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- 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.
- 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.
- ItemExperimental assessment of a micro-pulse lidar system in comparison with reference lidar measurements for aerosol optical properties retrieval(Katlenburg-Lindau : European Geosciences Union, 2021) Córdoba-Jabonero, Carmen; Ansmann, Albert; Jiménez, Cristofer; Baars, Holger; López-Cayuela, María-Ángeles; Engelmann, RonnySimultaneous observations of a polarized micro-pulse lidar (P-MPL) system and two reference European Aerosol Research Lidar Network lidars running at the Leipzig site Germany, 51.4g gN, 12.4g gE; 125gmga.s.l.) were performed during a comprehensive 2-month field intercomparison campaign in summer 2019. An experimental assessment regarding both the overlap (OVP) correction of the P-MPL signal profiles and the volume linear depolarization ratio (VLDR) analysis, together with its impact on the retrieval of the aerosol optical properties, is achieved; the experimental procedure used is also described. The optimal lidar-specific OVP function is experimentally determined, highlighting that the one delivered by the P-MPL manufacturer cannot be used long. Among the OVP functions examined, the averaged function between those obtained from the comparison of the P-MPL observations with those of the other two reference lidars seems to be the best proxy at both near- and far-field ranges. In addition, the impact of the OVP function on the accuracy of the retrieved profiles of the total particle backscatter coefficient (PBC) and the particle linear depolarization ratio (PLDR) is examined. The VLDR profile is obtained and compared with that derived from the reference lidar, showing that it needs to be corrected by a small offset value with good accuracy. Once P-MPL measurements are optimally (OVP, VLDR) corrected, both the PBC and PLDR profiles can be accurately derived and are in good agreement with reference aerosol retrievals. Overall, as a systematic requirement for lidar systems, an adequate OVP function determination and VLDR testing analysis needs to be performed on a regular basis to correct the P-MPL measurements in order to derive suitable aerosol products. A dust event observed in Leipzig in June 2019 is used for illustration.
- ItemVariability in the mass absorption cross section of black carbon (BC) aerosols is driven by BC internal mixing state at a central European background site (Melpitz, Germany) in winter(Katlenburg-Lindau : European Geosciences Union, 2021) Yuan, Jinfeng; Modini, Robin Lewis; Zanatta, Marco; Herber, Andreas B.; Müller, Thomas; Wehner, Birgit; Poulain, Laurent; Tuch, Thomas; Baltensperger, Urs; Gysel-Beer, MartinProperties of atmospheric black carbon (BC) particles were characterized during a field experiment at a rural background site (Melpitz, Germany) in February 2017. BC absorption at a wavelength of 870 nm was measured by a photoacoustic extinctiometer, and BC physical properties (BC mass concentration, core size distribution and coating thickness) were measured by a single-particle soot photometer (SP2). Additionally, a catalytic stripper was used to intermittently remove BC coatings by alternating between ambient and thermo-denuded conditions. From these data the mass absorption cross section of BC (MACBC) and its enhancement factor (EMAC) were inferred for essentially waterfree aerosol as present after drying to low relative humidity (RH). Two methods were applied independently to investigate the coating effect on EMAC: A correlation method (MACBC; ambient vs. BC coating thickness) and a denuding method (MACBC; ambient vs. MACBC; denuded). Observed EMAC values varied from 1.0 to 1.6 (lower limit from denuding method) or 1:2 to 1.9 (higher limit from correlation method), with the mean coating volume fraction ranging from 54% to 78% in the dominating mass equivalent BC core diameter range of 200?220 nm.MACBC and EMAC were strongly correlated with coating thickness of BC. By contrast, other potential drivers of EMAC variability, such as different BC sources (air mass origin and absorption Angström exponent), coating composition (ratio of inorganics to organics) and BC core size distribution, had only minor effects. These results for ambient BC measured at Melpitz during winter show that the lensing effect caused by coatings on BC is the main driver of the variations in MACBC and EMAC, while changes in other BC particle properties such as source, BC core size or coating composition play only minor roles at this rural background site with a large fraction of aged particles. Indirect evidence suggests that potential dampening of the lensing effect due to unfavorable morphology was most likely small or even negligible.
