1. Characterization of brown carbon absorption in different European environments through source contribution analysisHector Navarro-Barboza, Jordi Rovira, Vincenzo Obiso, Andrea Pozzer, Marta Via, Andrés Alastuey, Xavier Querol, Jesús Yus-Díez, Matic Ivančič, Martin Rigler, 2025, original scientific article Abstract: Brown carbon (BrC) is a fraction of organic aerosol (OA) that absorbs radiation in the ultraviolet and short visible wavelengths. Its contribution to radiative forcing is uncertain due to limited knowledge of its imaginary refractive index (k). This study investigates the variability of k for OA from wildfires, residential, shipping, and traffic emission sources over Europe. The Multiscale Online Nonhydrostatic Atmosphere Chemistry (MONARCH) model simulated OA concentrations and source contributions, feeding an offline optical tool to constrain k values at 370 nm. The model was evaluated against OA mass concentrations from aerosol chemical speciation monitors (ACSMs) and filter sample measurements, as well as aerosol light absorption measurements at 370 nm derived from an Aethalometer™ from 12 sites across Europe. Results show that MONARCH captures the OA temporal variability across environments (regional, suburban, and urban background). Residential emissions are a major OA source in colder months, while secondary organic aerosol (SOA) dominates in warmer periods. Traffic is a minor primary OA contributor. Biomass and coal combustion significantly influence OA absorption, with shipping emissions also notable near harbors. Optimizing k values at 370 nm revealed significant variability in OA light absorption, influenced by emission sources and environmental conditions. Derived k values for biomass burning (0.03 to 0.13), residential (0.008 to 0.13), shipping (0.005 to 0.08), and traffic (0.005 to 0.07) sources improved model representation of OA absorption compared to a constant k. Introducing such emission source-specific constraints is an innovative approach to enhance OA absorption in atmospheric models.
Keywords: aerosols, brown carbon, source contribution analysis
Published in RUNG: 04.03.2025; Views: 641; Downloads: 6
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3. Two-dimensional BC tracer model to distinguish between primary and secondary OC : lecture at The European Aerosol Conference 2024, 25. 8.-30. 8. 2024, Tampere, FinlandMatic Ivančič, Asta Gregorič, Gašper Lavrič, Bálint Alföldy, Irena Ježek, Iasonas Stavroulas, Martin Rigler, 2024, unpublished conference contribution Abstract: In this work, we propose an extension of this method. Using the Aethalometer model (Sandradewi et al., 2008), BC as a tracer for primary emitted aerosols can be successfully divided into two components – BCff related to the usage of fossil fuels and BCbb emitted from biomass burning. Because the OC/BC ratio is expected to be different for fossil fuels and biomass burning, we can similarly introduce the two components of POC – a fossil fuel-related POCff and a biomass-burning-related POCbb.
Keywords: BC tracer model, secondary organic carbon, black carbon
Published in RUNG: 14.11.2024; Views: 993; Downloads: 4
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4. 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, original scientific article Abstract: 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.
Keywords: black carbomn, coating, organic aerosol, light absorption
Published in RUNG: 10.05.2024; Views: 1681; Downloads: 5
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5. 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, original scientific article Abstract: 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.
Keywords: PM1, BC, source apportionment, Cyprus, long range transport
Published in RUNG: 10.05.2024; Views: 1400; Downloads: 6
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6. Particulate air pollution in the heart of the European Union : lessons learned from SAFICA 2017-2018 and SAAERO 2022-2023 projects in Central and Southeast EuropeKatja Džepina, Kristina Glojek, Martin Rigler, Asta Gregorič, Matic Ivančič, Irena Ježek, Griša Močnik, 2024, published scientific conference contribution abstract Abstract: Particularly during the cold weather season, countries of the Southeast Europe are experiencing some of the poorest air quality in the world due to the extensive use of solid fuels and old vehicle fleets. The city of Sarajevo is the capital of Bosnia and Herzegovina (BiH) situated within a basin surrounded by mountains. In the winter months (domestic heating season), topography and meteorology cause the pollutants to be trapped within the city basin. Countries of the Southeast Europe lack state-of-the-art atmospheric sciences research and access to sophisticated instrumentation and methodology, despite high levels of ambient pollution and position within the European Union (EU) borders, making it imperative to understand the emission sources, processing and the adverse health effects of atmospheric aerosol pollution.
