bluuebunny/crossref_metadata_2025 huggingface dataset:
Direct determination of highly size-resolved turbulent particle fluxes with the disjunct eddy covariance method and a 12 – stage electrical low pressure impactor
Authors: Schmidt A. , Klemm O.
Published: April 2010

Abstract. During summer 2007, turbulent vertical particle mass and number fluxes were measured for a period of 98 days near the city centre of Münster in north-west Germany. For this purpose, a valve controlled disjunct eddy covariance system was mounted at 65 m a.g.l. on a military radio tower. The concentration values for 11 size bins with aerodynamic diameters (D50) from 0.03 to 10 μm were measured with an electrical low pressure impactor. After comparison with other fluxes obtained from 10 Hz measurements with the classical eddy covariance method, the loss of information concerning high frequent parts of the flux could be stated as negligible. The results offer an extended insight in the turbulent atmospheric exchange of aerosol particles by highly size-resolved particle fluxes covering 11 size bins and show that the city of Münster acts as a relevant source for aerosol particles. Significant differences occur between the fluxes of the various particle size classes. While the total particle number flux shows a pattern which is strictly correlated to the diurnal course of the turbulence regime and the traffic intensity, the total mass flux exhibits a single minimum in the evening hours when coarse particles start to deposit. As a result, a mean mass deposition of about 10 mg m−2 per day was found above the urban test site, covering the aerosol size range from 40 nm to 2.0 μm. By contrast, the half-hourly total number fluxes accumulated over the lower ELPI stages range from −4.29×107 to +1.44×108 particles m−2 s−1 and are clearly dominated by the sub-micron particle fraction of the impactor stages with diameters between 40 nm and 320 nm. The averaged number fluxes of particles with diameters between 2.0 and 6.4 μm show lower turbulent dynamics during daytime and partially remarkably high negative fluxes with mean deposition velocities of 2×10−3 m s−1 that appear temporary during noontime and in the evening hours.
Large-scale planetary disturbances in stratospheric temperature at high-latitudes in the southern summer hemisphere
Authors: Shepherd M. G. , Tsuda T.
Published: April 2010

Abstract. The global structure and propagation of large-scale (periods >5 days) waves in the Southern Hemisphere summer (December 2006–February 2007) at 60° S–75° S latitude are examined using temperature data from GPS radio occultation measurements by COSMIC/FORMOSAT 3 satellite constellation at 20 km and 30 km altitude. Spectral analysis has revealed eastward propagating planetary scale perturbations with wavenumbers 1 and 2 and periods of 10, 16 and 23 days, and stationary waves with wavenumbers 1 and 2. The results obtained show a very dynamically active Antarctic summer stratosphere. The novel aspect of the work is in the use of the GPS COSMIC data providing multiple local times each day, thus allowing large-scale wave analysis at high Southern latitudes and revealing planetary wave activity not normally observed in summer, but more consistent with late winter and spring conditions in the stratosphere.
Traffic restrictions in Beijing during the Sino-African Summit 2006: aerosol size distribution and visibility compared to long-term in situ observations
Authors: Cheng Y. F. , Heintzenberg J. , Wehner B. , Wu Z. J. , Su H. , Hu M. , Mao J. T.
Published: April 2010

Abstract. Based on the long-term in-situ observations of aerosol particle number size distributions and meteorological parameters, the measures of traffic restriction during the Sino-African Summit (4–6 November 2006) in Beijing, China have been found to be efficient in reducing the number concentration of aerosol particles, in particular Aitken and accumulation mode particles, and in improving the visibility when local emissions dominated. The influence of traffic restrictions on the particle concentrations differed for different particle sizes. More significant effects on fine particles with diameters ranging from 40 to 500 nm have been found. Based on statistical analysis of long-term observations, under comparable weather conditions, the number concentrations of the particles in Aitken and accumulation modes seemingly were reduced by 20–60% when the traffic restrictions were in place. This change may be mainly due to the reduction of secondary particle contributions. However, it is worth to notice that the reduction of 60% might overestimate the effect of the measures of traffic control, due to the inherent data shortage with very high wind speeds in the comparison data population. Our size-dependent aerosol data also indicate that measures led to reductions in particulate air pollution in the optically most important diameter range, whereas further vehicle restriction measures might lead to an increase in ultrafine particle formation if the condensational sink further decreased. Assuming that there were no traffic restrictions and with normal levels of the vehicle emissions, the visibilities during the Summit would have been lower by about 20–45%. The fact that over 95% cases with visibility range lower than 5 km during 2004 to 2007 occurred when the local wind speed was lower than 3 m s−1 may suggest that the importance of the emission restrictions is highest when the wind speed is lower than 3 m s−1, concerning the improvement of serious low visibility situations in Beijing.
High spatial resolution measurements of NO2 applying Topographic Target Light scattering-Differential Optical Absorption Spectroscopy (ToTaL-DOAS)
Authors: Frins E. , Platt U. , Wagner T.
Published: April 2010

