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- ItemA phenomenology of new particle formation (NPF) at 13 European sites(Katlenburg-Lindau : European Geosciences Union, 2021) Bousiotis, Dimitrios; Pope, Francis D.; Beddows, David C. S.; Dall'Osto, Manuel; Massling, Andreas; Nøjgaard, Jakob Klenø; Nordstrøm, Claus; Niemi, Jarkko V.; Portin, Harri; Petäjä, Tuukka; Perez, Noemi; Alastuey, Andrés; Querol, Xavier; Kouvarakis, Giorgos; Mihalopoulos, Nikos; Vratolis, Stergios; Eleftheriadis, Konstantinos; Wiedensohler, Alfred; Weinhold, Kay; Merkel, Maik; Tuch, Thomas; Harrison, Roy M.New particle formation (NPF) events occur almost everywhere in the world and can play an important role as a particle source. The frequency and characteristics of NPF events vary spatially, and this variability is yet to be fully understood. In the present study, long-term particle size distribution datasets (minimum of 3 years) from 13 sites of various land uses and climates from across Europe were studied, and NPF events, deriving from secondary formation and not traffic-related nucleation, were extracted and analysed. The frequency of NPF events was consistently found to be higher at rural background sites, while the growth and formation rates of newly formed particles were higher at roadsides (though in many cases differences between the sites were small), underlining the importance of the abundance of condensable compounds of anthropogenic origin found there. The growth rate was higher in summer at all rural background sites studied. The urban background sites presented the highest uncertainty due to greater variability compared to the other two types of site. The origin of incoming air masses and the specific conditions associated with them greatly affect the characteristics of NPF events. In general, cleaner air masses present higher probability for NPF events, while the more polluted ones show higher growth rates. However, different patterns of NPF events were found, even at sites in close proximity (<ĝ€¯200ĝ€¯km), due to the different local conditions at each site. Region-wide events were also studied and were found to be associated with the same conditions as local events, although some variability was found which was associated with the different seasonality of the events at two neighbouring sites. NPF events were responsible for an increase in the number concentration of ultrafine particles of more than 400ĝ€¯% at rural background sites on the day of their occurrence. The degree of enhancement was less at urban sites due to the increased contribution of other sources within the urban environment. It is evident that, while some variables (such as solar radiation intensity, relative humidity, or the concentrations of specific pollutants) appear to have a similar influence on NPF events across all sites, it is impossible to predict the characteristics of NPF events at a site using just these variables, due to the crucial role of local conditions. © Author(s) 2021.
- ItemInfluence of low-level blocking and turbulence on the microphysics of a mixed-phase cloud in an inner-Alpine valley(Katlenburg-Lindau : European Geosciences Union, 2021) Ramelli, Fabiola; Henneberger, Jan; David, Robert O.; Lauber, Annika; Pasquier, Julie T.; Wieder, Jörg; Bühl, Johannes; Seifert, Patric; Engelmann, Ronny; Hervo, Maxime; Lohmann, UlrikePrevious studies that investigated orographic precipitation have primarily focused on isolated mountain barriers. Here we investigate the influence of low-level blocking and shear-induced turbulence on the cloud microphysics and precipitation formation in a complex inner-Alpine valley. The analysis focuses on a mid-level cloud in a post-frontal environment and a low-level feeder cloud induced by an in-valley circulation. Observations were obtained from an extensive set of instruments including ground-based remote sensing instrumentation, in situ instrumentation on a tethered-balloon system and ground-based precipitation measurements. During this event, the boundary layer was characterized by a blocked low-level flow and enhanced turbulence in the region of strong vertical wind shear at the boundary between the blocked layer in the valley and the stronger cross-barrier flow aloft. Cloud radar observations indicated changes in the microphysical cloud properties within the turbulent shear layer including enhanced linear depolarization ratio (i.e., change in particle shape or density) and increased radar reflectivity (i.e., enhanced ice growth). Based on the ice particle habits observed at the surface, we suggest that riming, aggregation and needle growth occurred within the turbulent layer. Collisions of fragile ice crystals (e.g., dendrites, needles) and the Hallett-Mossop process might have contributed to secondary ice production. Additionally, in situ instrumentation on the tethered-balloon system observed the presence of a low-level feeder cloud above a small-scale topographic feature, which dissipated when the low-level flow turned from a blocked to an unblocked state. Our observations indicate that the low-level blocking (due to the downstream mountain barrier) created an in-valley circulation, which led to the production of local updrafts and the formation of a low-level feeder cloud. Although the feeder cloud did not enhance precipitation in this particular case (since the majority of the precipitation sublimated when falling through a subsaturated layer above), we propose that local flow effects such as low-level blocking can induce the formation of feeder clouds in mountain valleys and on the leeward slope of foothills upstream of the main mountain barrier, where they can act to enhance orographic precipitation through the seeder-feeder mechanism.
