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- ItemLong-term studies of mesosphere and lower-thermosphere summer length definitions based on mean zonal wind features observed for more than one solar cycle at middle and high latitudes in the Northern Hemisphere(Katlenburg, Lindau : Copernicus, 2022) Jaen, Juliana; Renkwitz, Toralf; Chau, Jorge L.; He, Maosheng; Hoffmann, Peter; Yamazaki, Yosuke; Jacobi, Christoph; Tsutsumi, Masaki; Matthias, Vivien; Hall, ChrisSpecular meteor radars (SMRs) and partial reflection radars (PRRs) have been observing mesospheric winds for more than a solar cycle over Germany (g1/4g54g gN) and northern Norway (g1/4g69g gN). This work investigates the mesospheric mean zonal wind and the zonal mean geostrophic zonal wind from the Microwave Limb Sounder (MLS) over these two regions between 2004 and 2020. Our study focuses on the summer when strong planetary waves are absent and the stratospheric and tropospheric conditions are relatively stable. We establish two definitions of the summer length according to the zonal wind reversals: (1) the mesosphere and lower-thermosphere summer length (MLT-SL) using SMR and PRR winds and (2) the mesosphere summer length (M-SL) using the PRR and MLS. Under both definitions, the summer begins around April and ends around middle September. The largest year-to-year variability is found in the summer beginning in both definitions, particularly at high latitudes, possibly due to the influence of the polar vortex. At high latitudes, the year 2004 has a longer summer length compared to the mean value for MLT-SL as well as 2012 for both definitions. The M-SL exhibits an increasing trend over the years, while MLT-SL does not have a well-defined trend. We explore a possible influence of solar activity as well as large-scale atmospheric influences (e.g., quasi-biennial oscillation (QBO), El Niño-Southern Oscillation (ENSO), major sudden stratospheric warming events). We complement our work with an extended time series of 31 years at middle latitudes using only PRR winds. In this case, the summer length shows a breakpoint, suggesting a non-uniform trend, and periods similar to those known for ENSO and QBO.
- ItemThe realization of autonomous, aircraft-based, real-time aerosol mass spectrometry in the upper troposphere and lower stratosphere(Katlenburg-Lindau : Copernicus, 2022) Dragoneas, Antonis; Molleker, Sergej; Appel, Oliver; Hünig, Andreas; Böttger, Thomas; Hermann, Markus; Drewnick, Frank; Schneider, Johannes; Weigel, Ralf; Borrmann, StephanWe report on the developments that enabled the field deployment of a fully automated aerosol mass spectrometer, especially designed for high-altitude measurements on unpressurized aircraft. The merits of the two main categories of real-time aerosol mass spectrometry, i.e. (a) single-particle laser desorption and ionization and (b) continuous thermal desorption and electron impact ionization of aerosols, have been integrated into one compact apparatus with the aim to perform in situ real-time analysis of aerosol chemical composition. The demonstrated instrument, named the ERICA (European Research Council Instrument for Chemical composition of Aerosols), operated successfully aboard the high-altitude research aircraft M-55 Geophysica at altitudes up to 20 km while being exposed to ambient conditions of very low atmospheric pressure and temperature. A primary goal of those field deployments was the in situ study of the Asian tropopause aerosol layer (ATAL). During 11 research flights, the instrument operated for more than 49 h and collected chemical composition information of more than 150 000 single particles combined with quantitative chemical composition analysis of aerosol particle ensembles. This paper presents in detail the technical characteristics of the main constituent parts of the instrument, as well as the design considerations for its integration into the aircraft and its autonomous operation in the upper troposphere and lower stratosphere (UTLS). Additionally, system performance data from the first field deployments of the instrument are presented and discussed, together with exemplary mass spectrometry data collected during those flights.
- ItemCAMP: An instrumented platform for balloon-borne aerosol particle studies in the lower atmosphere(Katlenburg-Lindau : Copernicus, 2022) Pilz, Christian; Düsing, Sebastian; Wehner, Birgit; Müller, Thomas; Siebert, Holger; Voigtländer, Jens; Lonardi, MichaelAirborne observations of vertical aerosol particle distributions are crucial for detailed process studies and model improvements. Tethered balloon systems represent a less expensive alternative to aircraft to probe shallow atmospheric boundary layers (ABLs). This study presents the newly developed cubic aerosol measurement platform (CAMP) for balloon-borne observations of aerosol particle microphysical properties. With an edge length of 35 cm and a weight of 9 kg, the cube is an environmentally robust instrument platform intended for measurements at low temperatures, with a particular focus on applications in cloudy Arctic ABLs. The aerosol instrumentation on board CAMP comprises two condensation particle counters with different lower detection limits, one optical particle size spectrometer, and a miniaturized absorption photometer. Comprehensive calibrations and characterizations of the instruments were performed in laboratory experiments. The first field study with a tethered balloon system took place at the Leibniz Institute for Tropospheric Research (TROPOS) station in Melpitz, Germany, in the winter of 2019. At ambient temperatures between-8 and 15 C, the platform was operated up to a 1.5 km height on 14 flights under both clear-sky and cloudy conditions. The continuous aerosol observations at the ground station served as a reference for evaluating the CAMP measurements. Exemplary profiles are discussed to elucidate the performance of the system and possible process studies. Based on the laboratory instrument characterizations and the observations during the field campaign, CAMP demonstrated the capability to provide comprehensive aerosol particle measurements in cold and cloudy ABLs.
- 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.
- 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: