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- ItemMeasurements of aerosol and CCN properties in the Mackenzie River delta (Canadian Arctic) during spring-summer transition in May 2014(Katlenburg-Lindau : EGU, 2018) Herenz, Paul; Wex, Heike; Henning, Silvia; Kristensen, Thomas Bjerring; Rubach, Florian; Roth, Anja; Borrmann, Stephan; Bozem, Heiko; Schulz, Hannes; Stratmann, FrankWithin the framework of the RACEPAC (Radiation-Aerosol-Cloud Experiment in the Arctic Circle) project, the Arctic aerosol, arriving at a ground-based station in Tuktoyaktuk (Mackenzie River delta area, Canada), was characterized during a period of 3 weeks in May 2014. Basic meteorological parameters and particle number size distributions (PNSDs) were observed and two distinct types of air masses were found. One type were typical Arctic haze air masses, termed accumulation-type air masses, characterized by a monomodal PNSD with a pronounced accumulation mode at sizes above 100 nm. These air masses were observed during a period when back trajectories indicate an air mass origin in the north-east of Canada. The other air mass type is characterized by a bimodal PNSD with a clear minimum around 90ĝ€†nm and with an Aitken mode consisting of freshly formed aerosol particles. Back trajectories indicate that these air masses, termed Aitken-type air masses, originated from the North Pacific. In addition, the application of the PSCF receptor model shows that air masses with their origin in active fire areas in central Canada and Siberia, in areas of industrial anthropogenic pollution (Norilsk and Prudhoe Bay Oil Field) and the north-west Pacific have enhanced total particle number concentrations (N CN). Generally, N CN ranged from 20 to 500 cmg'3, while cloud condensation nuclei (CCN) number concentrations were found to cover a range from less than 10 up to 250 cmg'3 for a supersaturation (SS) between 0.1 and 0.7 %. The hygroscopicity parameter of the CCN was determined to be 0.23 on average and variations in were largely attributed to measurement uncertainties.
Furthermore, simultaneous PNSD measurements at the ground station and on the Polar 6 research aircraft were performed. We found a good agreement of ground-based PNSDs with those measured between 200 and 1200 m. During two of the four overflights, particle number concentrations at 3000 m were found to be up to 20 times higher than those measured below 2000 m; for one of these two flights, PNSDs measured above 2000 m showed a different shape than those measured at lower altitudes. This is indicative of long-range transport from lower latitudes into the Arctic that can advect aerosol from different regions in different heights. - ItemAfrican smoke particles act as cloud condensation nuclei in the wintertime tropical North Atlantic boundary layer over Barbados(Katlenburg-Lindau : EGU, 2023) Royer, Haley M.; Pöhlker, Mira L.; Krüger, Ovid; Blades, Edmund; Sealy, Peter; Lata, Nurun Nahar; Cheng, Zezhen; China, Swarup; Ault, Andrew P.; Quinn, Patricia K.; Zuidema, Paquita; Pöhlker, Christopher; Pöschl, Ulrich; Andreae, Meinrat; Gaston, Cassandra J.The number concentration and properties of aerosol particles serving as cloud condensation nuclei (CCN) are important for understanding cloud properties, including in the tropical Atlantic marine boundary layer (MBL), where marine cumulus clouds reflect incoming solar radiation and obscure the low-albedo ocean surface. Studies linking aerosol source, composition, and water uptake properties in this region have been conducted primarily during the summertime dust transport season, despite the region receiving a variety of aerosol particle types throughout the year. In this study, we compare size-resolved aerosol chemical composition data to the hygroscopicity parameter κ derived from size-resolved CCN measurements made during the Elucidating the Role of Clouds-Circulation Coupling in Climate (EUREC4A) and Atlantic Tradewind Ocean-Atmosphere Mesoscale Interaction Campaign (ATOMIC) campaigns from January to February 2020. We observed unexpected periods of wintertime long-range transport of African smoke and dust to Barbados. During these periods, the accumulation-mode aerosol particle and CCN number concentrations as well as the proportions of dust and smoke particles increased, whereas the average κ slightly decreased (κCombining double low line0.46±0.10) from marine background conditions (κCombining double low line0.52±0.09) when the submicron particles were mostly composed of marine organics and sulfate. Size-resolved chemical analysis shows that smoke particles were the major contributor to the accumulation mode during long-range transport events, indicating that smoke is mainly responsible for the observed increase in CCN number concentrations. Earlier studies conducted at Barbados have mostly focused on the role of dust on CCN, but our results show that aerosol hygroscopicity and CCN number concentrations during wintertime long-range transport events over the tropical North Atlantic are also affected by African smoke. Our findings highlight the importance of African smoke for atmospheric processes and cloud formation over the Caribbean.