- ItemCase study of a humidity layer above Arctic stratocumulus and potential turbulent coupling with the cloud top(Katlenburg-Lindau : European Geosciences Union, 2021) Egerer, Ulrike; Ehrlich, André; Gottschalk, Matthias; Griesche, Hannes; Neggers, Roel A.J.; Siebert, Holger; Wendisch, ManfredSpecific humidity inversions (SHIs) above low-level cloud layers have been frequently observed in the Arctic. The formation of these SHIs is usually associated with large-scale advection of humid air masses. However, the potential coupling of SHIs with cloud layers by turbulent processes is not fully understood. In this study, we analyze a 3 d period of a persistent layer of increased specific humidity above a stratocumulus cloud observed during an Arctic field campaign in June 2017. The tethered balloon system BELUGA (Balloon-bornE moduLar Utility for profilinG the lower Atmosphere) recorded vertical profile data of meteorological, turbulence, and radiation parameters in the atmospheric boundary layer. An in-depth discussion of the problems associated with humidity measurements in cloudy environments leads to the conclusion that the observed SHIs do not result from measurement artifacts. We analyze two different scenarios for the SHI in relation to the cloud top capped by a temperature inversion: (i) the SHI coincides with the cloud top, and (ii) the SHI is vertically separated from the lowered cloud top. In the first case, the SHI and the cloud layer are coupled by turbulence that extends over the cloud top and connects the two layers by turbulent mixing. Several profiles reveal downward virtual sensible and latent heat fluxes at the cloud top, indicating entrainment of humid air supplied by the SHI into the cloud layer. For the second case, a downward moisture transport at the base of the SHI and an upward moisture flux at the cloud top is observed. Therefore, the area between the cloud top and SHI is supplied with moisture from both sides. Finally, large-eddy simulations (LESs) complement the observations by modeling a case of the first scenario. The simulations reproduce the observed downward turbulent fluxes of heat and moisture at the cloud top. The LES realizations suggest that in the presence of a SHI, the cloud layer remains thicker and the temperature inversion height is elevated.
- ItemTropospheric and stratospheric wildfire smoke profiling with lidar: mass, surface area, CCN, and INP retrieval(Katlenburg-Lindau : European Geosciences Union, 2021) Ansmann, Albert; Ohneiser, Kevin; Mamouri, Rodanthi-Elisavet; Knopf, Daniel A.; Veselovskii, Igor; Baars, Holger; Engelmann, Ronny; Foth, Andreas; Jimenez, Cristofer; Seifert, Patric; Barja, BorisWe present retrievals of tropospheric and stratospheric height profiles of particle mass, volume, surface area, and number concentrations in the case of wildfire smoke layers as well as estimates of smoke-related cloud condensation nuclei (CCN) and ice-nucleating particle (INP) concentrations from backscatter lidar measurements on the ground and in space. Conversion factors used to convert the optical measurements into microphysical properties play a central role in the data analysis, in addition to estimates of the smoke extinction-to-backscatter ratios required to obtain smoke extinction coefficients. The set of needed conversion parameters for wildfire smoke is derived from AERONET observations of major smoke events, e.g., in western Canada in August 2017, California in September 2020, and southeastern Australia in January-February 2020 as well as from AERONET long-term observations of smoke in the Amazon region, southern Africa, and Southeast Asia. The new smoke analysis scheme is applied to CALIPSO observations of tropospheric smoke plumes over the United States in September 2020 and to ground-based lidar observation in Punta Arenas, in southern Chile, in aged Australian smoke layers in the stratosphere in January 2020. These case studies show the potential of spaceborne and ground-based lidars to document large-scale and long-lasting wildfire smoke events in detail and thus to provide valuable information for climate, cloud, and air chemistry modeling efforts performed to investigate the role of wildfire smoke in the atmospheric system. © 2021 Albert Ansmann et al.