Abstract. Topographic Target Light scattering – Differential Optical Absorption Spectroscopy (ToTaL-DOAS), also called Target-DOAS, is a novel experimental procedure to retrieve trace gas concentrations present in the low atmosphere. Scattered sunlight (diffuse or specular) reflected from natural or artificial targets located at different distances are analyzed to retrieve the spatial distribution of the concentration of different trace gases like NO2, SO2 and others. We report high spatial resolution measurements of NO2 mixing ratios in the city of Montevideo (Uruguay) observing three buildings as targets with a Mini-DOAS instrument. Our instrument was 146 m, 196 m, and 280 m apart from three different buildings located along a main Avenue. We obtain temporal variation of NO2 mixing ratios between 30 ppb and 65 ppb from measurements of November 2007 and mixing ratios up to 50 ppb from measurements of August and September 2008. Our measurements demonstrate that ToTaL-DOAS observations can be made over relative short distances. In polluted air masses, the retrieved absorption signal was found to be sufficiently strong to allow measurements over distances in the range of several tens of meters.
Mass concentrations of black carbon measured by four instruments in the middle of Central East China in June 2006
Authors: Kanaya Y. , Komazaki Y. , Pochanart P. , Liu Y. , Akimoto H. , Gao J. , Wang T. , Wang Z.
Published: April 2010

Abstract. Mass concentrations of black carbon (BC) were determined in June 2006 at the top of Mount Tai (36.26° N, 117.11° E, 1534 m a.s.l.), located in the middle of Central East China, using four different instruments: a multi-angle absorption photometer (5012 MAAP, Thermo), a particle soot absorption photometer (PSAP, Radiance Research), an ECOC semi-continuous analyzer (Sunset Laboratory) and an Aethalometer (AE-21, Magee Scientific). High correlation coefficients (R2>0.88) were obtained between the measurements of the BC mass concentrations made using the different instruments. From the range of the slopes of the linear least-square fittings, we concluded that BC concentrations regionally-representative of the area were measured in a range with a maximum-to-minimum ratio of 1.5 (an exception was that the BC (PM2.5) concentrations derived from MAAP were ~2 times higher than the optical measurements (PM2.5) derived from the ECOC analyzer). While this range is significant, it is still sufficiently narrow to better constrain the large and highly uncertain emission rate of BC from Central East China. In detail, two optical instruments (the MAAP and the PSAP equipped with a heated inlet 400°C) tended to give higher concentrations than the thermal EC concentrations observed by the ECOC analyzer. The ratios of optical BC to thermal EC showed a positive correlation with the OC/EC ratio reported by the ECOC analyzer, suggesting two explanations. One is that the optical instruments overestimated BC concentrations in spite of careful cancellation of the scattering effect in the MAAP instrument and the expected evaporation of volatile species by heating the inlet of the PSAP instrument. The other is that the determined split points between OC and EC were too late when a large amount of OC underwent charring during the analysis, resulting in an underestimation of EC by the ECOC analyzer. High ratios of optical BC to thermal EC were recorded when the NOx/NOy ratio was low, implying the coating of the particles became thicker in an aged air mass and thus resulted in the optical instruments overestimating BC concentrations because of the lensing effect.
Short- and medium-term atmospheric constituent effects of very large solar proton events
Authors: Jackman C. H. , Marsh D. R. , Vitt F. M. , Garcia R. R. , Fleming E. L. , Labow G. J. , Randall C. E. , López-Puertas M. , Funke B. , von Clarmann T. , Stiller G. P.
Published: April 2010

