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Keywords: carbonaceous aerosol, organic aerosol
Published in RUNG: 10.05.2024; Views: 54; Downloads: 0
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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: 52; Downloads: 0
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Abstract: La Paz and El Alto are two fast-growing, high-altitude Bolivian cities forming the second-largest metropolitan area in the country. Located between 3200 and 4050 m a.s.l. (above sea level), these cities are home to a burgeoning population of approximately 1.8 million residents. The air quality in this conurbation is heavily influenced by urbanization; however, there are no comprehensive studies evaluating the sources of air pollution and their health impacts. Despite their proximity, the substantial variation in altitude, topography, and socioeconomic activities between La Paz and El Alto result in distinct sources, dynamics, and transport of particulate matter (PM). In this investigation, PM10 samples were collected at two urban background stations located in La Paz and El Alto between April 2016 and June 2017. The samples were later analyzed for a wide range of chemical species including numerous source tracers (OC, EC, water-soluble ions, sugar anhydrides, sugar alcohols, trace metals, and molecular organic species). The United States Environmental Protection Agency (U.S. EPA) Positive Matrix Factorization (PMF v.5.0) receptor model was employed for the source apportionment of PM10. This is one of the first source apportionment studies in South America that incorporates an extensive suite of organic markers, including levoglucosan, polycyclic aromatic hydrocarbons (PAHs), hopanes, and alkanes, alongside inorganic species. The multisite PMF resolved 11 main sources of PM. The largest annual contribution to PM10 came from the following two major sources: the ensemble of the four vehicular emissions sources (exhaust and non-exhaust), accountable for 35 % and 25 % of the measured PM in La Paz and El Alto, respectively; and dust, which contributed 20 % and 32 % to the total PM mass. Secondary aerosols accounted for 22 % (24 %) in La Paz (El Alto). Agricultural smoke resulting from biomass burning in the Bolivian lowlands and neighboring countries contributed to 9 % (8 %) of the total PM10 mass annually, increasing to 17 % (13 %) between August–October. Primary biogenic emissions were responsible for 13 % (7 %) of the measured PM10 mass. Additionally, a profile associated with open waste burning occurring from May to August was identified. Although this source contributed only to 2 % (5 %) of the total PM10 mass, it constitutes the second largest source of PAHs, which are compounds potentially hazardous to human health. Our analysis additionally resolved two different traffic-related factors, a lubricant source (not frequently identified), and a non-exhaust emissions source. Overall, this study demonstrates that PM10 concentrations in La Paz and El Alto region are predominantly influenced by a limited number of local sources. In conclusion, to improve air quality in both cities, efforts should primarily focus on addressing dust, traffic emissions, open waste burning, and biomass burning.
Keywords: source apportionment, particular air pollution, high altitude, positive matrix factorization, PMF
Published in RUNG: 15.09.2023; Views: 805; Downloads: 5
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Abstract: Accurate measurements of the horizontal and vertical distribution of atmospheric aerosol particle optical properties are key for a better understanding of their impact on the climate. Here we present the results of a measurement campaign based on instrumented flights over north-eastern Spain. We measured vertical profiles of size-segregated atmospheric particulate matter (PM) mass concentrations and multi-wavelength scattering and absorption coefficients in the western Mediterranean basin (WMB). The campaign took place during typical summer conditions, characterized by the development of a vertical multi-layer structure, under both summer regional pollution episodes (REGs) and Saharan dust events (SDEs). REG patterns in the region form under high insolation and scarce precipitation in summer, favouring layering of highly aged fine-PM strata in the lower few kma.s.l. The REG scenario prevailed during the entire measurement campaign. Additionally, African dust outbreaks and plumes from northern African wildfires influenced the study area. The vertical profiles of climate-relevant intensive optical parameters such as single-scattering albedo (SSA); the asymmetry parameter (g); scattering, absorption and SSA Ångström exponents (SAE, AAE and SSAAE); and PM mass scattering and absorption cross sections (MSC and MAC) were derived from the measurements. Moreover, we compared the aircraft measurements with those performed at two GAW–ACTRIS (Global Atmosphere Watch–Aerosol, Clouds and Trace Gases) surface measurement stations located in north-eastern Spain, namely Montseny (MSY; regional background) and Montsec d'Ares (MSA; remote site). Airborne in situ measurements and ceilometer ground-based remote measurements identified aerosol air masses at altitudes up to more than 3.5 kma.s.l. The vertical profiles of the optical properties markedly changed according to the prevailing atmospheric scenarios. During SDE the SAE was low along the profiles, reaching values < 1.0 in the dust layers. Correspondingly, SSAAE was negative, and AAE reached values up to 2.0–2.5, as a consequence of the UV absorption increased by the presence of the coarse dust particles. During REG, the SAE increased to > 2.0, and the asymmetry parameter g was rather low (0.5–0.6) due to the prevalence of fine PM, which was characterized by an AAE close to 1.0, suggesting a fossil fuel combustion origin. During REG, some of the layers featured larger AAE (> 1.5), relatively low SSA at 525 nm (< 0.85) and high MSC (> 9 m2 g−1) and were associated with the influence of PM from wildfires. Overall, the SSA and MSC near the ground ranged around 0.85 and 3 m2 g−1, respectively, and increased at higher altitudes, reaching values above 0.95 and up to 9 m2 g−1. The PM, MSC and MAC were on average larger during REG compared to SDE due to the larger scattering and absorption efficiency of fine PM compared with dust. The SSA and MSC had quite similar vertical profiles and often both increased with height indicating the progressive shift toward PM with a larger scattering efficiency with altitude. This study contributes to our understanding of regional-aerosol vertical distribution and optical properties in the WMB, and the results will be useful for improving future climate projections and remote sensing or satellite retrieval algorithms.
Keywords: aerosol, climate change, Saharan dust, black carbon, aerosol absorption, aerosol scattering
Published in RUNG: 14.01.2021; Views: 2461; Downloads: 0
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