93 results
Search Results
Now showing 1 - 10 of 93
- 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. - ItemCharacterization of organic aerosol across the global remote troposphere: A comparison of ATom measurements and global chemistry models(Katlenburg-Lindau : EGU, 2020) Hodzic, Alma; Campuzano-Jost, Pedro; Bian, Huisheng; Chin, Mian; Colarco, Peter R.; Day, Douglas A.; Froyd, Karl D.; Heinold, Bernd; Katich, Joseph M.; Jo, Duseong S.; Kodros, John K.; Nault, Benjamin A.; Pierce, Jeffrey R.; Ray, Eric; Schacht, Jacob; Schill, Gregory P.; Schroder, Jason C.; Schwarz, Joshua P.; Sueper, Donna T.; Tegen, Ina; Tilmes, Simone; Tsigaridis, Kostas; Yu, Pengfei; Jimenez, Jose L.The spatial distribution and properties of submicron organic aerosol (OA) are among the key sources of uncertainty in our understanding of aerosol effects on climate. Uncertainties are particularly large over remote regions of the free troposphere and Southern Ocean, where very few data have been available and where OA predictions from AeroCom Phase II global models span 2 to 3 orders of magnitude, greatly exceeding the model spread over source regions. The (nearly) pole-to-pole vertical distribution of nonrefractory aerosols was measured with an aerosol mass spectrometer onboard the NASA DC-8 aircraft as part of the Atmospheric Tomography (ATom) mission during the Northern Hemisphere summer (August 2016) and winter (February 2017). This study presents the first extensive characterization of OA mass concentrations and their level of oxidation in the remote atmosphere. OA and sulfate are the major contributors by mass to submicron aerosols in the remote troposphere, together with sea salt in the marine boundary layer. Sulfate was dominant in the lower stratosphere. OA concentrations have a strong seasonal and zonal variability, with the highest levels measured in the lower troposphere in the summer and over the regions influenced by biomass burning from Africa (up to 10 μgsm-3). Lower concentrations (~ 0:1 0.3 μgsm-3) are observed in the northern middle and high latitudes and very low concentrations (< 0:1 μgsm-3) in the southern middle and high latitudes. The ATom dataset is used to evaluate predictions of eight current global chemistry models that implement a variety of commonly used representations of OA sources and chemistry, as well as of the AeroCom-II ensemble. The current model ensemble captures the average vertical and spatial distribution of measured OA concentrations, and the spread of the individual models remains within a factor of 5. These results are significantly improved over the AeroCom-II model ensemble, which shows large overestimations over these regions. However, some of the improved agreement with observations occurs for the wrong reasons, as models have the tendency to greatly overestimate the primary OA fraction and underestimate the sec-ondary fraction. Measured OA in the remote free troposphere is highly oxygenated, with organic aerosol to organic carbon (OA= OC) ratios of ~ 2.2 2.8, and is 30 % 60% more oxygenated than in current models, which can lead to significant errors in OA concentrations. The model measurement comparisons presented here support the concept of a more dynamic OA system as proposed by Hodzic et al. (2016), with enhanced removal of primary OA and a stronger production of secondary OA in global models needed to provide better agreement with observations. © 2020 IEEE Computer Society. All rights reserved.