- ItemEvaluating stratospheric ozone and water vapour changes in CMIP6 models from 1850 to 2100(Katlenburg-Lindau : European Geosciences Union, 2021) Keeble, James; Hassler, Birgit; Banerjee, Antara; Checa-Garcia, Ramiro; Chiodo, Gabriel; Davis, Sean; Eyring, Veronika; Griffiths, Paul T.; Morgenstern, Olaf; Nowack, Peer; Zeng, Guang; Zhang, Jiankai; Bodeker, Greg; Burrows, Susannah; Cameron-Smith, Philip; Cugnet, David; Danek, Christopher; Deushi, Makoto; Horowitz, Larry W.; Kubin, Anne; Li, Lijuan; Lohmann, Gerrit; Michou, Martine; Mills, Michael J.; Nabat, Pierre; Olivié, Dirk; Park, Sungsu; Seland, Øyvind; Stoll, Jens; Wieners, Karl-Hermann; Wu, TongwenStratospheric ozone and water vapour are key components of the Earth system, and past and future changes to both have important impacts on global and regional climate. Here, we evaluate long-term changes in these species from the pre-industrial period (1850) to the end of the 21st century in Coupled Model Intercomparison Project phase 6 (CMIP6) models under a range of future emissions scenarios. There is good agreement between the CMIP multi-model mean and observations for total column ozone (TCO), although there is substantial variation between the individual CMIP6 models. For the CMIP6 multi-model mean, global mean TCO has increased from ∼300 DU in 1850 to ∼ 305 DU in 1960, before rapidly declining in the 1970s and 1980s following the use and emission of halogenated ozone-depleting substances (ODSs). TCO is projected to return to 1960s values by the middle of the 21st century under the SSP2-4.5, SSP3-7.0, SSP4-3.4, SSP4-6.0, and SSP5-8.5 scenarios, and under the SSP3-7.0 and SSP5-8.5 scenarios TCO values are projected to be ∼ 10 DU higher than the 1960s values by 2100. However, under the SSP1-1.9 and SSP1-1.6 scenarios, TCO is not projected to return to the 1960s values despite reductions in halogenated ODSs due to decreases in tropospheric ozone mixing ratios. This global pattern is similar to regional patterns, except in the tropics where TCO under most scenarios is not projected to return to 1960s values, either through reductions in tropospheric ozone under SSP1-1.9 and SSP1-2.6, or through reductions in lower stratospheric ozone resulting from an acceleration of the Brewer-Dobson circulation under other Shared Socioeconomic Pathways (SSPs). In contrast to TCO, there is poorer agreement between the CMIP6 multi-model mean and observed lower stratospheric water vapour mixing ratios, with the CMIP6 multi-model mean underestimating observed water vapour mixing ratios by ∼ 0.5 ppmv at 70 hPa. CMIP6 multi-model mean stratospheric water vapour mixing ratios in the tropical lower stratosphere have increased by ∼ 0.5 ppmv from the pre-industrial to the present-day period and are projected to increase further by the end of the 21st century. The largest increases (∼ 2 ppmv) are simulated under the future scenarios with the highest assumed forcing pathway (e.g. SSP5-8.5). Tropical lower stratospheric water vapour, and to a lesser extent TCO, shows large variations following explosive volcanic eruptions. © Author(s) 2021.