- ItemOzone depletion in the Arctic and Antarctic stratosphere induced by wildfire smoke(Katlenburg-Lindau : EGU, 2022) Ansmann, Albert; Ohneiser, Kevin; Chudnovsky, Alexandra; Knopf, Daniel A.; Eloranta, Edwin W.; Villanueva, Diego; Seifert, Patric; Radenz, Martin; Barja, Boris; Zamorano, Félix; Jimenez, Cristofer; Engelmann, Ronny; Baars, Holger; Griesche, Hannes; Hofer, Julian; Althausen, Dietrich; Wandinger, UllaA record-breaking stratospheric ozone loss was observed over the Arctic and Antarctica in 2020. Strong ozone depletion occurred over Antarctica in 2021 as well. The ozone holes developed in smoke-polluted air. In this article, the impact of Siberian and Australian wildfire smoke (dominated by organic aerosol) on the extraordinarily strong ozone reduction is discussed. The study is based on aerosol lidar observations in the North Pole region (October 2019-May 2020) and over Punta Arenas in southern Chile at 53.2°S (January 2020-November 2021) as well as on respective NDACC (Network for the Detection of Atmospheric Composition Change) ozone profile observations in the Arctic (Ny-Ålesund) and Antarctica (Neumayer and South Pole stations) in 2020 and 2021. We present a conceptual approach on how the smoke may have influenced the formation of polar stratospheric clouds (PSCs), which are of key importance in the ozone-depleting processes. The main results are as follows: (a) the direct impact of wildfire smoke below the PSC height range (at 10-12 km) on ozone reduction seems to be similar to well-known volcanic sulfate aerosol effects. At heights of 10-12 km, smoke particle surface area (SA) concentrations of 5-7 μm2 cm-3 (Antarctica, spring 2021) and 6-10 μm2 cm-3 (Arctic, spring 2020) were correlated with an ozone reduction in terms of ozone partial pressure of 0.4-1.2 mPa (about 30 % further ozone reduction over Antarctica) and of 2-3.5 mPa (Arctic, 20 %-30 % reduction with respect to the long-term springtime mean). (b) Within the PSC height range, we found indications that smoke was able to slightly increase the PSC particle number and surface area concentration. In particular, a smoke-related additional ozone loss of 1-2 mPa (10 %-20 % contribution to the total ozone loss over Antarctica) was observed in the 14-23 km PSC height range in September-October 2020 and 2021. Smoke particle number concentrations ranged from 10 to 100 cm-3 and were about a factor of 10 (in 2020) and 5 (in 2021) above the stratospheric aerosol background level. Satellite observations indicated an additional mean column ozone loss (deviation from the long-term mean) of 26-30 Dobson units (9 %-10 %, September 2020, 2021) and 52-57 Dobson units (17 %-20 %, October 2020, 2021) in the smoke-polluted latitudinal Antarctic belt from 70-80°S. Copyright:
- 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.
