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- ItemModel studies of short-term variations induced in trace gases by particle precipitation in the mesosphere and lower thermosphere(Hoboken, NJ : Wiley, 2016) Fytterer, T.; Bender, S.; Berger, U.; Nieder, H.; Sinnhuber, M.; Wissing, J.M.The 3-D global chemistry and transport model (3dCTM) was used to investigate NO, OH, and O3 from January 2002 to May 2010 between 60 km and 133 km. Their daytime and nighttime mean zonal means (55°–75° geomagnetic latitude) were analyzed with respect to short-term variations associated with particle precipitation. The corresponding ionization rates were derived from the 3-D atmospheric ionization module Osnabrück (AIMOS), which is based on particle flux measurements. The trace gas variations with respect to their background were investigated by using a superposed epoch analysis. The 27 day signature associated with particle precipitation is found in NO, while it is only indicated in OH and O3 during winter. A varying solar spectrum associated with the 11 year solar cycle causes modifications of this signal up to 10%, while the main patterns are conserved. Published observations show a clear 27 day signal, qualitatively agreeing with the model results at altitudes >70 km except for O3 in Northern Hemisphere winter. Further differences occur with respect to the magnitude of the trace gas variations, primarily attributed to the different trace gas background and dynamical variations of the background atmosphere. Absolute OH variations are overestimated by the 3dCTM during winter, while the opposite is true for O3. These differences might originate from an unknown offset in AIMOS, incorrect chemical reaction rates, a different background of H2O and O3, and the model dynamics. However, their nonlinear relationship and their altitude of largest response are qualitatively captured in Southern Hemisphere winter.
- ItemThe Effect of Obliquity-Driven Changes on Paleoclimate Sensitivity During the Late Pleistocene(Hoboken, NJ : Wiley, 2018) Köhler, Peter; Knorr, Gregor; Stap, Lennert B.; Ganopolski, Andrey; de Boer, Bas; van de Wal, Roderik S. W.; Barker, Stephen; Rüpke, Lars H.We reanalyze existing paleodata of global mean surface temperature ΔTg and radiative forcing ΔR of CO2 and land ice albedo for the last 800,000 years to show that a state-dependency in paleoclimate sensitivity S, as previously suggested, is only found if ΔTg is based on reconstructions, and not when ΔTg is based on model simulations. Furthermore, during times of decreasing obliquity (periods of land ice sheet growth and sea level fall) the multimillennial component of reconstructed ΔTg diverges from CO2, while in simulations both variables vary more synchronously, suggesting that the differences during these times are due to relatively low rates of simulated land ice growth and associated cooling. To produce a reconstruction-based extrapolation of S for the future, we exclude intervals with strong ΔTg-CO2 divergence and find that S is less state-dependent, or even constant state-independent), yielding a mean equilibrium warming of 2–4 K for a doubling of CO2.
- ItemEffect of dimethylamine on the gas phase sulfuric acid concentration measured by Chemical Ionization Mass Spectrometry(Hoboken, NJ : Wiley, 2016) Rondo, L.; Ehrhart, S.; Kürten, A.; Adamov, A.; Bianchi, F.; Breitenlechner, M.; Duplissy, J.; Franchin, A.; Dommen, J.; Donahue, Neil M.; Dunne, E.M.; Flagan, R.C.; Hakala, J.; Hansel, A.; Keskinen, H.; Kim, J.; Jokinen, T.; Lehtipalo, K.; Leiminger, M.; Praplan, A.; Riccobono, F.; Rissanen, M.P.; Sarnela, N.; Schobesberger, S.; Simon, M.; Sipilä, M.; Smith, J.N.; Tomé, A.; Tröstl, J.; Tsagkogeorgas, G.; Vaattovaara, P.; Winkler, P.M.; Williamson, C.; Wimmer, D.; Baltensperger, U.; Kirkby, J.; Kulmala, M.; Petäjä, T.; Worsnop, D.R.; Curtius, J.Sulfuric acid is widely recognized as a very important substance driving atmospheric aerosol nucleation. Based on quantum chemical calculations it has been suggested that the quantitative detection of gas phase sulfuric acid (H2SO4) by use of Chemical Ionization Mass Spectrometry (CIMS) could be biased in the presence of gas phase amines such as dimethylamine (DMA). An experiment (CLOUD7 campaign) was set up at the CLOUD (Cosmics Leaving OUtdoor Droplets) chamber to investigate the quantitative detection of H2SO4 in the presence of dimethylamine by CIMS at atmospherically relevant concentrations. For the first time in the CLOUD experiment, the monomer sulfuric acid concentration was measured by a CIMS and by two CI-APi-TOF (Chemical Ionization-Atmospheric Pressure interface-Time Of Flight) mass spectrometers. In addition, neutral sulfuric acid clusters were measured with the CI-APi-TOFs. The CLOUD7 measurements show that in the presence of dimethylamine (<5 to 70 pptv) the sulfuric acid monomer measured by the CIMS represents only a fraction of the total H2SO4, contained in the monomer and the clusters that is available for particle growth. Although it was found that the addition of dimethylamine dramatically changes the H2SO4 cluster distribution compared to binary (H2SO4-H2O) conditions, the CIMS detection efficiency does not seem to depend substantially on whether an individual H2SO4 monomer is clustered with a DMA molecule. The experimental observations are supported by numerical simulations based on A Self-contained Atmospheric chemistry coDe coupled with a molecular process model (Sulfuric Acid Water NUCleation) operated in the kinetic limit.