- ItemNew particle formation and sub-10nm size distribution measurements during the A-LIFE field experiment in Paphos, Cyprus(Katlenburg-Lindau : EGU, 2020) Brilke, Sophia; Fölker, Nikolaus; Kandler, Konrad; Müller, Thomas; Gong, Xianda; Peischl, Jeff; Weinzierl, Bernadett; Winkler, Paul M.Atmospheric particle size distributions were measured in Paphos, Cyprus, during the A-LIFE (absorbing aerosol layers in a changing climate: ageing, lifetime and dynamics) field experiment from 3 to 30 April 2017. The newly developed differential mobility analyser train (DMAtrain) was deployed for the first time in an atmospheric environment for the direct measurement of the nucleation mode size range between 1.8 and 10 nm diameter. The DMA-train set-up consists of seven size channels, of which five are set to fixed particle mobility diameters and two additional diameters are obtained by alternating voltage settings in one DMA every 10 s. In combination with a conventional mobility particle size spectrometer (MPSS) and an aerodynamic particle sizer (APS) the complete atmospheric aerosol size distribution from 1.8 nm to 10 μ m was covered. The focus of the A-LIFE study was to characterize new particle formation (NPF) in the eastern Mediterranean region at a measurement site with strong local pollution sources. The nearby Paphos airport was found to be a large emission source for nucleation mode particles, and we analysed the size distribution of the airport emission plumes at approximately 500 m from the main runway. The analysis yielded nine NPF events in 27 measurement days from the combined analysis of the DMAtrain, MPSS and trace gas monitors. Growth rate calculations were performed, and a size dependency of the initial growth rate (< 10 nm) was observed for one event case. Fast changes of the sub-10 nm size distribution on a timescale of a few minutes were captured by the DMA-train measurement during early particle growth and are discussed in a second event case. In two cases, particle formation and growth were detected in the nucleation mode size range which did not exceed the 10 nm threshold. This finding implies that NPF likely occurs more frequently than estimated from studies where the lower nanometre size regime is not covered by the size distribution measurements. © 2020 Author(s).
- ItemA new model of meteoric calcium in the mesosphere and lower thermosphere(Katlenburg-Lindau : EGU, 2018-10-16) Plane, John M. C.; Feng, Wuhu; Gómez Martín, Juan Carlos; Gerding, Michael; Raizada, ShikhaMeteoric ablation produces layers of metal atoms in the mesosphere and lower thermosphere (MLT). It has been known for more than 30 years that the Ca atom layer is depleted by over 2 orders of magnitude compared with Na, despite these elements having nearly the same elemental abundance in chondritic meteorites. In contrast, the Ca+ ion abundance is depleted by less than a factor of 10. To explain these observations, a large database of neutral and ion–molecule reaction kinetics of Ca species, measured over the past decade, was incorporated into the Whole Atmosphere Community Climate Model (WACCM). A new meteoric input function for Ca and Na, derived using a chemical ablation model that has been tested experimentally with a Meteoric Ablation Simulator, shows that Ca ablates almost 1 order of magnitude less efficiently than Na. WACCM-Ca simulates the seasonal Ca layer satisfactorily when compared with lidar observations, but tends to overestimate Ca+ measurements made by rocket mass spectrometry and lidar. A key finding is that CaOH and CaCO3 are very stable reservoir species because they are involved in essentially closed reaction cycles with O2 and O. This has been demonstrated experimentally for CaOH, and in this study for CaCO3 using electronic structure and statistical rate theory. Most of the neutral Ca is therefore locked in these reservoirs, enabling rapid loss through polymerization into meteoric smoke particles, and this explains the extreme depletion of Ca.
- ItemIce-nucleating particle concentrations unaffected by urban air pollution in Beijing, China(Katlenburg-Lindau : EGU, 2018) Chen, Jie; Wu, Zhijun; Augustin-Bauditz, Stefanie; Grawe, Sarah; Hartmann, Markus; Pei, Xiangyu; Liu, Zirui; Ji, Dongsheng; Wex, HeikeExceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (NINP) in the range from -6 to -25 °C in Beijing. No correlations between NINP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between NINP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
- ItemA comprehensive characterization of ice nucleation by three different types of cellulose particles immersed in water(Katlenburg-Lindau : EGU, 2019) Hiranuma, Naruki; Adachi, Kouji; Bell, David M.; Belosi, Franco; Beydoun, Hassan; Bhaduri, Bhaskar; Bingemer, Heinz; Budke, Carsten; Clemen, Hans-Christian; Conen, Franz; Cory, Kimberly M.; Curtius, Joachim; DeMott, Paul J.; Eppers, Oliver; Grawe, Sarah; Hartmann, Susan; Hoffmann, Nadine; Höhler, Kristina; Jantsch, Evelyn; Kiselev, Alexei; Koop, Thomas; Kulkarni, Gourihar; Mayer, Amelie; Murakami, Masataka; Murray, Benjamin J.; Nicosia, Alessia; Petters, Markus D.; Piazza, Matteo; Polen, Michael; Reicher, Naama; Rudich, Yinon; Saito, Atsushi; Santachiara, Gianni; Schiebel, Thea; Schill, Gregg P.; Schneider, Johannes; Segev, Lior; Stopelli, Emiliano; Sullivan, Ryan