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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
- ItemGlobal observations of 2 day wave coupling to the diurnal tide in a high‐altitude forecast‐assimilation system(Hoboken, NJ : Wiley, 2017-4-18) Lieberman, R.S.; Riggin, D.M.; Nguyen, V.; Palo, S.E.; Siskind, D.E.; Mitchell, N.J.; Stober, G.; Wilhelm, S.; Livesey, N.J.We examine wave components in a high-altitude forecast-assimilation system that arise from nonlinear interaction between the diurnal tide and the westward traveling quasi 2 day wave. The process yields a westward traveling “sum” wave with zonal wave number 4 and a period of 16 h, and an eastward traveling “difference” wave with zonal wave number 2 and a period of 2 days. While the eastward 2 day wave has been reported in satellite temperatures, the westward 16 h wave lies outside the Nyquist limits of resolution of twice daily local time satellite sampling. Hourly output from a high-altitude forecast-assimilation model is used to diagnose the nonlinear quadriad. A steady state primitive equation model forced by tide-2 day wave advection is used to intepret the nonlinear wave products. The westward 16 h wave maximizes in the midlatitude winter mesosphere and behaves like an inertia-gravity wave. The nonlinearly generated component of the eastward 2 day wave maximizes at high latitudes in the lower thermosphere, and only weakly penetrates to low latitudes. The 16 h and the eastward 2 day waves are of comparable amplitude and alias to the same apparent frequency when viewed from a satellite perspective.
- 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.
- ItemOn statistics of the free-troposphere synoptic component: An evaluation of skewnesses and mixed third-order moments contribution to the synoptic-scale dynamics and fluxes of heat and humidity(Abingdon : Taylor and Francis Ltd., 2008) Petoukhov, V.; Eliseev, A.V.; Klein, R.; Oesterle, H.Based on the ERA40 data for 1976-2002 we calculated skewnesses and mixed third-order statistical moments (TOMs) for the synoptic variations [with (2.5-6) d timescales]of horizontal winds, temperature, vertical velocity and the specific humidity in Eulerian coordinates. All these variables show skewnesses which markedly deviate from zero, basically at the entries and the outlets of the mid-latitude storm tracks. In these regions, high values of skewness for vertical velocity, temperature and the specific humidity are revealed throughout the entire free troposphere, while the marked skewnesses for horizontal winds are traced in the lower free troposphere. We found a notable deviation of the synoptic-component statistics from the Gaussian statistics. We also made an estimate of the contribution from TOMs to the prognostic equations for the synoptic-scale kinetic energy and the meridional fluxes of sensible and latent heat, which appeared to be non-negligible, mainly in the storm tracks in winter. Our analysis attests that the most pronounced contribution of TOMs to the aforementioned equations comes from the self-advection by the horizontal synoptic-scale motions, while the TOMs induced by the metric terms in the original equations, and specifically the TOMs associated with the vertical self-advection by the synoptic-scale motions, are much less important.