This presentation will highlight the field measurements in Central and Southeast Europe during the Sarajevo Canton Winter Field Campaign 2017-2018 (SAFICA) and Sarajevo Aerosol Experiment 2022-2023 (SAAERO) projects, centered at the Sarajevo Bjelave supersite. Both projects were envisioned to produce crucial, not previously available information about aerosol emission sources and atmospheric transformations through a combination of online field and offline laboratory measurements. Online measurements during a) SAFICA and b) SAAERO included, a) black carbon, particle number and size distribution, and b) carbonaceous species, elemental composition and bulk chemical composition. SAAERO online measurements also included stationary and mobile measurements of gas- and particle-phase species on board the mobile laboratory in Sarajevo and Zenica, BiH, as well as in Ljubljana, Slovenia and Zagreb, Croatia. Finally, extended SAAERO project included measurements of black carbon at three additional urban centers: Ljubljana, Zagreb, and Belgrade, Serbia, enabling the first comparison of urban air quality in Central and Southeast Europe between two EU and two non-EU capitals.
During both projects, laboratory aerosol analyses determined aerosol bulk chemical composition, selected elements (Huremović et al., 2020; Žero et al., 2022) and molecular species (Pehnec et al., 2020). Aerosol chemical composition determined by aerosol mass spectrometry was further analyzed by Positive Matrix Factorization to separate organic aerosol into subtypes characteristic of specific sources and atmospheric processes. Aerosol oxidative potential was also determined to evaluate aerosol ability to generate reactive oxygen species. Sarajevo and Belgrade have high ambient loadings of aerosol and black carbon, indicative of strong and diverse combustion sources and a major public health hazard. Finally, aerosol surface concentrations will be discussed in the context of European air quality.
We thank Jasminka Džepina, Magee Scientific/Aerosol, TSI and Aerodyne for support. We acknowledge the contribution of the COST Action CA16109 COLOSSAL and SEE Change Net. KDž and ASHP acknowledge the grant by the Swiss NSF (Scientific Exchanges IZSEZ0_189495), KDž, GM and ASHP European Commission SAAERO grant (EU H2020 MSCA-IF 2020 #101028909), GM Slovenian ARIS grant (P1-0385), SF Croatian HRZZ grant (BiREADI IP-2018-01-3105), and AG, MR, MI, BA and IBJ Slovenian ARIS grant (L1-4386).
Pehnec, G., et al., Sci. Tot. Environ., 734, 139414, 2020.
Huremović, J., et al., Air Qual. Atmos. Health, 13, 965–976, 2020.
Žero, S., Žužul, S., et al., Environ. Sci. Technol., 56, 7052−7062, 2022.
Keywords: air pollution, sources of pollution, PMF
Published in RUNG: 18.03.2024; Views: 3261; Downloads: 7
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7. Heating rate and energy gradient from the tropics to the North PoleLuca Ferrero, Martin Rigler, Asta Gregorič, Griša Močnik, 2024, published scientific conference contribution abstract Abstract: Absorbing aerosol species, such as Black (BC) and Brown (BrC) Carbon, are able to warm the atmosphere. The role of aerosols is one of the least clear aspects in the so called “Arctic Amplification” (AA) and up to now this was mostly modelled [1,2]. For this reason, we took part in four scientific cruises (AREX, Arctic-Expedition, summer 2018, 2019, 2021 and EUREC4A, 2020) in the North Atlantic, eastward and south-eastward of Barbados, aiming at the determination of the aerosol chemical composition and properties from the Tropics to the North Pole.