C.; Suski, Kaitlyn; Szakáll, Miklós; Tajiri, Takuya; Taylor, Hans; Tobo, Yutaka; Ullrich, Romy; Weber, Daniel; Wex, Heike; Whale, Thomas F.; Whiteside, Craig L.; Yamashita, Katsuya; Zelenyuk, Alla; Möhler, OttmarWe present the laboratory results of immersion freezing efficiencies of cellulose particles at supercooled temperature (T) conditions. Three types of chemically homogeneous cellulose samples are used as surrogates that represent supermicron and submicron ice-nucleating plant structural polymers. These samples include microcrystalline cellulose (MCC), fibrous cellulose (FC) and nanocrystalline cellulose (NCC). Our immersion freezing dataset includes data from various ice nucleation measurement techniques available at 17 different institutions, including nine dry dispersion and 11 aqueous suspension techniques. With a total of 20 methods, we performed systematic accuracy and precision analysis of measurements from all 20 measurement techniques by evaluating T-binned (1 ∘C) data over a wide T range (−36 ∘C
- ItemTurbulence-induced cloud voids: Observation and interpretation(Katlenburg-Lindau : EGU, 2019) Karpińska, Katarzyna; Bodenschatz, Jonathan F.E.; Malinowski, Szymon P.; Nowak, Jakub L.; Risius, Steffen; Schmeissner, Tina; Shaw, Raymond A.; Siebert, Holger; Xi, Hengdong; Xu, Haitao; Bodenschatz, EberhardThe phenomenon of "cloud voids", i.e., elongated volumes inside a cloud that are devoid of droplets, was observed with laser sheet photography in clouds at a mountain-top station. Two experimental cases, similar in turbulence conditions yet with diverse droplet size distributions and cloud void prevalence, are reported. A theoretical explanation is proposed based on the study of heavy inertial sedimenting particles inside a Burgers vortex. A general conclusion regarding void appearance is drawn from theoretical analysis. Numerical simulations of polydisperse droplet motion with realistic vortex parameters and Mie scattering visual effects accounted for can explain the presence of voids with sizes similar to that of the observed ones. Clustering and segregation effects in a vortex tube are discussed for reasonable cloud conditions. © Author(s) 2019.
- ItemMultiphase MCM-CAPRAM modeling of the formation and processing of secondary aerosol constituents observed during the Mt. Tai summer campaign in 2014(Katlenburg-Lindau : EGU, 2020) Zhu, Yanhong; Tilgner, Andreas; Hoffmann, Erik Hans; Herrmann, Hartmut; Kawamura, Kimitaka; Yang, Lingxiao; Xue, Likun; Wang, WenxingDespite the high abundance of secondary aerosols in the atmosphere, their formation mechanisms remain poorly understood. In this study, the Master Chemical Mechanism (MCM) and the Chemical Aqueous-Phase Radical Mechanism (CAPRAM) are used to investigate the multiphase formation and processing of secondary aerosol constituents during the advection of air masses towards the measurement site of Mt. Tai in northern China. Trajectories with and without chemical–cloud interaction are modeled. Modeled radical and non-radical concentrations demonstrate that the summit of Mt. Tai, with an altitude of ∼1.5 km a.m.s.l., is characterized by a suburban oxidants budget. The modeled maximum gas-phase concentrations of the OH radical are 3.2×106 and 3.5×106 molec. cm−3 in simulations with and without cloud passages in the air parcel, respectively. In contrast with previous studies at Mt. Tai, this study has modeled chemical formation processes of secondary aerosol constituents under day vs. night and cloud vs. non-cloud cases along the trajectories towards Mt. Tai in detail. The model studies show that sulfate is mainly produced in simulations where the air parcel is influenced by cloud chemistry. Under the simulated conditions, the aqueous reaction of HSO−3 with H2O2 is the major contributor to sulfate formation, contributing 67 % and 60 % in the simulations with cloud and non-cloud passages, respectively. The modeled nitrate formation is higher at nighttime than during daytime. The major pathway is aqueous-phase N2O5 hydrolysis, with a contribution of 72 % when cloud passages are considered and 70 % when they are not. Secondary organic aerosol (SOA) compounds, e.g., glyoxylic, oxalic, pyruvic and malonic acid, are found to be mostly produced from the aqueous oxidations of hydrated glyoxal, hydrated glyoxylic acid, nitro-2-oxopropanoate and hydrated 3-oxopropanoic acid, respectively. Sensitivity studies reveal that gaseous volatile organic compound (VOC) emissions have a huge impact on the concentrations of modeled secondary aerosol compounds. Increasing the VOC emissions by a factor of 2 leads to linearly increased concentrations of the corresponding SOA compounds. Studies using the relative incremental reactivity (RIR) method have identified isoprene, 1,3-butadiene and toluene as the key precursors for glyoxylic and oxalic acid, but only isoprene is found to be a key precursor for pyruvic acid. Additionally, the model investigations demonstrate that an increased aerosol partitioning of glyoxal can play an important role in the aqueous-phase formation of glyoxylic and oxalic acid. Overall, the present study is the first that provides more detailed insights in the formation pathways of secondary aerosol constituents at Mt. Tai and clearly emphasizes the importance of aqueous-phase chemical processes on the production of multifunctional carboxylic acids.