Abstract. Solar eruptions sometimes produce protons, which impact the Earth's atmosphere. These solar proton events (SPEs) generally last a few days and produce high energy particles that precipitate into the Earth's atmosphere. The protons cause ionization and dissociation processes that ultimately lead to an enhancement of odd-hydrogen and odd-nitrogen in the polar cap regions (>60° geomagnetic latitude). We have used the Whole Atmosphere Community Climate Model (WACCM3) to study the atmospheric impact of SPEs over the period 1963–2005. The very largest SPEs were found to be the most important and caused atmospheric effects that lasted several months after the events. We present the short- and medium-term (days to a few months) atmospheric influence of the four largest SPEs in the past 45 years (August 1972; October 1989; July 2000; and October–November 2003) as computed by WACCM3 and observed by satellite instruments. Polar mesospheric NOx (NO+NO2) increased by over 50 ppbv and mesospheric ozone decreased by over 30% during these very large SPEs. Changes in HNO3, N2O5, ClONO2, HOCl, and ClO were indirectly caused by the very large SPEs in October–November 2003, were simulated by WACCM3, and previously measured by Envisat Michelson Interferometer for Passive Atmospheric Sounding (MIPAS). WACCM3 output was also represented by sampling with the MIPAS averaging kernel for a more valid comparison. Although qualitatively similar, there are discrepancies between the model and measurement with WACCM3 predicted HNO3 and ClONO2 enhancements being smaller than measured and N2O5 enhancements being larger than measured. The HOCl enhancements were fairly similar in amounts and temporal variation in WACCM3 and MIPAS. WACCM3 simulated ClO decreases below 50 km, whereas MIPAS mainly observed increases, a very perplexing difference. Upper stratospheric and lower mesospheric NOx increased by over 10 ppbv and was transported during polar night down to the middle stratosphere in several weeks past the SPE. The WACCM3 simulations confirmed the SH HALOE observations of enhanced NOx in September 2000 as a result of the July 2000 SPE and the NH SAGE II observations of enhanced NO2 in March 1990 as a result of the October 1989 SPEs.
Summertime elemental mercury exchange of temperate grasslands on an ecosystem-scale
Authors: Fritsche J. , Wohlfahrt G. , Ammann C. , Zeeman M. , Hammerle A. , Obrist D. , Alewell C.
Published: April 2010

Abstract. In order to estimate the air-surface mercury exchange of grasslands in temperate climate regions, fluxes of gaseous elemental mercury (GEM) were measured at two sites in Switzerland and one in Austria during summer 2006. Two classic micrometeorological methods (aerodynamic and modified Bowen ratio) have been applied to estimate net GEM exchange rates and to determine the response of the GEM flux to changes in environmental conditions (e.g. heavy rain, summer ozone) on an ecosystem-scale. Both methods proved to be appropriate to estimate fluxes on time scales of a few hours and longer. Average dry deposition rates up to 4.3 ng m−2 h−1 and mean deposition velocities up to 0.10 cm s−1 were measured, which indicates that during the active vegetation period temperate grasslands are a small net sink for atmospheric mercury. With increasing ozone concentrations depletion of GEM was observed, but could not be quantified from the flux signal. Night-time deposition fluxes of GEM were measured and seem to be the result of mercury co-deposition with condensing water. Effects of grass cuts could also be observed, but were of minor magnitude.
Development and evaluation of an operational SDS forecasting system for East Asia: CUACE/Dust
Authors: Zhou C. H. , Gong S. L. , Zhang X. Y. , Wang Y. Q. , Niu T. , Liu H. L. , Zhao T. L. , Yang Y. Q. , Hou Q.
Published: April 2010

