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Black carbon and particulate matter mass concentrations in the Metropolitan District of Caracas, Venezuela: An assessment of temporal variation and contributing sources
2022, Engelhardt, Vanessa, Pérez, Tibisay, Donoso, Loreto, Müller, Thomas, Wiedensohler, Alfred
Atmospheric aerosols play an important role in atmospheric processes and human health. Characterizing atmospheric aerosols and identifying their sources in large cities is relevant to propose site-specific air pollution mitigation strategies. In this study, we measured the mass concentration of atmospheric aerosols with an aerodynamic diameter smaller than 2.5 mm (PM2.5) in the city of Caracas (urban) and in a tropical montane cloud forest (suburban site, located in a mountainous area 11 km far from Caracas) between June 2018 and October 2019. We also measured equivalent black carbon (eBC) mass concentration in PM2.5 in Caracas during the same period. Our goal is to assess PM2.5 and eBC temporal variation and identify their major sources in the area. eBC showed a pronounced diurnal cycle in the urban site, mainly modulated by traffic circulation and the diurnal changes of the mixing layer height. In contrast, PM2.5 showed stable median values during the day with slight variations like that of eBC. In the forest site, PM2.5 values were higher in the afternoons due to the convective transport of aerosols from Caracas and other surrounding urban areas located in adjacent valleys. The annual median for eBC and PM2.5 was 1.6 and 9.2 mg m–3, respectively, in the urban site, while PM2.5 in the forest site was 6.6 mg m–3. To our knowledge, these are the first measurements of this type in the northernmost area of South America. eBC and PM2.5 sources identification during wet and dry seasons was obtained by percentiles of the conditional bivariate probability function (CBPF). CBPF showed seasonal variations of eBC and PM2.5 sources and that their contributions are higher during the dry season. Biomass burning events are a relevant contributing source of aerosols for both sites of measurements inferred by fire pixels from satellite data, the national fire department’s statistics data, and backward trajectories. Our results indicate that biomass burning might affect the atmosphere on a regional scale, contribute to regional warming, and have implications for local and regional air quality and, therefore, human health.
Strong impact of wildfires on the abundance and aging of black carbon in the lowermost stratosphere
2018, Ditas, Jeannine, Ma, Nan, Zhang, Yuxuan, Assmann, Denise, Neumaier, Marco, Riede, Hella, Karu, Einar, Williams, Jonathan, Scharffe, Dieter, Wang, Qiaoqiao, Saturno, Jorge, Schwarz, Joshua P., Katich, Joseph M., McMeeking, Gavin R., Zahn, Andreas, Hermann, Markus, Brenninkmeijer, Carl A. M., Andreae, Meinrat O., Pöschl, Ulrich, Su, Hang, Cheng, Yafang
Wildfires inject large amounts of black carbon (BC) particles into the atmosphere, which can reach the lowermost stratosphere (LMS) and cause strong radiative forcing. During a 14-month period of observations on board a passenger aircraft flying between Europe and North America, we found frequent and widespread biomass burning (BB) plumes, influencing 16 of 160 flight hours in the LMS. The average BC mass concentrations in these plumes (∼140 ng·m−3, standard temperature and pressure) were over 20 times higher than the background concentration (∼6 ng·m−3) with more than 100-fold enhanced peak values (up to ∼720 ng·m−3). In the LMS, nearly all BC particles were covered with a thick coating. The average mass equivalent diameter of the BC particle cores was ∼120 nm with a mean coating thickness of ∼150 nm in the BB plume and ∼90 nm with a coating of ∼125 nm in the background. In a BB plume that was encountered twice, we also found a high diameter growth rate of ∼1 nm·h−1 due to the BC particle coatings. The observed high concentrations and thick coatings of BC particles demonstrate that wildfires can induce strong local heating in the LMS and may have a significant influence on the regional radiative forcing of climate.
Influence of biomass burning on mixing state of sub-micron aerosol particles in the North China Plain
2017, Kecorius, Simonas, Ma, Nan, Teich, Monique, van Pinxteren, Dominik, Zhang, Shenglan, Gröβ, Johannes, Spindler, Gerald, Müller, Konrad, Iinuma, Yoshiteru, Hu, Min, Herrmann, Hartmut, Wiedensohler, Alfred
Particulate emissions from crop residue burning decrease the air quality as well as influence aerosol radiative properties on a regional scale. The North China Plain (NCP) is known for the large scale biomass burning (BB) of field residues, which often results in heavy haze pollution episodes across the region. We have been able to capture a unique BB episode during the international CAREBeijing-NCP intensive field campaign in Wangdu in the NCP (38.6°N, 115.2°E) from June to July 2014. It was found that aerosol particles originating from this BB event showed a significantly different mixing state compared with clean and non-BB pollution episodes. BB originated particles showed a narrower probability density function (PDF) of shrink factor (SF). And the maximum was found at shrink factor of 0.6, which is higher than in other episodes. The non-volatile particle number fraction during the BB episode decreased to 3% and was the lowest measured value compared to all other predefined episodes. To evaluate the influence of particle mixing state on aerosol single scattering albedo (SSA), SSA at different RHs was simulated using the measured aerosol physical-chemical properties. The differences between the calculated SSA for biomass burning, clean and pollution episodes are significant, meaning that the variation of SSA in different pollution conditions needs to be considered in the evaluation of aerosol direct radiative effects in the NCP. And the calculated SSA was found to be quite sensitive on the mixing state of BC, especially at low-RH condition. The simulated SSA was also compared with the measured values. For all the three predefined episodes, the measured SSA are very close to the calculated ones with assumed mixing states of homogeneously internal and core-shell internal mixing, indicating that both of the conception models are appropriate for the calculation of ambient SSA in the NCP.