- ItemSolar 27-day signatures in standard phase height measurements above central Europe(Katlenburg-Lindau : EGU, 2019) von Savigny, Christian; Peters, Dieter H.W.; Entzian, GünterWe report on the effect of solar variability at the 27-day and the 11-year timescales on standard phase heightmeasurements in the ionospheric D region carried out in cen-tral Europe. Standard phase height corresponds to the re-flection height of radio waves (for constant solar zenith dis-tance) in the ionosphere near 80 km altitude, where NO isionized by solar Lyman-αradiation. Using the superposedepoch analysis (SEA) method, we extract statistically highlysignificant solar 27-day signatures in standard phase heights.The 27-day signatures are roughly inversely correlated to so-lar proxies, such as the F10.7 cm radio flux or the Lyman-αflux. The sensitivity of standard phase height change to so-lar forcing at the 27-day timescale is found to be in goodagreement with the sensitivity for the 11-year solar cycle,suggesting similar underlying mechanisms. The amplitude ofthe 27-day signature in standard phase height is larger duringsolar minimum than during solar maximum, indicating thatthe signature is not only driven by photoionization of NO. Weidentified statistical evidence for an influence of ultra-longplanetary waves on the quasi 27-day signature of standardphase height in winters of solar minimum periods.
- ItemShip-based measurements of ice nuclei concentrations over the Arctic, Atlantic, Pacific and Southern oceans(Katlenburg-Lindau : EGU, 2020) Welti, André; Bigg, Keith E.; DeMott, Paul J.; Gong, Xianda; Hartmann, Markus; Harvey, Mike; Henning, Silvia; Herenz, Paul; Hill, Thomas C.J.; Hornblow, Blake; Leck, Caroline; Löffler, Mareike; McCluskey, Christina S.; Rauker, Anne Marie; Schmale, Julia; Tatzelt, Christian; van Pinxteren, Manuela; Stratmann, FrankAmbient concentrations of ice-forming particles measured during ship expeditions are collected and summarised with the aim of determining the spatial distribution and variability in ice nuclei in oceanic regions. The presented data from literature and previously unpublished data from over 23 months of ship-based measurements stretch from the Arctic to the Southern Ocean and include a circumnavigation of Antarctica. In comparison to continental observations, ship-based measurements of ambient ice nuclei show 1 to 2 orders of magnitude lower mean concentrations. To quantify the geographical variability in oceanic areas, the concentration range of potential ice nuclei in different climate zones is analysed by meridionally dividing the expedition tracks into tropical, temperate and polar climate zones. We find that concentrations of ice nuclei in these meridional zones follow temperature spectra with similar slopes but vary in absolute concentration. Typically, the frequency with which specific concentrations of ice nuclei are observed at a certain temperature follows a log-normal distribution. A consequence of the log-normal distribution is that the mean concentration is higher than the most frequently measured concentration. Finally, the potential contribution of ship exhaust to the measured ice nuclei concentration on board research vessels is analysed as function of temperature. We find a sharp onset of the influence at approximately 36 C but none at warmer temperatures that could bias ship-based measurements. © Author(s) 2020. This work is distributed under the Creative Commons Attribution 4.0 License.