- ItemTracking the Saharan Air Layer with shipborne lidar across the tropical Atlantic(Hoboken, NJ : Wiley, 2014) Kanitz, T.; Engelmann, R.; Heinold, B.; Baars, H.; Skupin, A.; Ansmann, A.Saharan dust was observed with shipborne lidar from 60° to 20°W along 14.5°N during a 1-month transatlantic cruise of the research vessel Meteor. About 4500 km off the coast of Africa, mean extinction and backscatter-related Ångström exponent of 0.1, wavelength-independent extinction-to-backscatter ratios (lidar ratios) of around 45 sr, and particle linear depolarization ratio of 20% were found for aged dust (transport time >10 days). In contrast, dust with a shorter atmospheric residence time of 2–3 days showed Ångström exponents of −0.5 (backscatter coefficient) and 0.1 (extinction coefficient), mean lidar ratios of 64 and 50 sr, and particle linear depolarization ratios of 22 and 26% at 355 and 532 nm wavelength, respectively. Traces of fire smoke were also detected in the observed dust layers. The lidar observations were complemented by Aerosol Robotic Network handheld Sun photometer measurements, which revealed a mean total atmospheric column aerosol optical thickness of 0.05 for pure marine conditions (in the absence of lofted aerosol layers) and roughly 0.9 during a strong Saharan dust outbreak. The achieved data set was compared with first Consortium for Small Scale Modeling-Multi-Scale Chemistry Aerosol Transport simulations. The simulated vertical aerosol distribution showed good agreement with the lidar observations.
- ItemPMC Turbo : Studying Gravity Wave and Instability Dynamics in the Summer Mesosphere Using Polar Mesospheric Cloud Imaging and Profiling From a Stratospheric Balloon(Hoboken, NJ : Wiley, 2019) Fritts, David C.; Miller, Amber D.; Kjellstrand, C. Bjorn; Geach, Christopher; Williams, Bifford P.; Kaifler, Bernd; Kaifler, Natalie; Jones, Glenn; Rapp, Markus; Limon, Michele; Reimuller, Jason; Wang, Ling; Hanany, Shaul; Gisinger, Sonja; Zhao, Yucheng; Stober, Gunter; Randall, Cora E.The Polar Mesospheric Cloud Turbulence (PMC Turbo) experiment was designed to observe and quantify the dynamics of small-scale gravity waves (GWs) and instabilities leading to turbulence in the upper mesosphere during polar summer using instruments aboard a stratospheric balloon. The PMC Turbo scientific payload comprised seven high-resolution cameras and a Rayleigh lidar. Overlapping wide and narrow camera field of views from the balloon altitude of ~38 km enabled resolution of features extending from ~20 m to ~100 km at the PMC layer altitude of ~82 km. The Rayleigh lidar provided profiles of temperature below the PMC altitudes and of the PMCs throughout the flight. PMCs were imaged during an ~5.9-day flight from Esrange, Sweden, to Northern Canada in July 2018. These data reveal sensitivity of the PMCs and the dynamics driving their structure and variability to tropospheric weather and larger-scale GWs and tides at the PMC altitudes. Initial results reveal strong modulation of PMC presence and brightness by larger-scale waves, significant variability in the occurrence of GWs and instability dynamics on time scales of hours, and a diversity of small-scale dynamics leading to instabilities and turbulence at smaller scales. At multiple times, the overall field of view was dominated by extensive and nearly continuous GWs and instabilities at horizontal scales from ~2 to 100 km, suggesting sustained turbulence generation and persistence. At other times, GWs were less pronounced and instabilities were localized and/or weaker, but not absent. An overview of the PMC Turbo experiment motivations, scientific goals, and initial results is presented here. © 2019. The Authors.
- ItemA study of the dissociative recombination of CaO+ with electrons: Implications for Ca chemistry in the upper atmosphere(Hoboken, NJ : Wiley, 2016) Bones, D.L.; Gerding, M.; Höffner, J.; Gómez Martín, Juan Carlos; Plane, J.M.C.The dissociative recombination of CaO+ ions with electrons has been studied in a flowing afterglow reactor. CaO+ was generated by the pulsed laser ablation of a Ca target, followed by entrainment in an Ar+ ion/electron plasma. A kinetic model describing the gas-phase chemistry and diffusion to the reactor walls was fitted to the experimental data, yielding a rate coefficient of (3.0 ± 1.0) × 10−7 cm3 molecule−1 s−1 at 295 K. This result has two atmospheric implications. First, the surprising observation that the Ca+/Fe+ ratio is ~8 times larger than Ca/Fe between 90 and 100 km in the atmosphere can now be explained quantitatively by the known ion-molecule chemistry of these two metals. Second, the rate of neutralization of Ca+ ions in a descending sporadic E layer is fast enough to explain the often explosive growth of sporadic neutral Ca layers.