- ItemRegional effects of atmospheric aerosols on temperature: An evaluation of an ensemble of online coupled models(Katlenburg-Lindau : EGU, 2017) Baró, Rocío; Palacios-Peña, Laura; Baklanov, Alexander; Balzarini, Alessandra; Brunner, Dominik; Forkel, Renate; Hirtl, Marcus; Honzak, Luka; Pérez, Juan Luis; Pirovano, Guido; San José, Roberto; Schröder, Wolfram; Werhahn, Johannes; Wolke, Ralf; Žabkar, Rahela; Jiménez-Guerrero, PedroThe climate effect of atmospheric aerosols is associated with their influence on the radiative budget of the Earth due to the direct aerosol-radiation interactions (ARIs) and indirect effects, resulting from aerosol-cloud-radiation interactions (ACIs). Online coupled meteorology-chemistry models permit the description of these effects on the basis of simulated atmospheric aerosol concentrations, although there is still some uncertainty associated with the use of these models. Thus, the objective of this work is to assess whether the inclusion of atmospheric aerosol radiative feedbacks of an ensemble of online coupled models improves the simulation results for maximum, mean and minimum temperature at 2m over Europe. The evaluated models outputs originate from EuMetChem COST Action ES1004 simulations for Europe, differing in the inclusion (or omission) of ARI and ACI in the various models. The cases studies cover two important atmospheric aerosol episodes over Europe in the year 2010: (i) a heat wave event and a forest fire episode (July-August 2010) and (ii) a more humid episode including a Saharan desert dust outbreak in October 2010. The simulation results are evaluated against observational data from the E-OBS gridded database. The results indicate that, although there is only a slight improvement in the bias of the simulation results when including the radiative feedbacks, the spatiotemporal variability and correlation coefficients are improved for the cases under study when atmospheric aerosol radiative effects are included.
- ItemThe vertical aerosol type distribution above Israel – 2 years of lidar observations at the coastal city of Haifa(Katlenburg-Lindau : EGU, 2022) Heese, Birgit; Floutsi, Athena Augusta; Baars, Holger; Althausen, Dietrich; Hofer, Julian; Herzog, Alina; Mewes, Silke; Radenz, Martin; Schechner, Yoav Y.For the first time, vertically resolved long-term lidar measurements of the aerosol distribution were conducted in Haifa, Israel. The measurements were performed by a PollyXT multi-wavelength Raman and polarization lidar. The lidar was measuring continuously over a 2-year period from March 2017 to May 2019. The resulting data set is a series of manually evaluated lidar optical property profiles. To identify the aerosol types in the observed layers, a novel aerosol typing method that was developed at TROPOS is used. This method applies optimal estimation to a combination of lidar-derived intensive aerosol properties to determine the statistically most-likely contribution per aerosol component in terms of relative volume. A case study that shows several elevated aerosol layers illustrates this method and shows, for example, that coarse dust particles are observed up to 5ĝ€¯km height over Israel. From the whole data set, the seasonal distribution of the observed aerosol components over Israel is derived. Throughout all seasons, coarse spherical particles like sea salt and hygroscopically grown continental aerosol were observed. These particles originate from continental Europe and were transported over the Mediterranean Sea. Sea-salt particles were observed frequently due to the coastal site of Haifa. The highest contributions of coarse spherical particles are present in summer, autumn, and winter. During spring, mostly coarse non-spherical particles that are attributed to desert dust were observed. This is consistent with the distinct dust season in spring in Israel. An automated time-height-resolved air mass source attribution method identifies the origin of the dust in the Sahara and the Arabian deserts. Fine-mode spherical particles contribute significantly to the observed aerosol mixture during all seasons. These particles originate mainly from the industrial region at the bay of Haifa.
