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Systematic observations of banner clouds at Mount Zugspitze in the Bavarian Alps are presented and discussed. One set of observations draws on daily time lapse movies, which were taken over several years at this mountain. Identifying banner clouds with the help of these movies and using simultaneous observations of standard variables at the summit of the mountain provides climatological information regarding the banner clouds. In addition, a week-long measurement campaign with an entire suite of instruments was carried through yielding a comprehensive set of data for two specific banner cloud events. <br></br> The duration of banner cloud events has a long-tailed distribution with a mean of about 40 min. The probability of occurrence has both a distinct diurnal and a distinct seasonal cycle, with a maximum in the afternoon and in the warm season, respectively. These cycles appear to correspond closely to analogous cycles of relative humidity, which maximize in the late afternoon and during the warm season. In addition, the dependence of banner cloud occurrence on wind speed is weak. Both results suggest that moisture conditions are a key factor for banner cloud occurrence. The distribution of wind direction during banner cloud events slightly deviates from climatology, suggesting an influence from the specific Zugspitz orography. <br></br> The two banner cloud events during the campaign have a number of common features: the windward and the leeward side are characterized by different wind regimes, however, with mean upward flow on both sides; the leeward air is both moister and warmer than the windward air; the background atmosphere has an inversion just above the summit of Mt. Zugspitze; the lifting condensation level increases with altitude. The results are discussed, and it is argued that they are consistent with previous Large Eddy Simulations using idealized orography.
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Measurements of atmospheric ions in the size range 0.8–42 nm were conducted at the environmental research station of the University of Crete at Finokalia from April 2008 to April 2009 in the frame of the EUCAARI project. Both positive and negative atmospheric ions were found to have a clear annual cycle, with minimum concentrations in summer. Their concentrations were found to vary with the prevailing meteorology and the abundance of aerosol particles in the atmosphere. High concentrations of ions were observed during new particle formation events. There were 53 nucleation events recorded. It was found that under certain atmospheric conditions enhanced ion concentrations can be observed during night. Overall, 39 night-time events were observed, all of them observed for the negatively charged particles while only 21 were observed for the positively charged particles. Night-time enhanced ion concentrations were more frequent during spring and autumn and no such events were recorded from July to September. A strong anti-correlation was found between air ion concentrations, especially at cluster sizes (1.25–1.66 nm), and condensation and coagulation sinks. Enhanced ion concentrations at night were found to be more frequent when air masses had traveled over the island of Crete, indicating possible association with local biogenic sources.
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Long term measurements in background air (Cape Grim, Tasmania) and firn air (NEEM, Greenland) of the potent long-lived greenhouse gas SF<sub>5</sub>CF<sub>3</sub> show that emissions declined after the late 1990s, having grown since the 1950s, and became indistinguishable from zero after 2003. The timing of this decline suggests that emissions of this gas may have been related to the production of certain fluorochemicals; production of which have been recently phased out. An earlier observation of closely correlated atmospheric abundances of SF<sub>5</sub>CF<sub>3</sub> and SF<sub>6</sub> are shown here to have likely been purely coincidental, as their respective trends diverged after 2002. Due to its long lifetime (ca. 900 yr), atmospheric concentrations of SF<sub>5</sub>CF<sub>3</sub> have not declined, and it is now well mixed between hemispheres, as is also shown here from interhemispheric aircraft measurements. Total cumulative emissions of SF<sub>5</sub>CF<sub>3</sub> amount to around 5 kT.