The Heating Rate (HR) was experimentally determined at 1 minute time-resolution along different latitudes by means of an innovative methodology [3], obtained by cumulatively taking into account the aerosol optical properties, i.e. the absorption coefficients (measured by AE33 Aethalometer) and incident radiation (direct, diffuse and reflected) across the entire solar spectrum. The HR computed along AREX and in Milan (in the same period) were used to determine the energy gradient, due to the LAA induced heat storage at mid-latitudes, which contributes to AA through the atmospheric heat transport northward.
Moreover, aerosol chemical composition was achieved by means of sampling via high volume sampler (ECHO-PUF Tecora) and analysis via ion chromatography, TCA08 for Total Carbon content, Aethalometer AE33 (for BC), ICP-OES for elements.
A clear latitudinal behaviour in Black Carbon concentrations, with the highest values at low latitudes (e.g. average BC concentration in Gdansk up to 1507±75 ng/m3) and a progressive decrease moving northwards and away from the big Arctic settlements (Black Carbon concentrations within the 81st parallel: 5±1 ng/m3).
According to the latitudinal behaviour of BC concentrations and solar radiation (decreases towards the north while the diffuse component increases), HR decreases noticeably towards the Arctic: e.g. higher in the harbor of Gdansk (0.290±0.010 K/day) followed by the Baltic Sea (0.04±0.01 K/day), the Norvegian Sea (0.010±0.010 K/day) and finally with the lowest values in the pure Arctic Ocean (0.003±0.001 K/day). Accordingly, the energy density added to the system by the aerosol, a positive forcing that differs by 2 orders of magnitude between mid-latitudes and North Pole was found: 347.3 ± 11.8 J/m3 (Milan), 244.8 ± 12.2 J/m3 (Gdansk) and 2.6 ± 0.2 J/m3 (80°N). These results highlight the presence of a great energy gradient between mid-latitudes and Arctic that can trigger a heat transport towards the Arctic. Moreover this was strengthen by the HR value for EUREC4A in Barbados that was 0.175±0.003 K/day. Finally, preliminary results from Antarctica collected onboard the Italian RV Laura Bassi cruising the Southern Ocean and the Ross Sea will be shown.
Acknoledgements: GEMMA Center, Project TECLA MIUR – Dipartimenti di Eccellenza 2023–2027. JPI EUREC4A-OA project. CAIAC (oCean Atmosphere Interactions in the Antarctic regions and Convergence latitude) PNRA project
References
[1] Navarro, J. C. A. et al. (2016) Nat. Geosci. 9, 277–281.
[2] Shindell, D. and Faluvegi, G. (2009) Nat. Geosci. 2, 294–300.
[3] Ferrero, L. et al. (2018) Environ. Sci. Technol. 52, 3546 3555.
Keywords: blackcarbon, brown carbon, atmospheric heating rate, climate change
Published in RUNG: 18.03.2024; Views: 2342; Downloads: 68
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8. Contribution of black carbon and desert dust to aerosol absorption in the atmosphere of the Eastern Arabian PeninsulaMohamed M. K. Mahfouz, Gregor Skok, Jean Sciare, Michael Pikridas, M. R. Alfarra, Shamjad Moosakutty, Bálint Alföldy, Matic Ivančič, Martin Rigler, Asta Gregorič, Rok Podlipec, Griša Močnik, 2024, original scientific article Abstract: Discriminating the absorption coefficients of aerosol mineral dust and black carbon (BC) in different aerosol size fractions is a challenge because of BC's large mass absorption cross-section compared to dust. Ambient aerosol wavelength dependent absorption coefficients in supermicron and submicron size fractions were determined with a high time resolution. The measurements were performed simultaneously using identical systems at an urban and a regional background site in Qatar. At each site, measurements were taken by co-located Aethalometers, one with a virtual impactor (VI) and the other with a PM1 cyclone to respectively collect super-micron-enhanced and submicron fractions. The combined measurement of aerosol absorption and scattering coefficients enabled the particles to be classified based on their optical properties' wavelength dependence. The classification reveals the presence of BC internally/externally mixed with different aerosols. Helium ion microscopy images provided information concerning the extent of mineral dust in the submicron fraction. The determination of absorption coefficients during dust storms and non-dust periods was used to establish the absorption Ångström exponent for dust and BC. Non-parametric wind regression, potential source contribution function and back-trajectory analysis reveal major regional sources of desert dust associated with north-westerly winds and a minor local dust contribution. In contrast, major BC sources found locally were associated with south-westerly winds with a smaller contribution made by offshore emissions transported by north-easterly and easterly winds. The use of a pair of Aethalometers with VI and PM1 inlets separates contributions of BC and dust to the aerosol absorption coefficient.