- ItemAerosol optical properties in the southeastern United States in summer - Part 2: Sensitivity of aerosol optical depth to relative humidity and aerosol parameters(Katlenburg-Lindau : EGU, 2016) Brock, Charles A.; Wagner, Nicholas L.; Anderson, Bruce E.; Attwood, Alexis R.; Beyersdorf, Andreas; Campuzano-Jost, Pedro; Carlton, Annmarie G.; Day, Douglas A.; Diskin, Glenn S.; Gordon, Timothy D.; Jimenez, Jose L.; Lack, Daniel A.; Liao, Jin; Markovic, Milos Z.; Middlebrook, Ann M.; Ng, Nga L.; Perring, Anne E.; Richardson, Matthews S.; Schwarz, Joshua P.; Washenfelder, Rebecca A.; Welti, Andre; Xu, Lu; Ziemba, Luke D.; Murphy, Daniel M.Aircraft observations of meteorological, trace gas, and aerosol properties were made between May and September 2013 in the southeastern United States (US). Regionally representative aggregate vertical profiles of median and interdecile ranges of the measured parameters were constructed from 37 individual aircraft profiles made in the afternoon when a well-mixed boundary layer with typical fair-weather cumulus was present (Wagner et al., 2015). We use these 0–4 km aggregate profiles and a simple model to calculate the sensitivity of aerosol optical depth (AOD) to changes in dry aerosol mass, relative humidity, mixed-layer height, the central diameter and width of the particle size distribution, hygroscopicity, and dry and wet refractive index, while holding the other parameters constant. The calculated sensitivity is a result of both the intrinsic sensitivity and the observed range of variation in these parameters. These observationally based sensitivity studies indicate that the relationship between AOD and dry aerosol mass in these conditions in the southeastern US can be highly variable and is especially sensitive to relative humidity (RH). For example, calculated AOD ranged from 0.137 to 0.305 as the RH was varied between the 10th and 90th percentile profiles with dry aerosol mass held constant. Calculated AOD was somewhat less sensitive to aerosol hygroscopicity, mean size, and geometric standard deviation, σg. However, some chemistry–climate models prescribe values of σg substantially larger than we or others observe, leading to potential high biases in model-calculated AOD of ∼ 25 %. Finally, AOD was least sensitive to observed variations in dry and wet aerosol refractive index and to changes in the height of the well-mixed surface layer. We expect these findings to be applicable to other moderately polluted and background continental air masses in which an accumulation mode between 0.1–0.5 µm diameter dominates aerosol extinction.
- ItemRemote sensing and modelling analysis of the extreme dust storm hitting the Middle East and eastern Mediterranean in September 2015(Katlenburg-Lindau : EGU, 2017) Solomos, Stavros; Ansmann, Albert; Mamouri, Rodanthi-Elisavet; Binietoglou, Ioannis; Patlakas, Platon; Marinou, Eleni; Amiridis, VassilisThe extreme dust storm that affected the Middle East and the eastern Mediterranean in September 2015 resulted in record-breaking dust loads over Cyprus with aerosol optical depth exceeding 5.0 at 550ĝ€nm. We analyse this event using profiles from the European Aerosol Research Lidar Network (EARLINET) and the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO), geostationary observations from the Meteosat Second Generation (MSG) Spinning Enhanced Visible and Infrared Imager (SEVIRI), and high-resolution simulations from the Regional Atmospheric Modeling System (RAMS). The analysis of modelling and remote sensing data reveals the main mechanisms that resulted in the generation and persistence of the dust cloud over the Middle East and Cyprus. A combination of meteorological and surface processes is found, including (a) the development of a thermal low in the area of Syria that results in unstable atmospheric conditions and dust mobilization in this area, (b) the convective activity over northern Iraq that triggers the formation of westward-moving haboobs that merge with the previously elevated dust layer, and (c) the changes in land use due to war in the areas of northern Iraq and Syria that enhance dust erodibility.
