61. Absorption enhancement of black carbon particles in a Mediterranean city and countryside : effect of particulate matter chemistry, ageing and trend analysisJesús Yus-Díez, Marta Via, Andrés Alastuey, Angeliki Karanasiou, Maria Cruz Minguillon, Noemí Perez, Xavier Querol, Cristina Reche, Matic Ivančič, Martin Rigler, 2022, izvirni znanstveni članek Opis: Abstract. Black carbon (BC) is recognized as the most important warming agent among atmospheric aerosol particles. The absorption efficiency of pure BC is rather well-known, nevertheless the mixing of BC with other aerosol particles can enhance the BC light absorption efficiency, thus directly affecting Earth's radiative balance. The effects on climate of the BC absorption enhancement due to the mixing with these aerosols are not yet well constrained because these effects depend on the availability of material for mixing with BC, thus creating regional variations. Here we present the mass absorption cross-section (MAC) and absorption enhancement of BC particles (Eabs), at different wavelengths (from 370 to 880 nm for online measurements and at 637 nm for offline measurements) measured at two sites in the western Mediterranean, namely Barcelona (BCN; urban background) and Montseny (MSY; regional background). The Eabs values ranged between 1.24 and 1.51 at the urban station, depending on the season and wavelength used as well as on the pure BC MAC used as a reference. The largest contribution to Eabs was due to the internal mixing of BC particles with other aerosol compounds, on average between a 91 % and a 100 % at 370 and 880 nm, respectively. Additionally, 14.5 % and 4.6 % of the total enhancement at the short ultraviolet (UV) wavelength (370 nm) was due to externally mixed brown carbon (BrC) particles during the cold and the warm period, respectively. On average, at the MSY station, a higher Eabs value was observed (1.83 at 637 nm) compared to BCN (1.37 at 637 nm), which was associated with the higher fraction of organic aerosols (OA) available for BC coating at the regional station, as denoted by the higher organic carbon to elemental carbon (OC:EC) ratio observed at MSY compared to BCN. At both BCN and MSY, Eabs showed an exponential increase with the amount of non-refractory (NR) material available for coating (RNR-PM). The Eabs at 637 nm at the MSY regional station reached values up to 3 during episodes with high RNR-PM, whereas in BCN, Eabs kept values lower than 2 due to the lower relative amount of coating materials measured at BCN compared to MSY. The main sources of OA influencing Eabs throughout the year were hydrocarbon OA (HOA) and cooking-related OA (COA), i.e. primary OA (POA) from traffic and cooking emissions, respectively, at both 370 and 880 nm. At the short UV wavelength (370 nm), a strong contribution to Eabs from biomass burning OA (BBOA) and less oxidized oxygenated OA (LO-OOA) sources was observed in the colder period. Moreover, we found an increase of Eabs with the ageing state of the particles, especially during the colder period. This increase of Eabs with particle ageing was associated with a larger relative amount of secondary OA (SOA) compared to POA. The availability of a long dataset at both stations from offline measurements enabled a decade-long trend analysis of Eabs at 637 nm, that showed statistically significant (s.s.) positive trends of Eabs during the warmer months at the MSY station. This s.s. positive trend in MSY mirrored the observed increase of the OC:EC ratio over time. Moreover, in BCN during the COVID-19 lockdown period in spring 2020 we observed a sharp increase of Eabs due to the observed sharp increase of the OC:EC ratio. Our results show similar values of Eabs to those found in the literature for similar background stations.