- ItemContrasting ice formation in Arctic clouds: surface-coupled vs. surface-decoupled clouds(Katlenburg-Lindau : European Geosciences Union, 2021) Griesche, Hannes J.; Ohneiser, Kevin; Seifert, Patric; Radenz, Martin; Engelmann, Ronny; Ansmann, AlbertIn the Arctic summer of 2017 (1 June to 16 July) measurements with the OCEANET-Atmosphere facility were performed during the Polarstern cruise PS106. OCEANET comprises amongst other instruments the multiwavelength polarization lidar PollyXT_OCEANET and for PS106 was complemented with a vertically pointed 35 GHz cloud radar. In the scope of the presented study, the influence of cloud height and surface coupling on the probability of clouds to contain and form ice is investigated. Polarimetric lidar data were used for the detection of the cloud base and the identification of the thermodynamic phase. Both radar and lidar were used to detect cloud top. Radiosonde data were used to derive the thermodynamic structure of the atmosphere and the clouds. The analyzed data set shows a significant impact of the surface-coupling state on the probability of ice formation. Surface-coupled clouds were identified by a quasi-constant potential temperature profile from the surface up to liquid layer base. Within the same minimum cloud temperature range, ice-containing clouds have been observed more frequently than surface-decoupled clouds by a factor of up to 6 (temperature intervals between -7.5 and -5 C, 164 vs. 27 analyzed intervals of 30 min). The frequency of occurrence of surface-coupled ice-containing clouds was found to be 2-3 times higher (e.g., 82% vs. 35% between -7.5 and -5 C). These findings provide evidence that above -10 C heterogeneous ice formation in Arctic mixed-phase clouds occurs by a factor of 2-6 more often when the cloud layer is coupled to the surface. In turn, for minimum cloud temperatures below -15 C, the frequency of ice-containing clouds for coupled and decoupled conditions approached the respective curve for the central European site of Leipzig, Germany (51 N, 12 E). This corroborates the hypothesis that the free-tropospheric ice nucleating particle (INP) reservoir over the Arctic is controlled by continental aerosol. Two sensitivity studies, also using the cloud radar for detection of ice particles and applying a modified coupling state detection, both confirmed the findings, albeit with a lower magnitude. Possible explanations for the observations are discussed by considering recent in situ measurements of INP in the Arctic, of which much higher concentrations were found in the surface-coupled atmosphere in close vicinity to the ice shore.
- ItemChanges in black carbon emissions over Europe due to COVID-19 lockdowns(Katlenburg-Lindau : European Geosciences Union, 2021) Evangeliou, Nikolaos; Platt, Stephen M.; Eckhardt, Sabine; Lund Myhre, Cathrine; Laj, Paolo; Alados-Arboledas, Lucas; Backman, John; Brem, Benjamin T.; Fiebig, Markus; Flentje, Harald; Marinoni, Angela; Pandolfi, Marco; Yus-Dìez, Jesus; Prats, Natalia; Putaud, Jean P.; Sellegri, Karine; Sorribas, Mar; Eleftheriadis, Konstantinos; Vratolis, Stergios; Wiedensohler, Alfred; Stohl, AndreasFollowing the emergence of the severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) responsible for COVID-19 in December 2019 in Wuhan (China) and its spread to the rest of the world, the World Health Organization declared a global pandemic in March 2020. Without effective treatment in the initial pandemic phase, social distancing and mandatory quarantines were introduced as the only available preventative measure. In contrast to the detrimental societal impacts, air quality improved in all countries in which strict lockdowns were applied, due to lower pollutant emissions. Here we investigate the effects of the COVID-19 lockdowns in Europe on ambient black carbon (BC), which affects climate and damages health, using in situ observations from 17 European stations in a Bayesian inversion framework. BC emissions declined by 23 kt in Europe (20 % in Italy, 40 % in Germany, 34 % in Spain, 22 % in France) during lockdowns compared to the same period in the previous 5 years, which is partially attributed to COVID-19 measures. BC temporal variation in the countries enduring the most drastic restrictions showed the most distinct lockdown impacts. Increased particle light absorption in the beginning of the lockdown, confirmed by assimilated satellite and remote sensing data, suggests residential combustion was the dominant BC source. Accordingly, in central and Eastern Europe, which experienced lower than average temperatures, BC was elevated compared to the previous 5 years. Nevertheless, an average decrease of 11 % was seen for the whole of Europe compared to the start of the lockdown period, with the highest peaks in France (42 %), Germany (21 %), UK (13 %), Spain (11 %) and Italy (8 %). Such a decrease was not seen in the previous years, which also confirms the impact of COVID-19 on the European emissions of BC.