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Based on density functional theory calculations we present a study of the gaseous oxidation of SO<sub>2</sub> to SO<sub>3</sub> by an anionic O<sub>3</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> cluster, <i>n</i> = 0–5. The configurations of the most relevant reactants, transition states, and products are discussed and compared to previous findings. Two different classes of transition states have been identified. One class is characterised by strong networks of hydrogen bonds, very similar to the reactant complexes. The other class is characterised by sparser structures of hydration water and is stabilised by high entropy. At temperatures relevant for atmospheric chemistry, the most energetically favourable class of transition states vary with the number of water molecules attached. A kinetic model is utilised, taking into account the most likely outcomes of the initial SO<sub>2</sub> O<sub>3</sub><sup>−</sup>(H<sub>2</sub>O)<sub><i>n</i></sub> collision complexes. This model shows that the reaction takes place at collision rates regardless of the number of water molecules involved. A lifetime analysis of the collision complexes supports this conclusion. Hereafter, the thermodynamics of water and O<sub>2</sub> condensation and evaporation from the product SO<sub>3</sub><sup>−</sup>O<sub>2</sub>(H<sub>2</sub>O)<sub><i>n</i></sub> cluster is considered and the final products are predicted to be O<sub>2</sub>SO<sub>3</sub><sup>−</sup> and O<sub>2</sub>SO<sub>3</sub><sup>−</sup>(H<sub>2</sub>O)<sub>1</sub>. The low degree of hydration is rationalised through a charge analysis of the relevant complexes. Finally, the thermodynamics of a few relevant reactions of the O<sub>2</sub>SO<sub>3</sub><sup>−</sup> and O<sub>2</sub>SO<sub>3</sub><sup>−</sup>(H<sub>2</sub>O)<sub>1</sub> complexes are considered.
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The relatively warm 2009–2010 Arctic winter was an exceptional one as the North Atlantic Oscillation index attained persistent extreme negative values. Here, selected aspects of the Arctic stratosphere during this winter inspired by the analysis of the international field experiment RECONCILE are presented. First of all, and as a kind of reference, the evolution of the polar vortex in its different phases is documented. Special emphasis is put on explaining the formation of the exceptionally cold vortex in mid winter after a sequence of stratospheric disturbances which were caused by upward propagating planetary waves. A major sudden stratospheric warming (SSW) occurring near the end of January 2010 concluded the anomalous cold vortex period. Wave ice polar stratospheric clouds were frequently observed by spaceborne remote-sensing instruments over the Arctic during the cold period in January 2010. Here, one such case observed over Greenland is analysed in more detail and an attempt is made to correlate flow information of an operational numerical weather prediction model to the magnitude of the mountain-wave induced temperature fluctuations. Finally, it is shown that the forecasts of the ECMWF ensemble prediction system for the onset of the major SSW were very skilful and the ensemble spread was very small. However, the ensemble spread increased dramatically after the major SSW, displaying the strong non-linearity and internal variability involved in the SSW event.
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During a three-year field campaign of measuring waterfall generated ions, we monitored five different waterfalls in the Austrian Alps. Most measurements were performed at the Krimml waterfall (Salzburg, Austria), which is the biggest waterfall in Europe, and the Gartl waterfall (Mölltal, Austria). We characterized spatial, time and size distributions of waterfall-generated ions under the influence of surrounding topography. The smallest ions with boundary diameters of 0.9, 1.5 and 2 nm, were measured with a cylindrical air ion detector (CDI-06), while ion sizes from 5.5 to 350 nm were measured using a modified Grimm SMPS aerosol spectrometer. High negative ion concentration gradients are detected in the vicinity of the waterfalls, whereas the increase of positive ions was only moderate. Ions in the nano range were the most abundant at 2 nm, and at 120 nm in the sub-micrometer range.
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Agricultural biomass burning (ABB) in Central and East China occurs every year from May to October and peaks in June. The biomass burning event in June 2007 was very strong. During the period from 26 May to 16 June 2007, ABB occurred mainly in Anhui, Henan, Jiangsu and Shandong provinces. A comprehensive set of aerosol optical depth (AOD) data, produced by a merger of AOD product data from the Moderate Resolution Imaging Spectroradiometer (MODIS) and the Multiangle Imaging Spectroradiometer (MIRS), is used to study the spatial and temporal distribution of agricultural biomass aerosols in Central and East China combining with ground observations from both AErosol RObotic NETwork (AERONET) and China Aerosol Remote Sensing NETwork (CARSNET) measurements. We compared merged AOD data with single-sensor single-algorithm AOD data (MODIS Dark Target AOD data, MODIS Deep Blue AOD data, SRAP-MODIS AOD data and MISR AOD data). In this comparison, we found merged AOD products can improve the quality of AOD products from single-sensor single-algorithm data sets by expanding the spatial coverage of the study area and keeping the statistical confidence in AOD parameters. There existed high correlation (0.8479) between the merged AOD data and AERONET measurements. Our merged AOD data make use of synergetic information conveyed in all of the available satellite data. The merged AOD data were used for the analysis of the biomass burning event from 26 May to 16 June 2007 together with meteorological data. The merged AOD products and the ground observations from China suggest that biomass burning in Central and East China has had great impact on AOD over China. Influenced by this ABB, the highest AOD value in Beijing on 12 June 2007 reached 5.71.