- ItemAcidity and the multiphase chemistry of atmospheric aqueous particles and clouds(Katlenburg-Lindau : European Geosciences Union, 2021) Tilgner, Andreas; Schaefer, Thomas; Alexander, Becky; Barth, Mary; Collett, Jeffrey L.; Fahey, Kathleen M.; Nenes, Athanasios; Pye, Havala O.T.; Herrmann, Hartmut; McNeill, V. FayeThe acidity of aqueous atmospheric solutions is a key parameter driving both the partitioning of semi-volatile acidic and basic trace gases and their aqueous-phase chemistry. In addition, the acidity of atmospheric aqueous phases, e.g., deliquesced aerosol particles, cloud, and fog droplets, is also dictated by aqueous-phase chemistry. These feedbacks between acidity and chemistry have crucial implications for the tropospheric lifetime of air pollutants, atmospheric composition, deposition to terrestrial and oceanic ecosystems, visibility, climate, and human health. Atmospheric research has made substantial progress in understanding feedbacks between acidity and multiphase chemistry during recent decades. This paper reviews the current state of knowledge on these feedbacks with a focus on aerosol and cloud systems, which involve both inorganic and organic aqueous-phase chemistry. Here, we describe the impacts of acidity on the phase partitioning of acidic and basic gases and buffering phenomena. Next, we review feedbacks of different acidity regimes on key chemical reaction mechanisms and kinetics, as well as uncertainties and chemical subsystems with incomplete information. Finally, we discuss atmospheric implications and highlight the need for future investigations, particularly with respect to reducing emissions of key acid precursors in a changing world, and the need for advancements in field and laboratory measurements and model tools.
- ItemTerrestrial or marine – indications towards the origin of ice-nucleating particles during melt season in the European Arctic up to 83.7° N(Katlenburg-Lindau : European Geosciences Union, 2021) Hartmann, Markus; Gong, Xianda; Kecorius, Simonas; van Pinxteren, Manuela; Vogl, Teresa; Welti, André; Wex, Heike; Zeppenfeld, Sebastian; Herrmann, Hartmut; Wiedensohler, Alfred; Stratmann, FrankIce-nucleating particles (INPs) initiate the primary ice formation in clouds at temperatures above ca. -38gC and have an impact on precipitation formation, cloud optical properties, and cloud persistence. Despite their roles in both weather and climate, INPs are not well characterized, especially in remote regions such as the Arctic. We present results from a ship-based campaign to the European Arctic during May to July 2017. We deployed a filter sampler and a continuous-flow diffusion chamber for offline and online INP analyses, respectively. We also investigated the ice nucleation properties of samples from different environmental compartments, i.e., the sea surface microlayer (SML), the bulk seawater (BSW), and fog water. Concentrations of INPs (NINP) in the air vary between 2 to 3 orders of magnitudes at any particular temperature and are, except for the temperatures above -10gC and below -32gC, lower than in midlatitudes. In these temperature ranges, INP concentrations are the same or even higher than in the midlatitudes. By heating of the filter samples to 95gC for 1ĝ€¯h, we found a significant reduction in ice nucleation activity, i.e., indications that the INPs active at warmer temperatures are biogenic. At colder temperatures the INP population was likely dominated by mineral dust. The SML was found to be enriched in INPs compared to the BSW in almost all samples. The enrichment factor (EF) varied mostly between 1 and 10, but EFs as high as 94.97 were also observed. Filtration of the seawater samples with 0.2ĝ€¯μm syringe filters led to a significant reduction in ice activity, indicating the INPs are larger and/or are associated with particles larger than 0.2ĝ€¯μm. A closure study showed that aerosolization of SML and/or seawater alone cannot explain the observed airborne NINP unless significant enrichment of INP by a factor of 105 takes place during the transfer from the ocean surface to the atmosphere. In the fog water samples with -3.47gC, we observed the highest freezing onset of any sample. A closure study connecting NINP in fog water and the ambient NINP derived from the filter samples shows good agreement of the concentrations in both compartments, which indicates that INPs in the air are likely all activated into fog droplets during fog events. In a case study, we considered a situation during which the ship was located in the marginal sea ice zone and NINP levels in air and the SML were highest in the temperature range above -10gC. Chlorophyll a measurements by satellite remote sensing point towards the waters in the investigated region being biologically active. Similar slopes in the temperature spectra suggested a connection between the INP populations in the SML and the air. Air mass history had no influence on the observed airborne INP population. Therefore, we conclude that during the case study collected airborne INPs originated from a local biogenic probably marine source. © Author(s) 2021.