- ItemFirst triple-wavelength lidar observations of depolarization and extinction-to-backscatter ratios of Saharan dus(Katlenburg-Lindau : EGU, 2022) Haarig, Moritz; Ansmann, Albert; Engelmann, Ronny; Baars, Holger; Toledano, Carlos; Torres, Benjamin; Althausen, Dietrich; Radenz, Martin; Wandinger, UllaTwo layers of Saharan dust observed over Leipzig, Germany, in February and March 2021 were used to provide the first-ever lidar measurements of the dust lidar ratio (extinction-to-backscatter ratio) and linear depolarization ratio at all three classical lidar wavelengths (355, 532 and 1064gnm). The pure-dust conditions during the first event exhibit lidar ratios of 47g±g8, 50g±g5 and 69g±g14gsr and particle linear depolarization ratios of 0.242g±g0.024, 0.299g±g0.018 and 0.206g±g0.010 at wavelengths of 355, 532 and 1064gnm, respectively. The second, slightly polluted-dust case shows a similar spectral behavior of the lidar and depolarization ratio with values of the lidar ratio of 49g±g4, 46g±g5 and 57g±g9gsr and the depolarization ratio of 0.174g±g0.041, 0.298g±g0.016 and 0.242g±g0.007 at 355, 532 and 1064gnm, respectively. The results were compared with Aerosol Robotic Network (AERONET) version 3 (v3) inversion solutions and the Generalized Retrieval of Aerosol and Surface Properties (GRASP) at six and seven wavelengths. Both retrieval schemes make use of a spheroid shape model for mineral dust. The spectral slope of the lidar ratio from 532 to 1064gnm could be well reproduced by the AERONET and GRASP retrieval schemes. Higher lidar ratios in the UV were retrieved by AERONET and GRASP. The enhancement was probably caused by the influence of fine-mode pollution particles in the boundary layer which are included in the columnar photometer measurements. Significant differences between the measured and retrieved wavelength dependence of the particle linear depolarization ratio were found. The potential sources for these uncertainties are discussed.