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This work presents a novel formulation of the ice nucleation spectrum, i.e. the function relating the ice crystal concentration to cloud formation conditions and aerosol properties. The new formulation is physically-based and explicitly accounts for the dependency of the ice crystal concentration on temperature, supersaturation, cooling rate, and particle size, surface area and composition. This is achieved by introducing the concepts of ice nucleation coefficient (the number of ice germs present in a particle) and nucleation probability dispersion function (the distribution of ice nucleation coefficients within the aerosol population). The new formulation is used to generate ice nucleation parameterizations for the homogeneous freezing of cloud droplets and the heterogeneous deposition ice nucleation on dust and soot ice nuclei. For homogeneous freezing, it was found that by increasing the dispersion in the droplet volume distribution the fraction of supercooled droplets in the population increases. For heterogeneous ice nucleation the new formulation consistently describes singular and stochastic behavior within a single framework. Using a fundamentally stochastic approach, both cooling rate independence and constancy of the ice nucleation fraction over time, features typically associated with singular behavior, were reproduced. Analysis of the temporal dependency of the ice nucleation spectrum suggested that experimental methods that measure the ice nucleation fraction over few seconds would tend to underestimate the ice nuclei concentration. It is shown that inferring the aerosol heterogeneous ice nucleation properties from measurements of the onset supersaturation and temperature may carry significant error as the variability in ice nucleation properties within the aerosol population is not accounted for. This work provides a simple and rigorous ice nucleation framework where theoretical predictions, laboratory measurements and field campaign data can be reconciled, and that is suitable for application in atmospheric modeling studies.
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The radiative forcing of dust emitted from the Southwest United States (US) deserts and its impact on monsoon circulation and precipitation over the North America monsoon (NAM) region are simulated using a coupled meteorology and aerosol/chemistry model (WRF-Chem) for 15 years (1995–2009). During the monsoon season, dust has a cooling effect (−0.90 W m<sup>−2</sup>) at the surface, a warming effect (0.40 W m<sup>−2</sup>) in the atmosphere, and a negative top-of-the-atmosphere (TOA) forcing (−0.50 W m<sup>−2</sup>) over the deserts on 24-h average. Most of the dust emitted from the deserts concentrates below 800 hPa and accumulates over the western slope of the Rocky Mountains and Mexican Plateau. The absorption of shortwave radiation by dust heats the lower atmosphere by up to 0.5 K day<sup>−1</sup> over the western slope of the Mountains. Model sensitivity simulations with and without dust for 15 summers (June-July-August) show that dust heating of the lower atmosphere over the deserts strengthens the low-level southerly moisture fluxes on both sides of the Sierra Madre Occidental. It also results in an eastward migration of NAM-driven moisture convergence over the western slope of the Mountains. These monsoonal circulation changes lead to a statistically significant increase of precipitation by up to ~40 % over the eastern slope of the Mountains (Arizona-New~Mexico-Texas regions). This study highlights the interaction between dust and the NAM system and motivates further investigation of possible dust feedback on monsoon precipitation under climate change and the mega-drought conditions projected for the future.
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Mesospheric water vapour has been observed above ALOMAR in northern Norway (69° N 16° E) by our group since 1995 using a 22 GHz ground based microwave spectrometer. A new instrument with higher sensitivity, providing a much better time resolution especially in the upper mesosphere, was installed in May 2008. The time resolution is high enough to provide observations of daily variations in the water vapour mixing ratio. We present the first ground based detections of tidal behaviour in the polar middle atmospheric water vapour distribution. <br><br> Diurnal and semidiurnal variations of water vapour have been observed and due to the long chemical lifetime of water they are assumed to be caused by changing wind patterns which transport water-rich or poor air into the observed region. The detected tidal behaviour does not follow any single other dynamical field but is instead assumed to be a result of the different wind components. <br><br> Both the diurnal and semidiurnal amplitude and phase components are resolved. The former shows a stable seasonal behaviour consistent with earlier observations of wind fields and model calculations, whereas the latter appears more complex and no regular behaviour has so far been observed.