6 results
Search Results
Now showing 1 - 6 of 6
- ItemStrong particle production and condensational growth in the upper troposphere sustained by biogenic VOCs from the canopy of the Amazon Basin(Katlenburg-Lindau : EGU, 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, YafangNucleation 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.
- ItemLong-term study on coarse mode aerosols in the Amazon rain forest with the frequent intrusion of Saharan dust plumes(Katlenburg-Lindau : EGU, 2018) Moran-Zuloaga, Daniel; Ditas, Florian; Walter, David; Saturno, Jorge; Brito, Joel; Carbone, Samara; Chi, Xuguang; Hrabě de Angelis, Isabella; Baars, Holger; Godoi, Ricardo H. M.; Heese, Birgit; Holanda, Bruna A.; Lavrič, Jošt V.; Martin, Scot T.; Ming, Jing; Pöhlker, Mira L.; Ruckteschler, Nina; Su, Hang; Wang, Yaqiang; Wang, Qiaoqiao; Wang, Zhibin; Weber, Bettina; Wolff, Stefan; Artaxo, Paulo; Pöschl, Ulrich; Andreae, Meinrat O.; Pöhlker, ChristopherIn the Amazonian atmosphere, the aerosol coarse mode comprises a complex, diverse, and variable mixture of bioaerosols emitted from the rain forest ecosystem, long-range transported Saharan dust (we use Sahara as shorthand for the dust source regions in Africa north of the Equator), marine aerosols from the Atlantic Ocean, and coarse smoke particles from deforestation fires. For the rain forest, the coarse mode particles are of significance with respect to biogeochemical and hydrological cycling, as well as ecology and biogeography. However, knowledge on the physicochemical and biological properties as well as the ecological role of the Amazonian coarse mode is still sparse. This study presents results from multi-year coarse mode measurements at the remote Amazon Tall Tower Observatory (ATTO) site. It combines online aerosol observations, selected remote sensing and modeling results, as well as dedicated coarse mode sampling and analysis. The focal points of this study are a systematic characterization of aerosol coarse mode abundance and properties in the Amazonian atmosphere as well as a detailed analysis of the frequent, pulse-wise intrusion of African long-range transport (LRT) aerosols (comprising Saharan dust and African biomass burning smoke) into the Amazon Basin.We find that, on a multi-year time scale, the Amazonian coarse mode maintains remarkably constant concentration levels (with 0.4 cmĝ'3 and 4.0 μg mĝ'3 in the wet vs. 1.2 cmĝ'3 and 6.5 μg mĝ'3 in the dry season) with rather weak seasonality (in terms of abundance and size spectrum), which is in stark contrast to the pronounced biomass burning-driven seasonality of the submicron aerosol population and related parameters. For most of the time, bioaerosol particles from the forest biome account for a major fraction of the coarse mode background population. However, from December to April there are episodic intrusions of African LRT aerosols, comprising Saharan dust, sea salt particles from the transatlantic passage, and African biomass burning smoke. Remarkably, during the core period of this LRT season (i.e., February-March), the presence of LRT influence, occurring as a sequence of pulse-like plumes, appears to be the norm rather than an exception. The LRT pulses increase the coarse mode concentrations drastically (up to 100 μg mĝ'3) and alter the coarse mode composition as well as its size spectrum. Efficient transport of the LRT plumes into the Amazon Basin takes place in response to specific mesoscale circulation patterns in combination with the episodic absence of rain-related aerosol scavenging en route. Based on a modeling study, we estimated a dust deposition flux of 5-10 kg haĝ'1 aĝ'1 in the region of the ATTO site. Furthermore, a chemical analysis quantified the substantial increase of crustal and sea salt elements under LRT conditions in comparison to the background coarse mode composition. With these results, we estimated the deposition fluxes of various elements that are considered as nutrients for the rain forest ecosystem. These estimates range from few g haĝ'1 aĝ'1 up to several hundreds of g haĝ'1 aĝ'1 in the ATTO region.The long-term data presented here provide a statistically solid basis for future studies of the manifold aspects of the dynamic coarse mode aerosol cycling in the Amazon. Thus, it may help to understand its biogeochemical relevance in this ecosystem as well as to evaluate to what extent anthropogenic influences have altered the coarse mode cycling already.
- ItemInflux of African biomass burning aerosol during the Amazonian dry season through layered transatlantic transport of black carbon-rich smoke(Katlenburg-Lindau : EGU, 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, ChristopherBlack 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).