- ItemAerosol activation characteristics and prediction at the central European ACTRIS research station of Melpitz, Germany(Katlenburg-Lindau : EGU, 2022) Wang, Yuan; Henning, Silvia; Poulain, Laurent; Lu, Chunsong; Stratmann, Frank; Wang, Yuying; Niu, Shengjie; Pöhlker, Mira L.; Herrmann, Hartmut; Wiedensohler, AlfredUnderstanding aerosol particle activation is essential for evaluating aerosol indirect effects (AIEs) on climate. Long-term measurements of aerosol particle activation help to understand the AIEs and narrow down the uncertainties of AIEs simulation. However, they are still scarce. In this study, more than 4 years of comprehensive aerosol measurements were utilized at the central European research station of Melpitz, Germany, to gain insight into the aerosol particle activation and provide recommendations on improving the prediction of number concentration of cloud condensation nuclei (CCN, NCCN). (1) The overall CCN activation characteristics at Melpitz are provided. As supersaturation (SS) increases from 0.1% to 0.7%, the median NCCN increases from 399 to 2144cm-3, which represents 10% to 48% of the total particle number concentration with a diameter range of 10-800nm, while the median hygroscopicity factor (κ) and critical diameter (Dc) decrease from 0.27 to 0.19 and from 176 to 54nm, respectively. (2) Aerosol particle activation is highly variable across seasons, especially at low-SS conditions. At SSCombining double low line0.1%, the median NCCN and activation ratio (AR) in winter are 1.6 and 2.3 times higher than the summer values, respectively. (3) Both κ and the mixing state are size-dependent. As the particle diameter (Dp) increases, κ increases at Dp of 1/440 to 100nm and almost stays constant at Dp of 100 to 200nm, whereas the degree of the external mixture keeps decreasing at Dp of 1/440 to 200nm. The relationships of κ vs. Dp and degree of mixing vs. Dp were both fitted well by a power-law function. (4) Size-resolved κ improves the NCCN prediction. We recommend applying the κ-Dp power-law fit for NCCN prediction at Melpitz, which performs better than using the constant κ of 0.3 and the κ derived from particle chemical compositions and much better than using the NCCN (AR) vs. SS relationships. The κ-Dp power-law fit measured at Melpitz could be applied to predict NCCN for other rural regions. For the purpose of improving the prediction of NCCN, long-term monodisperse CCN measurements are still needed to obtain the κ-Dp relationships for different regions and their seasonal variations.
- ItemThe role of Antarctic overwintering teams and their significance for German polar research(Göttingen : Copernicus, 2022) Franke, Steven; Eckstaller, Alfons; Heitland, Tim; Schaefer, Thomas; Asseng, JölundGermany has been operating permanently crewed research stations in Antarctica for more than 45 years. The opening of the Georg Forster Station (1976) and Georg von Neumayer Station (1981) initiated a period of continuous environmental monitoring that allowed both the former East Germany and West Germany to become contracting parties in, and achieve consultative status with, the framework of the Antarctic Treaty. This marked a milestone in German polar research. Continuous research at the Neumayer Station III, its two predecessors, and the now-dismantled former German Democratic Republic (GDR) Georg Forster Station is undertaken by teams of so-called "overwinterers", presently with nine members, who stay at the base for longer than an entire Antarctic winter. Their long-Term stay in Antarctica is defined by isolation, separation from civilization, routine work to sustain long-Term scientific observations, and unique personal experiences. This article is dedicated to them and outlines their part and role in the German Antarctic research landscape.
- ItemNucleation of jet engine oil vapours is a large source of aviation-related ultrafine particles(London : Springer Nature, 2022) Ungeheuer, Florian; Caudillo, Lucía; Ditas, Florian; Simon, Mario; van Pinxteren, Dominik; Kılıç, Doğuşhan; Rose, Diana; Jacobi, Stefan; Kürten, Andreas; Curtius, Joachim; Vogel, Alexander L.Large airports are a major source of ultrafine particles, which spread across densely populated residential areas, affecting air quality and human health. Jet engine lubrication oils are detectable in aviation-related ultrafine particles, however, their role in particle formation and growth remains unclear. Here we show the volatility and new-particle-formation ability of a common synthetic jet oil, and the quantified oil fraction in ambient ultrafine particles downwind of Frankfurt International Airport, Germany. We find that the oil mass fraction is largest in the smallest particles (10-18 nm) with 21% on average. Combining ambient particle-phase concentration and volatility of the jet oil compounds, we determine a lower-limit saturation ratio larger than 1 × 105 for ultra-low volatility organic compounds. This indicates that the oil is an efficient nucleation agent. Our results demonstrate that jet oil nucleation is an important mechanism that can explain the abundant observations of high number concentrations of non-refractory ultrafine particles near airports.