Keywords: aerosol absorption, black carbon, mineral dust, desert dust, Arabian Peninsula
Published in RUNG: 29.02.2024; Views: 2818; Downloads: 13
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9. A device and a method for complete carbonaceous aerosol analysis in real time : European patent application EP4033242A1, 25. 8. 2021Asta Gregorič, Matic Ivančič, Martin Rigler, 2022, patent application Abstract: The present invention belongs to the field of methods and devices for analysing materials by determining their chemical or physical properties by the use of thermos-optical means. The invention relates to a device and a method for complete carbonaceous aerosol analysis in real time, which is essentially a system combining two different instruments, wherein the first instrument measures total carbon (TC) using flash heating of collected aerosol samples and generation of CO2, while the second instrument performs an optical attenuation analysis at 7 wavelengths from near UV (370 nm) to near IR range (950 nm) in order to characterize a Black Carbon (BC/EC) aerosols accumulated on a glass-fiber/PTFE filter tape. The device, i.e., the system of said instruments, collects and processes collected data of both instruments, wherein said processing may be performed by any of the instruments or by a separate processing means, computer or computer application.
Keywords: carbonaceous aerosol, black carbon, total carbon, brown carbon
Published in RUNG: 02.02.2024; Views: 2330; Downloads: 12
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10. Determining the Aethalometer multiple scattering enhancement factor C from the filter loading parameterLuca Ferrero, Niccolò Losi, Martin Rigler, Asta Gregorič, C. Colombi, L. D'Angelo, E. Cuccia, A. M. Cefalì, I. Gini, A. Doldi, 2024, original scientific article Abstract: Light-absorbing aerosols heat the atmosphere; an accurate quantification of their absorption coefficient is mandatory. However, standard reference instruments (CAPS, MAAP, PAX, PTAAM) are not always available at each measuring site around the world.
By integrating all previous published studies concerning the Aethalometers, the AE33 filter loading parameter, provided by the dual-spot algorithm, were used to determine the multiple scattering enhancement factor from the Aethalometer itself (hereinafter CAE) on an yearly and a monthly basis. The method was developed in Milan, where Aethalometer measurements were compared with MAAP data; the comparison showed a good agreement in terms of equivalent black carbon (R2 = 0.93; slope = 1.02 and a negligible intercept = 0.12 μg m−3) leading to a yearly experimental multiple scattering enhancement factor of 2.51 ± 0.04 (hereinafter CMAAP). On a yearly time base the CAE values obtained using the new approach was 2.52 ± 0.01, corresponding to the experimental one (CMAAP). Considering the seasonal behavior, higher experimental CMAAP and computed CAE values were found in summer (2.83 ± 0.12) whereas, the lower ones in winter/early-spring (2.37 ± 0.03), in agreement with the single scattering albedo behavior in the Po Valley.
Overall, the agreement between the experimental CMAAP and CAE showed a root mean squared error (RMSE) of just 0.038 on the CMAAP prediction, characterized by a slope close to 1 (1.001 ± 0.178), a negligible intercept (−0.002 ± 0.455) and a high degree of correlation (R2 = 0.955). From an environmental point of view, the application of a dynamic (space/time) determination of CAE increases the accuracy of the aerosol heating rate (compared to applying a fixed C value) up to 16 % solely in Milan, and to 114 % when applied in the Arctic at 80°N.
Keywords: aethalometer, C factor, loading parameter, MAAP, heating rate
Published in RUNG: 02.02.2024; Views: 3166; Downloads: 29
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