Ključne besede: black carbomn, coating, organic aerosol, light absorption
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62. The potential of high temporal resolution automatic measurements of ▫$PM_2.5$▫ composition as an alternative to the filter-based manual method used in routine monitoringMarsailidh M. Twigg, Chiara F. Di Marco, Elizabeth A. McGhee, Christine F. Braban, Eiko Nemitz, Richard J. C. Brown, Kevin C. Blakley, Sarah R. Leeson, Agnieszka Sanocka, Marta Via, 2023, izvirni znanstveni članek Ključne besede: PM2.5, inorganic aerosol, ACSM, HR-TOF-AMS, MARGA, AIM
Objavljeno v RUNG: 10.05.2024; Ogledov: 165; Prenosov: 1
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63. A European aerosol phenomenology - 7 : high-time resolution chemical characteristics of submicron particulate matter across EuropeM. Bressi, F. Cavalli, Jean-Philippe Putaud, R. Fröhlich, J. -E. Petit, W. Aas, M. Äijälä, A. Alastuey, J. D. Allan, M. Aurela, Iasonas Stavroulas, Marta Via, 2021, izvirni znanstveni članek Opis: Similarities and differences in the submicron atmospheric aerosol chemical composition are analyzed from a unique set of measurements performed at 21 sites across Europe for at least one year. These sites are located between 35 and 62°N and 10° W – 26°E, and represent various types of settings (remote, coastal, rural, industrial, urban). Measurements were all carried out on-line with a 30-min time resolution using mass spectroscopy based instruments known as Aerosol Chemical Speciation Monitors (ACSM) and Aerosol Mass Spectrometers (AMS) and following common measurement guidelines. Data regarding organics, sulfate, nitrate and ammonium concentrations, as well as the sum of them called non-refractory submicron aerosol mass concentration ([NR-PM1]) are discussed. NR-PM1 concentrations generally increase from remote to urban sites. They are mostly larger in the mid-latitude band than in southern and northern Europe. On average, organics account for the major part (36–64%) of NR-PM1 followed by sulfate (12–44%) and nitrate (6–35%). The annual mean chemical composition of NR-PM1 at rural (or regional background) sites and urban background sites are very similar. Considering rural and regional background sites only, nitrate contribution is higher and sulfate contribution is lower in mid-latitude Europe compared to northern and southern Europe. Large seasonal variations in concentrations (μg/m³) of one or more components of NR-PM1 can be observed at all sites, as well as in the chemical composition of NR-PM1 (%) at most sites. Significant diel cycles in the contribution to [NR-PM1] of organics, sulfate, and nitrate can be observed at a majority of sites both in winter and summer. Early morning minima in organics in concomitance with maxima in nitrate are common features at regional and urban background sites. Daily variations are much smaller at a number of coastal and rural sites. Looking at NR-PM1 chemical composition as a function of NR-PM1 mass concentration reveals that although organics account for the major fraction of NR-PM1 at all concentration levels at most sites, nitrate contribution generally increases with NR-PM1 mass concentration and predominates when NR-PM1 mass concentrations exceed 40 μg/m³ at half of the sites.
Ključne besede: aerosol, chemical composition, mass spectrometry, phenomenology
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64. Assessment of the COVID-19 lockdown effects on spectral aerosol scattering and absorption properties in Athens, GreeceDimitris G. Kaskaoutis, Georgios Grivas, Eleni Liakakou, Nikos Kalivitis, Giorgos Kouvarakis, Iasonas Stavroulas, Panayiotis Kalkavouras, Pavlos Zarmpas, Umesh Chandra Dumka, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2021, izvirni znanstveni članek Opis: COVID-19 is evolving into one of the worst pandemics in recent history, claiming a death toll of over 1.5 million as of December 2020. In an attempt to limit the expansion of the pandemic in its initial phase, nearly all countries imposed restriction measures, which resulted in an unprecedented reduction of air pollution. This study aims to assess the impact of the lockdown effects due to COVID-19 on in situ measured aerosol properties, namely spectral-scattering (bsca) and absorption (babs) coefficients, black carbon (BC) concentrations, single-scattering albedo (SSA), scattering and absorption Ångström exponents (SAE, AAE) in Athens, Greece. Moreover, a comparison is performed with the regional background site of Finokalia, Crete, for a better assessment of the urban impact on observed differences. The study examines pre-lockdown (1–22 March 2020), lockdown (23 March–3 May 2020) and post-lockdown (4–31 May 2020) periods, while the aerosol properties are also compared with a 3–4 year preceding period (2016/2017–2019). Comparison of meteorological parameters in Athens, between the lockdown period and respective days in previous years, showed only marginal variation, which is not deemed sufficient in order to justify the notable changes in aerosol concentrations and optical properties. The largest reduction during the lockdown period was observed for babs compared to the pre-lockdown (−39%) and to the same period in previous years (−36%). This was intensified during the morning traffic hours (−60%), reflecting the large decrease in vehicular emissions. Furthermore, AAE increased during the lockdown period due to reduced emissions from fossil-fuel combustion, while a smaller (−21%) decrease was observed for bsca along with slight increases (6%) in SAE and SSA values, indicating that scattering aerosol properties were less affected by the decrease in vehicular emissions, as they are more dependent on regional sources and atmospheric processing. Nighttime BC emissions related to residential wood-burning were slightly increased during the lockdown period, with respect to previous-year means. On the contrary, aerosol and pollution changes during the lockdown period at Finokalia were low and highly sensitive to natural sources and processes.