- ItemIdentification and source attribution of organic compounds in ultrafine particles near Frankfurt International Airport(Katlenburg-Lindau : European Geosciences Union, 2021) Ungeheuer, Florian; van Pinxteren, Dominik; Vogel, Alexander L.Analysing the composition of ambient ultrafine particles (UFPs) is a challenging task due to the low mass and chemical complexity of small particles, yet it is a prerequisite for the identification of particle sources and the assessment of potential health risks. Here, we show the molecular characterization of UFPs, based on cascade impactor (Nano-MOUDI) samples that were collected at an air quality monitoring station near one of Europe's largest airports, in Frankfurt, Germany. At this station, particle-size-distribution measurements show an enhanced number concentration of particles smaller than 50 nm during airport operating hours. We sampled the lower UFP fraction (0.010-0.018, 0.018-0.032, 0.032-0.056 classCombining double low lineinline-formula/m) when the air masses arrived from the airport. We developed an optimized filter extraction procedure using ultra-high-performance liquid chromatography (UHPLC) for compound separation and a heated electrospray ionization (HESI) source with an Orbitrap high-resolution mass spectrometer (HRMS) as a detector for organic compounds. A non-Target screening detected classCombining double low lineinline-formulag1/4200/ organic compounds in the UFP fraction with sample-To-blank ratios larger than 5. We identified the largest signals as homologous series of pentaerythritol esters (PEEs) and trimethylolpropane esters (TMPEs), which are base stocks of aircraft lubrication oils. We unambiguously attribute the majority of detected compounds to jet engine lubrication oils by matching retention times, high-resolution and accurate mass measurements, and comparing tandem mass spectrometry (MS classCombining double low lineinline-formula2/) fragmentation patterns between both ambient samples and commercially available jet oils. For each UFP stage, we created molecular fingerprints to visualize the complex chemical composition of the organic fraction and their average carbon oxidation state. These graphs underline the presence of the homologous series of PEEs and TMPEs and the appearance of jet oil additives (e.g.Tricresyl phosphate, TCP). Targeted screening of TCP confirmed the absence of the harmful tri-iortho/i isomer, while we identified a thermal transformation product of TMPE-based lubrication oil (trimethylolpropane phosphate, TMP-P). Even though a quantitative determination of the identified compounds is limited, the presented method enables the qualitative detection of molecular markers for jet engine lubricants in UFPs and thus strongly improves the source apportionment of UFPs near airports./p. © 2021 BMJ Publishing Group. All rights reserved.
- ItemWildfire smoke, Arctic haze, and aerosol effects on mixed-phase and cirrus clouds over the North Pole region during MOSAiC: an introduction(Katlenburg-Lindau : European Geosciences Union, 2021) Engelmann, Ronny; Ansmann, Albert; Ohneiser, Kevin; Griesche, Hannes; Radenz, Martin; Hofer, Julian; Althausen, Dietrich; Dahlke, Sandro; Maturilli, Marion; Veselovskii, Igor; Jimenez, Cristofer; Wiesen, Robert; Baars, Holger; Bühl, Johannes; Gebauer, Henriette; Haarig, Moritz; Seifert, Patric; Wandinger, Ulla; Macke, AndreasAn advanced multiwavelength polarization Raman lidar was operated aboard the icebreaker Polarstern during the MOSAiC (Multidisciplinary drifting Observatory for the Study of Arctic Climate) expedition to continuously monitor aerosol and cloud layers in the central Arctic up to 30gkm height. The expedition lasted from September 2019 to October 2020 and measurements were mostly taken between 85 and 88.5ggN. The lidar was integrated into a complex remote-sensing infrastructure aboard the Polarstern. In this article, novel lidar techniques, innovative concepts to study aerosol-cloud interaction in the Arctic, and unique MOSAiC findings will be presented. The highlight of the lidar measurements was the detection of a 10gkm deep wildfire smoke layer over the North Pole region between 7-8gkm and 17-18gkm height with an aerosol optical thickness (AOT) at 532gnm of around 0.1 (in October-November 2019) and 0.05 from December to March. The dual-wavelength Raman lidar technique allowed us to unambiguously identify smoke as the dominating aerosol type in the aerosol layer in the upper troposphere