Modification of local urban aerosol properties by long-range transport of biomass burning aerosol
2018, Stachlewska, Iwona S., Samson, Mateusz, Zawadzka, Olga, Harenda, Kamila M., Janicka, Lucja, Poczta, Patryk, Szczepanik, Dominika, Heese, Birgit, Wang, Dongxiang, Borek, Karolina, Tetoni, Eleni, Proestakis, Emmanouil, Siomos, Nikolaos, Nemuc, Anca, Chojnicki, Bogdan H., Markowicz, Krzysztof M., Pietruczuk, Aleksander, Szkop, Artur, Althausen, Dietrich, Stebel, Kerstin, Schuettemeyer, Dirk, Zehner, Claus
During August 2016, a quasi-stationary high-pressure system spreading over Central and North-Eastern Europe, caused weather conditions that allowed for 24/7 observations of aerosol optical properties by using a complex multi-wavelength PollyXT lidar system with Raman, polarization and water vapour capabilities, based at the European Aerosol Research Lidar Network (EARLINET network) urban site in Warsaw, Poland. During 24–30 August 2016, the lidar-derived products (boundary layer height, aerosol optical depth, Ångström exponent, lidar ratio, depolarization ratio) were analysed in terms of air mass transport (HYSPLIT model), aerosol load (CAMS data) and type (NAAPS model) and confronted with active and passive remote sensing at the ground level (PolandAOD, AERONET, WIOS-AQ networks) and aboard satellites (SEVIRI, MODIS, CATS sensors). Optical properties for less than a day-old fresh biomass burning aerosol, advected into Warsaw’s boundary layer from over Ukraine, were compared with the properties of long-range transported 3–5 day-old aged biomass burning aerosol detected in the free troposphere over Warsaw. Analyses of temporal changes of aerosol properties within the boundary layer, revealed an increase of aerosol optical depth and Ångström exponent accompanied by an increase of surface PM10 and PM2.5. Intrusions of advected biomass burning particles into the urban boundary layer seem to affect not only the optical properties observed but also the top height of the boundary layer, by moderating its increase.
Investigating African trace gas sources, vertical transport, and oxidation using IAGOS-CARIBIC measurements between Germany and South Africa between 2009 and 2011
2017, Thorenz, U.R., Baker, A.K., Leedham Elvidge, E.C., Sauvage, C., Riede, H., van Velthoven, P.F.J., Hermann, M., Weigelt, A., Oram, D.E., Brenninkmeijer, C.A.M., Zahn, A., Williams, J.
Between March 2009 and March 2011 a commercial airliner equipped with a custom built measurement container (IAGOS-CARIBIC observatory) conducted 13 flights between South Africa and Germany at 10–12 km altitude, traversing the African continent north-south. In-situ measurements of trace gases (CO, CH4, H2O) and aerosol particles indicated that strong surface sources (like biomass burning) and rapid vertical transport combine to generate maximum concentrations in the latitudinal range between 10°N and 10°S coincident with the inter-tropical convergence zone (ITCZ). Pressurized air samples collected during these flights were subsequently analyzed for a suite of trace gases including C2-C8 non-methane hydrocarbons (NMHC) and halocarbons. These shorter-lived trace gases, originating from both natural and anthropogenic sources, also showed near equatorial maxima highlighting the effectiveness of convective transport in this region. Two source apportionment methods were used to investigate the specific sources of NMHC: positive matrix factorization (PMF), which is used for the first time for NMHC analysis in the upper troposphere (UT), and enhancement ratios to CO. Using the PMF method three characteristic airmass types were identified based on the different trace gas concentrations they obtained: biomass burning, fossil fuel emissions, and “background” air. The first two sources were defined with reference to previously reported surface source characterizations, while the term “background” was given to air masses in which the concentration ratios approached that of the lifetime ratios. Comparison of enhancement ratios between NMHC and CO for the subset of air samples that had experienced recent contact with the planetary boundary layer (PBL) to literature values showed that the burning of savanna and tropical forest is likely the main source of NMHC in the African upper troposphere (10–12 km). Photochemical aging patterns for the samples with PBL contact revealed that the air had different degradation histories depending on the hemisphere in which they were emitted. In the southern hemisphere (SH) air masses experienced more dilution by clean background air whereas in the northern hemisphere (NH) air masses are less diluted or mixed with background air still containing longer lived NMHC. Using NMHC photochemical clocks ozone production was seen in the BB outflow above Africa in the NH.