Ključne besede: COVID-19, traffic, aerosol scattering, absorption, SSA, Greece
Objavljeno v RUNG: 10.05.2024; Ogledov: 169; Prenosov: 3
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65. Apportionment of black and brown carbon spectral absorption sources in the urban environment of Athens, Greece, during winterDimitris G. Kaskaoutis, Georgios Grivas, Iasonas Stavroulas, Aikaterini Bougiatioti, Eleni Liakakou, Umesh Chandra Dumka, Evangelos Gerasopoulos, Nikolaos Mihalopoulos, 2021, izvirni znanstveni članek Opis: This study examines the spectral properties and source characteristics of absorbing aerosols (BC: Black Carbon; BrC: Brown Carbon, based on aethalometer measurements) in the urban background of Athens during December 2016–February 2017. Using common assumptions regarding the spectral dependence of absorption due to BC (AAEBC = 1) and biomass burning (AAEbb = 2), and calculating an optimal AAEff value for the dataset (1.18), the total spectral absorption was decomposed into five components, corresponding to absorption of BC and BrC from fossil-fuel (ff) combustion and biomass burning (bb), and to secondary BrC estimated using the BC-tracer minimum R-squared (MRS) method. Substantial differences in the contribution of various components to the total absorption were found between day and night, due to differences in emissions and meteorological dynamics, while BrC and biomass burning aerosols presented higher contributions at shorter wavelengths. At 370 nm, the absorption due to BCff contributed 36.3% on average, exhibiting a higher fraction (58.1%) during daytime, while the mean BCbb absorption was estimated at 18.4%. The mean absorption contributions due to BrCff, BrCbb and BrCsec were 6.7%, 32.3% and 4.9%, respectively. The AbsBCff,370 component maximized during the morning traffic hours and was strongly correlated with NOx (R2 = 0.76) and CO (R2 = 0.77), while a similar behavior was seen for the AbsBrCff,370 component. AbsBCbb and AbsBrCbb levels escalated during nighttime and were highly associated with nss-K+ and with the organic aerosol (OA) components related to fresh and fast-oxidized biomass burning (BBOA and SV-OOA) as obtained from ACSM measurements. Multiple linear regression was used to attribute BrC absorption to five OA components and to determine their absorption contributions and efficiencies, revealing maximum contributions of BBOA (33%) and SV-OOA (21%). Sensitivity analysis was performed in view of the methodological uncertainties and supported the reliability of the results, which can have important implications for radiative transfer models.
Ključne besede: spectral absorption, black carbon, brown carbon, fossil fuel, biomass burning, source apportionment
Objavljeno v RUNG: 10.05.2024; Ogledov: 196; Prenosov: 0
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66. Impacts of severe residential wood burning on atmospheric processing, water-soluble organic aerosol and light absorption, in an inland city of Southeastern EuropeDimitris G. Kaskaoutis, Georgios Grivas, K. Oikonomou, P. Tavernaraki, Kyriaki Papoutsidaki, M. Tsagkaraki, Iasonas Stavroulas, Pavlos Zarmpas, D. Paraskevopoulou, Aikaterini Bougiatioti, 2022, izvirni znanstveni članek Opis: This study examines the concentrations and characteristics of carbonaceous aerosols (including saccharides) and inorganic species measured by PM2.5 filter sampling and a multi-wavelength Aethalometer during two campaigns in a mountainous, medium-sized, Greek city (Ioannina). The first campaign was conducted in summer and used as a baseline of low concentrations, while the second took place in winter under intensive residential wood burning (RWB) emissions. Very high winter-mean OC concentrations (26.0 μg m−3) were observed, associated with an OC/EC ratio of 9.9, and mean BCwb and PM2.5 levels of 4.5 μg m−3 and 57.5 μg m−3, respectively. Simultaneously, record-high levoglucosan (Lev) concentrations (mean: 6.0 μg m−3; max: 15.9 μg m−3) were measured, revealing a severely biomass burning (BB)-laden environment. The water-soluble OC component (WSOC) accounted for 56 ± 9% of OC in winter, exhibiting high correlations (R2 = 0.93–0.97) with BB tracers (nss-K+, BCwb, Lev), nitrate and light absorption, potentially indicating the formation of water-soluble brown carbon (BrC) from fast oxidation processes. The examination of diagnostic ratios involving BB tracers indicated the prevalence of hardwood burning, while the mean Lev/OC ratio (22%) was remarkably higher than literature values. Applying a mono-tracer method based on levoglucosan, we estimated very high BB contributions to OC (∼92%), EC (∼64%) and WSOC (∼87%) during winter. On the contrary, low levels were registered during summer for all carbonaceous components, with winter/summer ratios of 4–5 for PM2.5 and BC, 10 for OC, 30 for BCwb and ∼1100 for levoglucosan. The absence of local BB sources in summer, combined with the photochemical processing and aging of regional organic aerosols, resulted in higher WSOC/OC fractions (64 ± 13%). The results indicate highly soluble fine carbonaceous aerosol fraction year-round, which when considered alongside the extreme concentration levels in winter can have important implications for short- and long-term health effects.