Abstract. CUACE/Dust, an operational mesoscale sand and dust storm (SDS) forecasting system for East Asia, has been developed by online coupling a dust aerosol emission scheme and dust aerosol microphysics onto a regional meteorological model with improved advection and diffusion schemes and a detailed Northeast Asia soil erosion database. With improved initial dust aerosol conditions through a 3-DVar data assimilation system, CUACE/Dust successfully forecasted most of the 31 SDS processes in East Asia. A detailed comparison of the model predictions for the 8–12 March SDS process with surface network observations and lidar measurements revealed a robust forecasting ability of the system. The time series of the operationally forecasted dust concentrations for a number of representative stations for the whole spring 2006 (1 March–31 May) were evaluated against surface PM10 monitoring data, showing a good agreement in terms of the SDS timing and magnitudes at and near the source regions where dust aerosols dominate. For the operational forecasts of spring 2006 in East Asia, a TS (threat score) system evaluated the performance of CUACE/Dust against all available observations and rendered a spring averaged TS value of 0.31 for FT1 (24 h forecasts), 0.23 for FT2 (48 h forecasts) and 0.21 for FT3 (72 h forecasts).
Investigation of molar volume and surfactant characteristics of water-soluble organic compounds in biomass burning aerosol
Authors: Asa-Awuku A. , Sullivan A. P. , Hennigan C. J. , Weber R. J. , Nenes A.
Published: April 2010

Abstract. In this study, we characterize the CCN activity of the water-soluble organics in biomass burning aerosol. The aerosol after collection upon filters is dissolved in water using sonication. Hydrophobic and hydrophilic components are fractionated from a portion of the original sample using solid phase extraction, and subsequently desalted. The surface tension and CCN activity of these different samples are measured with a KSV CAM 200 goniometer and a DMT Streamwise Thermal Gradient CCN Counter, respectively. The measurements show that the strongest surfactants are isolated in the hydrophobic fraction, while the hydrophilics exhibit negligible surface tension depression. The presence of salts (primarily (NH4)2SO4) in the hydrophobic fraction substantially enhances surface tension depression; their synergistic effects considerably enhance CCN activity, exceeding that of pure (NH4)2SO4. From our analysis, average thermodynamic properties (i.e, molar volume) are determined for samples using our newly developed Köhler Theory Analysis (KTA) method. The molar mass of the hydrophilic and hydrophobic aerosol components is estimated to be 87±26 g mol−1 and 780±231 g mol−1, respectively. KTA also suggests that the relative proportion (in moles) of hydrophobic to hydrophilic compounds in the original sample to be 1:3. For the first time, KTA is applied to an aerosol with this level of complexity and displays its potential for providing physically-based constraints for GCM parameterizations of the aerosol indirect effect.
Long-term climatology of air mass transport through the Tropical Tropopause Layer (TTL) during NH winter
Authors: Krüger K. , Tegtmeier S. , Rex M.
Published: April 2010

Abstract. A long-term climatology of air mass transport through the tropical tropopause layer (TTL) is presented, covering the period from 1962–2005. The transport through the TTL is calculated with a Lagrangian approach using radiative heating rates as vertical velocities in an isentropic trajectory model. We demonstrate the improved performance of such an approach compared to previous studies using vertical winds from meteorological analyses. Within the upper part of the TTL, the averaged diabatic ascent is 0.5 K/day during Northern Hemisphere (NH) winters 1992–2001. Climatological maps show a cooling and strengthening of this part of the residual circulation during the 1990s and early 2000s compared to the long-term mean. Lagrangian cold point (LCP) fields show systematic differences for varying time periods and natural forcing components. The interannual variability of LCP temperature and density fields is found to be influenced by volcanic eruptions, El Niño Southern Oscillation (ENSO), Quasi-Biennial Oscillation (QBO) and the solar cycle. The coldest and driest TTL is reached during QBO easterly phase and La Niña over the western Pacific, whereas during volcanic eruptions, El Niño and QBO westerly phase it is warmer and less dry.
Weekly periodicities of Aerosol Optical Thickness over Central Europe – evidence of an anthropogenic direct aerosol effect
Authors: Bäumer D. , Rinke R. , Vogel B.
Published: April 2010