- ItemRegional modelling of polycyclic aromatic hydrocarbons: WRF-Chem-PAH model development and East Asia case studies(Katlenburg-Lindau : EGU, 2017) Mu, Qing; Lammel, Gerhard; Gencarelli, Christian N.; Hedgecock, Ian M.; Chen, Ying; Přibylová, Petra; Teich, Monique; Zhang, Yuxuan; Zheng, Guangjie; van Pinxteren, Dominik; Zhang, Qiang; Herrmann, Hartmut; Shiraiwa, Manabu; Spichtinger, Peter; Su, Hang; Pöschl, Ulrich; Cheng, YafangPolycyclic aromatic hydrocarbons (PAHs) are hazardous pollutants, with increasing emissions in pace with economic development in East Asia, but their distribution and fate in the atmosphere are not yet well understood. We extended the regional atmospheric chemistry model WRF-Chem (Weather Research Forecast model with Chemistry module) to comprehensively study the atmospheric distribution and the fate of low-concentration, slowly degrading semivolatile compounds. The WRF-Chem-PAH model reflects the state-of-the-art understanding of current PAHs studies with several new or updated features. It was applied for PAHs covering a wide range of volatility and hydrophobicity, i.e. phenanthrene, chrysene and benzo[a]pyrene, in East Asia. Temporally highly resolved PAH concentrations and particulate mass fractions were evaluated against observations. The WRF-Chem-PAH model is able to reasonably well simulate the concentration levels and particulate mass fractions of PAHs near the sources and at a remote outflow region of East Asia, in high spatial and temporal resolutions. Sensitivity study shows that the heterogeneous reaction with ozone and the homogeneous reaction with the nitrate radical significantly influence the fate and distributions of PAHs. The methods to implement new species and to correct the transport problems can be applied to other newly implemented species in WRF-Chem.
- ItemNatural sea-salt emissions moderate the climate forcing of anthropogenic nitrate(Katlenburg-Lindau : EGU, 2020) Chen, Ying; Cheng, Yafang; Ma, Nan; Wei, Chao; Ran, Liang; Wolke, Ralf; Größ, Johannes; Wang, Qiaoqiao; Denier van der Gon, Hugo A.C.; Spindler, Gerald; Lelieveld, Jos; Tegen, Ina; Su, Hang; Wiedensohler, AlfredNatural sea-salt aerosols, when interacting with anthropogenic emissions, can enhance the formation of particulate nitrate. This enhancement has been suggested to increase the direct radiative forcing of nitrate, called the “mass-enhancement effect”. Through a size-resolved dynamic mass transfer modeling approach, we show that interactions with sea salt shift the nitrate from sub- to super-micron-sized particles (“redistribution effect”), and hence this lowers its efficiency for light extinction and reduces its lifetime. The redistribution effect overwhelms the mass-enhancement effect and significantly moderates nitrate cooling; e.g., the nitrate-associated aerosol optical depth can be reduced by 10 %–20 % over European polluted regions during a typical sea-salt event, in contrast to an increase by ∼10 % when only accounting for the mass-enhancement effect. Global model simulations indicate significant redistribution over coastal and offshore regions worldwide. Our study suggests a strong buffering by natural sea-salt aerosols that reduces the climate forcing of anthropogenic nitrate, which had been expected to dominate the aerosol cooling by the end of the century. Comprehensive considerations of this redistribution effect foster better understandings of climate change and nitrogen deposition.
- ItemA parameterization of the heterogeneous hydrolysis of N2O5 for mass-based aerosol models: Improvement of particulate nitrate prediction(Katlenburg-Lindau : EGU, 2018) Chen, Ying; Wolke, Ralf; Ran, Liang; Birmili, Wolfram; Spindler, Gerald; Schröder, Wolfram; Su, Hang; Cheng, Yafang; Tegen, Ina; Wiedensohler, AlfredThe heterogeneous hydrolysis of N2O5 on the surface of deliquescent aerosol leads to HNO3 formation and acts as a major sink of NOx in the atmosphere during night-time. The reaction constant of this heterogeneous hydrolysis is determined by temperature (T), relative humidity (RH), aerosol particle composition, and the surface area concentration (S). However, these parameters were not comprehensively considered in the parameterization of the heterogeneous hydrolysis of N2O5 in previous mass-based 3-D aerosol modelling studies. In this investigation, we propose a sophisticated parameterization (NewN2O5) of N2O5 heterogeneous hydrolysis with respect to T, RH, aerosol particle compositions, and S based on laboratory experiments. We evaluated closure between NewN2O5 and a state-of-the-art parameterization based on a sectional aerosol treatment. The comparison showed a good linear relationship (R Combining double low line 0.91) between these two parameterizations. NewN2O5 was incorporated into a 3-D fully online coupled model, COSMO-Muscat, with the mass-based aerosol treatment. As a case study, we used the data from the HOPE Melpitz campaign (10-25 September 2013) to validate model performance. Here, we investigated the improvement of nitrate prediction over western and central Europe. The modelled particulate nitrate mass concentrations ([NO3-]) were validated by filter measurements over Germany (Neuglobsow, Schmücke, Zingst, and Melpitz). The modelled [NO3-] was significantly overestimated for this period by a factor of 5-19, with the corrected NH3 emissions (reduced by 50 %) and the original parameterization of N2O5 heterogeneous hydrolysis. The NewN2O5 significantly reduces the overestimation of [NO3-] by ∼ 35 %. Particularly, the overestimation factor was reduced to approximately 1.4 in our case study (12, 17-18 and 25 September 2013) when [NO3-] was dominated by local chemical formations. In our case, the suppression of organic coating was negligible over western and central Europe, with an influence on [NO3-] of less than 2 % on average and 20 % at the most significant moment. To obtain a significant impact of the organic coating effect, N2O5, SOA, and NH3 need to be present when RH is high and T is low. However, those conditions were rarely fulfilled simultaneously over western and central Europe. Hence, the organic coating effect on the reaction probability of N2O5 may not be as significant as expected over western and central Europe.