- ItemMarine nanogels as a source of atmospheric nanoparticles in the high Arctic(Hoboken, NJ : Wiley, 2013) Karl, Matthias; Leck, Caroline; Coz, Esther; Heintzenberg, JostThe high Arctic (north of 80°N) in summer is a region characterized by clean air and low abundances of preexisting particles. Marine colloidal nanogels i.e., assembled dissolved organic carbohydrate polymer networks have recently been confirmed to be present in both airborne particles and cloud water over the Arctic pack ice area. A novel route to atmospheric nanoparticles that appears to be operative in the high Arctic is suggested. It involves the injection of marine granular nanogels into the air from evaporating fog and cloud droplets, and is supported by observational and theoretical evidence obtained from a case study. Statistical analysis of the aerosol size distribution data recorded in the years 1991, 1996, 2001, and 2008 classified 75 nanoparticle events - covering 17% of the observed time period - as nanogel-type events, characterized by the spontaneous appearance of several distinct size bands below 200 nm diameter.
- ItemView angle dependence of MODIS liquid water path retrievals in warm oceanic clouds(Hoboken, NJ : Wiley, 2014) Horváth, Ákos; Seethala, Chellappan; Deneke, HartwigWe investigated the view angle dependence of domain mean Moderate Resolution Imaging Spectroradiometer (MODIS) liquid water path (LWP) and that of corresponding cloud optical thickness, effective radius, and liquid cloud fraction as proxy for plane-parallel retrieval biases. Independent Advanced Microwave Scanning Radiometer–EOS LWP was used to corroborate that the observed variations with sun-view geometry were not severely affected by seasonal/latitudinal changes in cloud properties. Microwave retrievals showed generally small (<10%) cross-swath variations. The view angle (cross-swath) dependence of MODIS optical thickness was weaker in backscatter than forward scatter directions and transitioned from mild ∩ shape to stronger ∪ shape as heterogeneity, sun angle, or latitude increased. The 2.2 µm effective radius variations always had a ∪ shape, which became pronounced and asymmetric toward forward scatter in the most heterogeneous clouds and/or at the lowest sun. Cloud fraction had the strongest and always ∪-shaped view angle dependence. As a result, in-cloud MODIS cloud liquid water path (CLWP) showed surprisingly good view angle (cross-swath) consistency, usually comparable to that of microwave retrievals, due to cancelation between optical thickness and effective radius biases. Larger (20–40%) nadir-relative increases were observed in the most extreme heterogeneity and sun angle bins, that is, typically in the polar regions, which, however, constituted only 3–8% of retrievals. The good consistency of MODIS in-cloud CLWP was lost for gridbox mean LWP, which was dominated by the strong cloud fraction increase with view angle. More worryingly, MODIS LWP exhibited significant and systematic absolute increases with heterogeneity and sun angle that is not present in microwave LWP.
- ItemLong‐Term Changes in the Northern Midwinter Middle Atmosphere in Relation to the Quasi‐Biennial Oscillation(Hoboken, NJ : Wiley, 2019) Gabriel, A.Long-term changes in the middle atmosphere due to anthropogenic greenhouse gas emissions are examined in relation to the effect of the equatorial Quasi-Biennial Oscillation (QBO) on the northern midwinter circulation. The examinations are based on the Coupled Model Intercomparison Project Phase 5 simulations for 1979–2100 with the Earth-System-Model MPI-ESM-MR that generates the QBO internally. In particular, the three-dimensional residual circulation is used as proxy for the Brewer-Dobson circulation, revealing an increasing downwelling in the center of the polar low over Northern Europe/Siberia (~5% per decade). The changes in northern midwinter temperature, zonal wind, and residual circulation are much stronger during westerly (QBO-W) than easterly (QBO-E) phase of QBO (e.g., for a moderate increase in greenhouse gases, we find maximum decreases in the zonal mean westerly jet at 60°N and 3 hPa of about −14.8 ± 5.4 m/s for QBO-W but only −4.7 ± 5.2 m/s for QBO-E). This is due to a change of the extratropical QBO-W signature toward QBO-E signature while the equatorial QBO remains nearly unchanged (i.e., a change toward disappearance of the so-called Holton-Tan relationship). Similar to the current change from QBO-W to QBO-E signature, the changes during QBO-W include an increase in amplitude and eastward shift in phase of stratospheric stationary Wave 1 at the cost of Wave 2, with decreasing westerlies over North America and increasing downwelling over Siberia. The eastward shift in phase of stationary Wave 1 is related to the associated increase in meridional transport of planetary vorticity. © 2019. The Authors.
- 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.