Ključne besede: carbonaceous aerosols, biomass burning, levoglucosan, WSOC, heterogeneous chemistry, Greece
Objavljeno v RUNG: 10.05.2024; Ogledov: 201; Prenosov: 2
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67. Development and evaluation of an improved offline aerosol mass spectrometry techniqueChristina Vasilakopoulou, Kalliopi Florou, Christos Kaltsonoudis, Iasonas Stavroulas, Nikolaos Mihalopoulos, Spyros N. Pandis, 2023, izvirni znanstveni članek Opis: Abstract. The offline aerosol mass spectrometry technique is
a useful tool for the source apportionment of organic aerosol (OA) in areas
and periods during which an aerosol mass spectrometer (AMS) is not available. However, the technique is
based on the extraction of aerosol samples in water, while several
atmospheric OA components are partially or fully insoluble in water. In this work an improved offline technique was developed and evaluated in an effort to capture most of the partially soluble and insoluble organic aerosol material, reducing significantly the uncertainty of the corresponding source
apportionment. A major advantage of the proposed approach is that no
corrections are needed for the offline analysis to account for the limited
water solubility of some OA components. The improved offline AMS analysis
was tested in three campaigns: two during winter and one during summer.
Collocated online AMS measurements were performed for the evaluation of the offline method. Source apportionment analysis was performed separately for the online and the offline measurements using positive matrix
factorization (PMF). The PMF results showed that the fractional contribution of each factor to the total OA differed between the online and the offline PMF results by less than 15 %. The differences in the AMS spectra of the
factors of the two approaches could be significant, suggesting that the use
of factor profiles from the literature in the offline analysis may lead to
complications. Part of the good agreement between the online and the
offline PMF results is due to the ability of the improved offline AMS
technique to capture a bigger part of the OA, including insoluble organic
material. This was evident by the significant fraction of submicrometer
suspended insoluble particles present in the water extract and by the
reduced insoluble material on the filters after the extraction process. More than half of the elemental carbon (EC) was on average missing from the
filters after the water extraction. Significant EC concentrations were
measured in the produced aerosol that was used as input to the AMS during
the offline analysis.
Ključne besede: organic aerosol, receptor modeling, offline PMF, Greece
Objavljeno v RUNG: 10.05.2024; Ogledov: 187; Prenosov: 2
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68. Ambient carbonaceous aerosol levels in Cyprus and the role of pollution transport from the Middle EastAliki Christodoulou, Iasonas Stavroulas, Mihalis Vrekoussis, Maximillien Desservettaz, Michael Pikridas, Elie Bimenyimana, Jonilda Kushta, Matic Ivančič, Martin Rigler, Philippe Goloub, 2023, izvirni znanstveni članek Opis: Abstract. The geographical origin and source apportionment of submicron carbonaceous aerosols (organic aerosols, OAs, and black carbon, BC) have been investigated here for the first time, deploying high time-resolution measurements at an urban background site of Nicosia, the capital
city of Cyprus, in the eastern Mediterranean. This study covers a half-year
period, encompassing both the cold and warm periods with continuous
observations of the physical and chemical properties of PM1 performed
with an Aerosol Chemical Speciation Monitor (ACSM), an aethalometer,
accompanied by a suite of various ancillary offline and online measurements. Carbonaceous aerosols were dominant during both seasons (cold and warm periods), with a contribution of 57 % and 48 % to PM1, respectively, and exhibited recurrent intense nighttime peaks (> 20–30 µg m−3) during the cold period, associated with local domestic heating. The findings of this study show that high concentrations of sulfate (close to 3 µg m−3) were continuously recorded, standing among the highest ever reported for Europe and originating from the Middle East region. Source apportionment of the OA and BC fractions was performed using the
positive matrix factorization (PMF) approach and the combination of two
models (aethalometer model and multilinear regression), respectively. Our
study revealed elevated hydrocarbon-like organic aerosol (HOA)
concentrations in Nicosia (among the highest reported for a European urban
background site), originating from a mixture of local and regional
fossil fuel combustion sources. Although air masses from the Middle East had
a low occurrence and were observed mostly during the cold period, they were
shown to strongly affect the mean concentrations levels of BC and OA in
Nicosia during both seasons. Overall, the present study brings to our
attention the need to further characterize primary and secondary
carbonaceous aerosols in the Middle East, an undersampled region
characterized by continuously increasing fossil fuel (oil and gas) emissions
and extreme environmental conditions, which can contribute to photochemical
ageing.
