SNICAR) model and in the Los Alamos sea ice model, version 4 (CICE4), both of which are employed in the Community Earth System Model and in the Norwegian Earth System Model (NorESM). In this study, we evaluate the effect of snow grain shape on climate simulated by NorESM in a slab ocean configuration of the model. An experiment with spherical snow grains (SPH) is compared with another (NONSPH) in which the snow shortwave single-scattering properties are based on a combination of three non-spherical snow grain shapes optimized using measurements of angular scattering by blowing snow. The key difference between these treatments is that the asymmetry parameter is smaller in the non-spherical case (0.77-0.78 in the visible region) than in the spherical case (similar to 0.89). Therefore, for the same effective snow grain size (or equivalently, the same specific projected area), the snow broadband albedo is higher when assuming non-spherical rather than spherical snow grains, typically by 0.02-0.03. Considering the spherical case as the baseline, this results in an instantaneous negative change in net shortwave radiation with a global-mean top-of-the-model value of ca. -0.22Wm(-2). Although this global-mean radiative effect is rather modest, the impacts on the climate simulated by NorESM are substantial. The global annual-mean 2m air temperature in NONSPH is 1.17K lower than in SPH, with substantially larger differences at high latitudes. The climatic response is amplified by strong snow and sea ice feedbacks. It is further demonstrated that the effect of snow grain shape could be largely offset by adjusting the snow grain size. When assuming non-spherical snow grains with the parameterized grain size increased by ca. 70 %, the climatic differences to the SPH experiment become very small. Finally, the impact of assumed snow grain shape on the radiative effects of absorbing aerosols in snow is discussed.
  • Petäjä, T.; Järvi, L.; Kerminen, V. -M.; Ding, A. J.; Sun, J. N.; Nie, W.; Kujansuu, J.; Virkkula, A.; Yang, X. -Q.; Fu, C. B.; Zilitinkevich, S.; Kulmala, M. (2016)
    Severe air pollution episodes have been frequent in China during the recent years. While high emissions are the primary reason for increasing pollutant concentrations, the ultimate cause for the most severe pollution episodes has remained unclear. Here we show that a high concentration of particulate matter (PM) will enhance the stability of an urban boundary layer, which in turn decreases the boundary layer height and consequently cause further increases in PM concentrations. We estimate the strength of this positive feedback mechanism by combining a new theoretical framework with ambient observations. We show that the feedback remains moderate at fine PM concentrations lower than about 200 mu g m(-3), but that it becomes increasingly effective at higher PM loadings resulting from the combined effect of high surface PM emissions and massive secondary PM production within the boundary layer. Our analysis explains why air pollution episodes are particularly serious and severe in megacities and during the days when synoptic weather conditions stay constant.
  • Poom, Age; Willberg, Elias; Toivonen, Tuuli (2021)
    Daily travel through the urban fabric exposes urban dwellers to a range of environmental conditions that may have an impact on their health and wellbeing. Knowledge about exposures during travel, their associations with travel behavior, and their social and health outcomes are still limited. In our review, we aim to explain how the current environmental exposure research addresses the interactions between human and environmental systems during travel through their spatial, temporal and contextual dimensions. Based on the 104 selected studies, we identify significant recent advances in addressing the spatiotemporal dynamics of exposure during travel. However, the conceptual and methodological framework for understanding the role of multiple environmental exposures in travel environments is still in an early phase, and the health and wellbeing impacts at individual or population level are not well known. Further research with greater geographical balance is needed to fill the gaps in the empirical evidence, and linking environmental exposures during travel with the causal health and wellbeing outcomes. These advancements can enable evidence-based urban and transport planning to take the next step in advancing urban livability.
