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- 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.
- ItemMeteorological conditions during the ACLOUD/PASCAL field campaign near Svalbard in early summer 2017(Katlenburg-Lindau : EGU, 2018) Knudsen, Erlend M.; Heinold, Bernd; Dahlke, Sandro; Bozem, Heiko; Crewell, Susanne; Gorodetskaya, Irina V.; Heygster, Georg; Kunkel, Daniel; Maturilli, Marion; Mech, Mario; Viceto, Carolina; Rinke, Annette; Schmithüsen, Holger; Ehrlich, André; Macke, Andreas; Lüpkes, Christof; Wendisch, ManfredThe two concerted field campaigns, Arctic CLoud Observations Using airborne measurements during polar Day (ACLOUD) and the Physical feedbacks of Arctic planetary boundary level Sea ice, Cloud and AerosoL (PASCAL), took place near Svalbard from 23 May to 26 June 2017. They were focused on studying Arctic mixed-phase clouds and involved observations from two airplanes (ACLOUD), an icebreaker (PASCAL) and a tethered balloon, as well as ground-based stations. Here, we present the synoptic development during the
- ItemSimultaneous observations of NLCs and MSEs at midlatitudes: Implications for formation and advection of ice particles(Göttingen : Copernicus GmbH, 2018) Gerding, M.; Zöllner, J.; Zecha, M.; Baumgarten, K.; Höffner, J.; Stober, G.; Lübken, F.-J.We combined ground-based lidar observations of noctilucent clouds (NLCs) with collocated, simultaneous radar observations of mesospheric summer echoes (MSEs) in order to compare ice cloud altitudes at a midlatitude site (Kühlungsborn, Germany, 54° N, 12° E). Lidar observations are limited to larger particles ( > 10 nm), while radars are also sensitive to small particles ( < 10 nm), but require sufficient ionization and turbulence at the ice cloud altitudes. The combined lidar and radar data set thus includes some information on the size distribution within the cloud and through this on the of the cloud. The soundings for this study are carried out by the IAP Rayleigh-Mie-Raman (RMR) lidar and the OSWIN VHF radar. On average, there is no difference between the lower edges (lowNLC and lowMSE). The mean difference of the upper edges upNLC and upMSE is g1/4 500 m, which is much less than expected from observations at higher latitudes. In contrast to high latitudes, the MSEs above our location typically do not reach much higher than the NLCs. In addition to earlier studies from our site, this gives additional evidence for the supposition that clouds containing large enough particles to be observed by lidar are not formed locally but are advected from higher latitudes. During the advection process, the smaller particles in the upper part of the cloud either grow and sediment, or they sublimate. Both processes result in a thinning of the layer. High-altitude MSEs, usually indicating nucleation of ice particles, are rarely observed in conjunction with lidar observations of NLCs at Kühlungsborn. © Author(s) 2018.