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Strong particle production and condensational growth in the upper troposphere sustained by biogenic VOCs from the canopy of the Amazon Basin
2023, Liu, Yunfan, Su, Hang, Wang, Siwen, Wei, Chao, Tao, Wei, Pöhlker, Mira L., Pöhlker, Christopher, Holanda, Bruna A., Krüger, Ovid O., Hoffmann, Thorsten, Wendisch, Manfred, Artaxo, Paulo, Pöschl, Ulrich, Andreae, Meinrat O., Cheng, Yafang
Nucleation and condensation associated with biogenic volatile organic compounds (BVOCs) are important aerosol formation pathways, yet their contribution to the upper-tropospheric aerosols remains inconclusive, hindering the understanding of aerosol climate effects. Here, we develop new schemes describing these organic aerosol formation processes in the WRF-Chem model and investigate their impact on the abundance of cloud condensation nuclei (CCN) in the upper troposphere (UT) over the Amazon Basin. We find that the new schemes significantly increase the simulated CCN number concentrations in the UT (e.g., up to -1/4 400 cm-3 at 0.52 % supersaturation) and greatly improve the agreement with the aircraft observations. Organic condensation enhances the simulated CCN concentration by 90 % through promoting particle growth, while organic nucleation, by replenishing new particles, contributes an additional 14 %. Deep convection determines the rate of these organic aerosol formation processes in the UT through controlling the upward transport of biogenic precursors (i.e., BVOCs). This finding emphasizes the importance of the biosphere-atmosphere coupling in regulating upper-tropospheric aerosol concentrations over the tropical forest and calls for attention to its potential role in anthropogenic climate change.
Influx of African biomass burning aerosol during the Amazonian dry season through layered transatlantic transport of black carbon-rich smoke
2020, Holanda, Bruna A., Pöhlker, Mira L., Walter, David, Saturno, Jorge, Sörgel, Matthias, Ditas, Jeannine, Ditas, Florian, Schulz, Christiane, Aurélio Franco, Marco, Wang, Qiaoqiao, Donth, Tobias, Artaxo, Paulo, Barbosa, Henrique M.J., Borrmann, Stephan, Braga, Ramon, Brito, Joel, Cheng, Yafang, Dollner, Maximilian, Kaiser, JohannesW., Klimach, Thomas, Knote, Christoph, Krüger, Ovid O., Fütterer, Daniel, Lavrič, Jošt V., Ma, Nan, Machado, Luiz A.T., Ming, Jing, Morais, Fernando G., Paulsen, Hauke, Sauer, Daniel, Schlager, Hans, Schneider, Johannes, Su, Hang, Weinzierl, Bernadett, Walser, Adrian, Wendisch, Manfred, Ziereis, Helmut, Zöger, Martin, Pöschl, Ulrich, Andreae, Meinrat O., Pöhlker, Christopher
Black carbon (BC) aerosols influence the Earth's atmosphere and climate, but their microphysical properties, spatiotemporal distribution, and long-range transport are not well constrained. This study presents airborne observations of the transatlantic transport of BC-rich African biomass burning (BB) smoke into the Amazon Basin using a Single Particle Soot Photometer (SP2) as well as several complementary techniques. We base our results on observations of aerosols and trace gases off the Brazilian coast onboard the HALO (High Altitude and LOng range) research aircraft during the ACRIDICON-CHUVA campaign in September 2014. During flight AC19 over land and ocean at the northeastern coastline of the Amazon Basin, we observed a BCrich layer at ∼ 3:5 km altitude with a vertical extension of ∼ 0:3 km. Backward trajectories suggest that fires in African grasslands, savannas, and shrublands were the main source of this pollution layer and that the observed BB smoke had undergone more than 10 d of atmospheric transport and aging over the South Atlantic before reaching the Amazon Basin. The aged smoke is characterized by a dominant accumulation mode, centered at about 130 nm, with a particle concentration of Nacc D 850±330 cm-3. The rBC particles account for ∼ 15 % of the submicrometer aerosol mass and ∼ 40 % of the total aerosol number concentration. This corresponds to a mass concentration range from 0.5 to 2 μ g m-3 (1st to 99th percentiles) and a number concentration range from 90 to 530 cm-3. Along with rBC, high cCO (150 ± 30 ppb) and cO3 (56 ± 9 ppb) mixing ratios support the biomass burning origin and pronounced photochemical aging of this layer. Upon reaching the Amazon Basin, it started to broaden and to subside, due to convective mixing and entrainment of the BB aerosol into the boundary layer. Satellite observations show that the transatlantic transport of pollution layers is a frequently occurring process, seasonally peaking in August/September. By analyzing the aircraft observations together with the long-term data from the Amazon Tall Tower Observatory (ATTO), we found that the transatlantic transport of African BB smoke layers has a strong impact on the northern and central Amazonian aerosol population during the BBinfluenced season (July to December). In fact, the early BB season (July to September) in this part of the Amazon appears to be dominated by African smoke, whereas the later BB season (October to December) appears to be dominated by South American fires. This dichotomy is reflected in pronounced changes in aerosol optical properties such as the single scattering albedo (increasing from 0.85 in August to 0.90 in November) and the BC-to-CO enhancement ratio (decreasing from 11 to 6 ng m-3 ppb-1). Our results suggest that, despite the high fraction of BC particles, the African BB aerosol acts as efficient cloud condensation nuclei (CCN), with potentially important implications for aerosol-cloud interactions and the hydrological cycle in the Amazon. © 2020 Author(s).