- ItemSatellite retrievals of dust aerosol over the Red Sea and the Persian Gulf (2005-2015)(Katlenburg-Lindau : EGU, 2017) Banks, Jamie R.; Brindley, Helen E.; Stenchikov, Georgiy; Schepanski, KerstinThe inter-annual variability of the dust aerosol presence over the Red Sea and the Persian Gulf is analysed over the period 2005-2015. Particular attention is paid to the variation in loading across the Red Sea, which has previously been shown to have a strong, seasonally dependent latitudinal gradient. Over the 11 years considered, the July mean 630 nm aerosol optical depth (AOD) derived from the Spinning Enhanced Visible and InfraRed Imager (SEVIRI) varies between 0.48 and 1.45 in the southern half of the Red Sea. In the north, the equivalent variation is between 0.22 and 0.66. The temporal and spatial pattern of variability captured by SEVIRI is also seen in AOD retrievals from the MODerate Imaging Spectroradiometer (MODIS), but there is a systematic offset between the two records. Comparisons of both sets of retrievals with ship-and land-based AERONET measurements show a high degree of correlation with biases of <0.08. However, these comparisons typically only sample relatively low aerosol loadings. When both records are stratified by AOD retrievals from the Multi-angle Imaging SpectroRadiometer (MISR), opposing behaviour is revealed at high MISR AODs (>1), with offsets of C0.19 for MODIS and 0.06 for SEVIRI. Similar behaviour is also seen over the Persian Gulf. Analysis of the scattering angles at which retrievals from the SEVIRI and MODIS measurements are typically performed in these regions suggests that assumptions concerning particle sphericity may be responsible for the differences seen.
- ItemMeasurement report: Long-range transport and the fate of dimethyl sulfide oxidation products in the free troposphere derived from observations at the high-altitude research station Chacaltaya (5240ma.s.l.) in the Bolivian Andes(Katlenburg-Lindau : EGU, 2023) Scholz, Wiebke; Shen, Jiali; Aliaga, Diego; Wu, Cheng; Carbone, Samara; Moreno, Isabel; Zha, Qiaozhi; Huang, Wei; Heikkinen, Liine; Jaffrezo, Jean Luc; Uzu, Gaelle; Partoll, Eva; Leiminger, Markus; Velarde, Fernando; Laj, Paolo; Ginot, Patrick; Artaxo, Paolo; Wiedensohler, Alfred; Kulmala, Markku; Mohr, Claudia; Andrade, Marcos; Sinclair, Victoria; Bianchi, Federico; Hansel, ArminDimethyl sulfide (DMS) is the primary natural contributor to the atmospheric sulfur burden. Observations concerning the fate of DMS oxidation products after long-range transport in the remote free troposphere are, however, sparse. Here we present quantitative chemical ionization mass spectrometric measurements of DMS and its oxidation products sulfuric acid (H2SO4), methanesulfonic acid (MSA), dimethylsulfoxide (DMSO), dimethylsulfone (DMSO2), methanesulfinic acid (MSIA), methyl thioformate (MTF), methanesulfenic acid (MSEA, CH3SOH), and a compound of the likely structure CH3S(O)2OOH in the gas phase, as well as measurements of the sulfate and methanesulfonate aerosol mass fractions. The measurements were performed at the Global Atmosphere Watch (GAW) station Chacaltaya in the Bolivian Andes located at 5240m above sea level (a.s.l.). DMS and DMS oxidation products are brought to the Andean high-altitude station by Pacific air masses during the dry season after convective lifting over the remote Pacific ocean to 6000-8000ma.s.l. and subsequent long-range transport in the free troposphere (FT). Most of the DMS reaching the station is already converted to the rather unreactive sulfur reservoirs DMSO2 in the gas phase and methanesulfonate (MS-) in the particle phase, which carried nearly equal amounts of sulfur to the station. The particulate sulfate at Chacaltaya is however dominated by regional volcanic emissions during the time of the measurement and not significantly affected by the marine air masses. In one of the FT events, even some DMS was observed next to reactive intermediates such as methyl thioformate, dimethylsulfoxide, and methanesulfinic acid. Also for this event, back trajectory calculations show that the air masses came from above the ocean (distance >330km) with no local surface contacts. This study demonstrates the potential impact of marine DMS emissions on the availability of sulfur-containing vapors in the remote free troposphere far away from the ocean.