  • Nieminen, Tuomo; Kerminen, Veli-Matti; Petäjä, Tuukka; Aalto, Pasi P.; Arshinov, Mikhail; Asmi, Eija; Baltensperger, Urs; Beddows, David C. S.; Beukes, Johan Paul; Collins, Don; Ding, Aijun; Harrison, Roy M.; Henzing, Bas; Hooda, Rakesh; Hu, Min; Horrak, Urmas; Kivekäs, Niku; Komsaare, Kaupo; Krejci, Radovan; Kristensson, Adam; Laakso, Lauri; Laaksonen, Ari; Leaitch, W. Richard; Lihavainen, Heikki; Mihalopoulos, Nikolaos; Nemeth, Zoltan; Nie, Wei; O'Dowd, Colin; Salma, Imre; Sellegri, Karine; Svenningsson, Birgitta; Swietlicki, Erik; Tunved, Peter; Ulevicius, Vidmantas; Vakkari, Ville; Vana, Marko; Wiedensohler, Alfred; Wu, Zhijun; Virtanen, Annele; Kulmala, Markku (2018)
    Atmospheric new particle formation (NPF) is an important phenomenon in terms of global particle number concentrations. Here we investigated the frequency of NPF, formation rates of 10 nm particles, and growth rates in the size range of 10-25 nm using at least 1 year of aerosol number size-distribution observations at 36 different locations around the world. The majority of these measurement sites are in the Northern Hemisphere. We found that the NPF frequency has a strong seasonal variability. At the measurement sites analyzed in this study, NPF occurs most frequently in March-May (on about 30 % of the days) and least frequently in December-February (about 10 % of the days). The median formation rate of 10 nm particles varies by about 3 orders of magnitude (0.01-10 cm(-3) s(-1)) and the growth rate by about an order of magnitude (1-10 nm h(-1)). The smallest values of both formation and growth rates were observed at polar sites and the largest ones in urban environments or anthropogenically influenced rural sites. The correlation between the NPF event frequency and the particle formation and growth rate was at best moderate among the different measurement sites, as well as among the sites belonging to a certain environmental regime. For a better understanding of atmospheric NPF and its regional importance, we would need more observational data from different urban areas in practically all parts of the world, from additional remote and rural locations in North America, Asia, and most of the Southern Hemisphere (especially Australia), from polar areas, and from at least a few locations over the oceans.
  • Doulgeris, Konstantinos-Matthaios; Komppula, Mika; Romakkaniemi, Sami; Hyvarinen, Antti-Pekka; Kerminen, Veli-Matti; Brus, David (2020)
    Continuous, semi-long-term, ground-based in situ cloud measurements were conducted during the Pallas Cloud Experiment (PaCE) in 2013. The measurements were carried out in Finnish sub-Arctic region at Sammaltunturi station (67 degrees 58 ' N, 24 degrees 07 ' E; 560m a.s.l.), part of Pallas Atmosphere - Ecosystem Supersite and Global Atmosphere Watch (GAW) program. The main motivation of the campaign was to conduct in situ cloud measurements with three different cloud spectrometer probes and perform an evaluation of their ground-based setups. Therefore, we mutually compared the performance of the cloud and aerosol spectrometer (CAS), the cloud droplet probe (CDP) and the forward-scattering spectrometer probe (FSSP-100) (DMT; Boulder, CO, USA). We investigated how different meteorological parameters affect each instrument's ground-based setup operation and quantified possible biases and discrepancies of different microphysical cloud properties. Based on the obtained results we suggested limitations for further use of the instrument setups in campaigns where the focus is on investigating aerosol-cloud interactions. Measurements in this study were made by instruments owned by the Finnish Meteorological Institute and results concern their operation in sub-Arctic conditions with frequently occurring supercooled clouds. The measured parameter from each instrument was the size distribution, and additionally we derived the number concentration, the effective diameter, the median volume diameter and the liquid water content. A complete intercomparison between the CAS probe and the FSSP-100 ground setups and additionally between the FSSP-100 and the CDP probe ground setups was made and presented. Unfortunately, there was not a sufficient amount of common data to compare all three probes together due to operational problems of the CDP ground setup in sub-zero conditions. The CAS probe that was fixed to one direction lost a significant number of cloud droplets when the wind direction was out of wind iso-axial conditions in comparison with the FSSP-100 and the CDP, which were both placed on a rotating platform. We revealed that CAS and FSSP-100 had good agreement in deriving sizing parameters (effective diameter and median volume diameter from 5 to 35 mu m) even though CAS was losing a significant amount of cloud droplets. The most sensitive derived parameter was liquid water content, which was strongly connected to the wind direction and temperature.