Ključne besede: PM1, BC, source apportionment, Cyprus, long range transport
Objavljeno v RUNG: 10.05.2024; Ogledov: 195; Prenosov: 2
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69. Impact of peri-urban forest fires on air quality and aerosol optical and chemical properties : the case of the August 2021 wildfires in Athens, GreeceDimitris G. Kaskaoutis, Kalliopi Petrinoli, Georgios Grivas, Panayiotis Kalkavouras, M. Tsagkaraki, Kyriaki Papoutsidaki, Iasonas Stavroulas, D. Paraskevopoulou, Aikaterini Bougiatioti, 2024, izvirni znanstveni članek Ključne besede: biomass burning, carbonaceous aerosols, scattering, absorption, chemical composition, Mediterranean
Objavljeno v RUNG: 10.05.2024; Ogledov: 189; Prenosov: 0
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70. Intra- and inter-city variability of ▫$PM_2.5$▫ concentrations in Greece as determined with a low-cost sensor networkKonstantinos Dimitriou, Iasonas Stavroulas, Georgios Grivas, Charalampos Chatzidiakos, Georgios Kosmopoulos, Andreas Kazantzidis, Konstantinos Kourtidis, Athanasios Karagioras, Nikolaos Hatzianastassiou, Spyros N. Pandis, 2023, izvirni znanstveni članek Opis: Measurements of PM2.5 concentrations in five major Greek cities over a two-year period using calibrated low-cost sensor-based particulate matter (PM) monitors (Purple Air PA-II) were combined with local meteorological parameters, synoptic patterns and air mass residence time models to investigate the factors controlling PM2.5 spatiotemporal variability over continental Greece. Fourteen sensors nodes in Athens, Patras, Ioannina, Xanthi, and Thermi (in the Metropolitan Area of Thessaloniki) were selected out of more than 100 of a countrywide network for detailed analysis. The cities have populations ranging from 65k to 3M inhabitants and cover different latitudes along the South-North axis. High correlations between the daily average PM2.5 levels were observed among all sites, indicating strong intra- and inter-city covariance of concentrations, both in cold and warm periods. Higher PM2.5 concentrations in all cities during the cold period were primarily associated with low temperatures and stagnant anticyclonic conditions, favoring the entrapment of residential heating emissions from biomass burning. Anticyclonic conditions were also connected to an increased frequency of PM2.5 episodes, exceeding the updated daily guideline value (15 μg m−3) of the World Health Organization (WHO). During the warm period, nearly uniform PM2.5 levels were encountered across continental Greece, independently of their population size. This uniformity strongly suggests the importance of long-range transport and regional secondary aerosol formation for PM2.5 during this period. Peak concentrations were associated mainly with regional northern air flows over Greece and the Balkan Peninsula. The use of the measurements from dense air quality sensor networks, provided that a robust calibration protocol and continuous data quality assurance practices are followed, appears to be an efficient tool to gain insights on the levels and variability of PM2.5 concentrations, underpinning the characterization of spatial and seasonal particularities and supporting real-time public information and warning.
Ključne besede: particulate matter, PM2.5, biomass burning, low-cost sensors, purple air PA-II, concentration weighted trajectory, potential source contribution function
Objavljeno v RUNG: 10.05.2024; Ogledov: 200; Prenosov: 2
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