and lower stratosphere (UTLS). An additional contribution to the 532gnm AOT by volcanic sulfate aerosol (Raikoke eruption) was estimated to always be lower than 15g%. The optical and microphysical properties of the UTLS smoke layer are presented in an accompanying paper . This smoke event offered the unique opportunity to study the influence of organic aerosol particles (serving as ice-nucleating particles, INPs) on cirrus formation in the upper troposphere. An example of a closure study is presented to explain our concept of investigating aerosol-cloud interaction in this field. The smoke particles were obviously able to control the evolution of the cirrus system and caused low ice crystal number concentration. After the discussion of two typical Arctic haze events, we present a case study of the evolution of a long-lasting mixed-phase cloud layer embedded in Arctic haze in the free troposphere. The recently introduced dual-field-of-view polarization lidar technique was applied, for the first time, to mixed-phase cloud observations in order to determine the microphysical properties of the water droplets. The mixed-phase cloud closure experiment (based on combined lidar and radar observations) indicated that the observed aerosol levels controlled the number concentrations of nucleated droplets and ice crystals.
- ItemIntercomparison and characterization of 23 Aethalometers under laboratory and ambient air conditions: procedures and unit-to-unit variabilities(Katlenburg-Lindau : European Geosciences Union, 2021) Cuesta-Mosquera, Andrea; Močnik, Griša; Drinovec, Luka; Müller, Thomas; Pfeifer, Sascha; Minguillón, María Cruz; Briel, Björn; Buckley, Paul; Dudoitis, Vadimas; Fernández-García, Javier; Fernández-Amado, María; Ferreira De Brito, Joel; Riffault, Veronique; Flentje, Harald; Heffernan, Eimear; Kalivitis, Nikolaos; Kalogridis, Athina-Cerise; Keernik, Hannes; Marmureanu, Luminita; Luoma, Krista; Marinoni, Angela; Pikridas, Michael; Schauer, Gerhard; Serfozo, Norbert; Servomaa, Henri; Titos, Gloria; Yus-Díez, Jesús; Zioła, Natalia; Wiedensohler, AlfredAerosolized black carbon is monitored worldwide to quantify its impact on air quality and climate. Given its importance, measurements of black carbon mass concentrations must be conducted with instruments operating in qualitychecked and ensured conditions to generate data which are reliable and comparable temporally and geographically. In this study, we report the results from the largest characterization and intercomparison of filter-based absorption photometers, the Aethalometer model AE33, belonging to several European monitoring networks. Under controlled laboratory conditions, a total of 23 instruments measured mass concentrations of black carbon from three wellcharacterized aerosol sources: synthetic soot, nigrosin particles, and ambient air from the urban background of Leipzig, Germany. The objective was to investigate the individual performance of the instruments and their comparability; we analyzed the response of the instruments to the different aerosol sources and the impact caused by the use of obsolete filter materials and the application of maintenance activities. Differences in the instrument-to-instrument variabilities from equivalent black carbon (eBC) concentrations reported at 880 nm were determined before maintenance activities (for soot measurements, average deviation from total least square regression was-2.0% and the range-16% to 7 %; for nigrosin measurements, average deviation was 0.4% and the range-15% to 17 %), and after they were carried out (for soot measurements, average deviation was-1.0% and the range-14% to 8 %; for nigrosin measurements, the average deviation was 0.5%and the range-12%to 15 %). The deviations are in most of the cases explained by the type of filter material employed by the instruments, the total particle load on the filter, and the flow calibration. The results of this intercomparison activity show that relatively small unit-to-unit variability of AE33-based particle light absorbing measurements is possible with wellmaintained instruments. It is crucial to follow the guidelines for maintenance activities and the use of the proper filter tape in the AE33 to ensure high quality and comparable black carbon (BC) measurements among international observational networks. © 2021 Author(s). This work is distributed under the Creative Commons Attribution 4.0 License.
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