Abstract. Statistical analyses of data from ground-based sun photometer stations in Central Europe are presented. All stations are part of the Aerosol Robotic Network (AERONET), and only data of the highest data quality level 2.0 has been applied. The averages by weekday of Aerosol Optical Thickness (AOT) at a wavelength of 440 nm of 12 of the 14 stations in the investigation area show a weekly periodicity with lowest values on Sunday and Monday, but greatest values from Wednesday until Saturday, that is significant at least on a 90% level. The stations in Germany and in Greater Paris show weekly cycles with ranges of about 20% on average. In Northern Italy and Switzerland this range is about 10% on average. By applying several checks, we exclude that the weekly cycles were caused by a maintenance effect or by different retrieval conditions as a consequence of a weekly cycle in cloud cover. The corresponding weekly cycle of anthropogenic gaseous and particulate emissions leads us to the conclusion of the anthropogenic origin of the weekly AOT cycle. Since these AOT patterns are derived from the reduction of the direct sun radiation by the columnar atmospheric aerosol, this result represents strong evidence for an anthropogenic direct aerosol effect on shortwave radiation. Furthermore, this study makes a first contribution to the understanding and explanation of recently observed weekly periodicities in meteorological variables as temperature in Germany.
The response of surface ozone to climate change over the Eastern United States
Authors: Racherla P. N. , Adams P. J.
Published: April 2010

Abstract. We investigate the response of surface ozone (O3) to future climate change in the eastern United States by performing simulations corresponding to present (1990s) and future (2050s) climates using an integrated model of global climate, tropospheric gas-phase chemistry, and aerosols. A future climate has been imposed using ocean boundary conditions corresponding to the IPCC SRES A2 scenario for the 2050s decade. Present-day anthropogenic emissions and CO2/CH4 mixing ratios have been used in both simulations while climate-sensitive emissions were allowed to vary with the simulated climate. The severity and frequency of O3 episodes in the eastern U.S. increased due to future climate change, primarily as a result of increased O3 chemical production. The 95th percentile O3 mixing ratio increased by 5 ppbv and the largest frequency increase occured in the 80–90 ppbv range; the US EPA's current 8-h ozone primary standard is 80 ppbv. The increased O3 chemical production is due to increases in: 1) natural isoprene emissions; 2) hydroperoxy radical concentrations resulting from increased water vapor concentrations; and, 3) NOx concentrations resulting from reduced PAN. The most substantial and statistically significant (p<0.05) increases in episode frequency occurred over the southeast and midatlantic U.S., largely as a result of 20% higher annual-average natural isoprene emissions. These results suggest a lengthening of the O3 season over the eastern U.S. in a future climate to include late spring and early fall months. Increased chemical production and shorter average lifetime are two consistent features of the seasonal response of surface O3, with increased dry deposition loss rates contributing most to the reduced lifetime in all seasons except summer. Significant interannual variability is observed in the frequency of O3 episodes and we find that it is necessary to utilize 5 years or more of simulation data in order to separate the effects of interannual variability and climate change on O3 episodes in the eastern United States.
On the vertical distribution of boundary layer halogens over coastal Antarctica: implications for O3, HOx, NOx and the Hg lifetime
Authors: Saiz-Lopez A. , Plane J. M. C. , Mahajan A. S. , Anderson P. S. , Bauguitte S. J.-B. , Jones A. E. , Roscoe H. K. , Salmon R. A. , Bloss W. J. , Lee J. D. , Heard D. E.
Published: April 2010

Abstract. A one-dimensional chemical transport model has been developed to investigate the vertical gradients of bromine and iodine compounds in the Antarctic coastal boundary layer (BL). The model has been applied to interpret recent year-round observations of iodine and bromine monoxides (IO and BrO) at Halley Station, Antarctica. The model requires an equivalent I atom flux of ~1010 molecule cm−2 s−1 from the snowpack in order to account for the measured IO levels, which are up to 20 ppt during spring. Using the current knowledge of gas-phase iodine chemistry, the model predicts significant gradients in the vertical distribution of iodine species. However, recent ground-based and satellite observations of IO imply that the radical is well-mixed in the Antarctic boundary layer, indicating a longer than expected atmospheric lifetime for the radical. This can be modelled by including photolysis of the higher iodine oxides (I2O2, I2O3, I2O4 and I2O5), and rapid recycling of HOI and INO3 through sea-salt aerosol. The model also predicts significant concentrations (up to 25 ppt) of I2O5 in the lowest 10 m of the boundary layer. Heterogeneous chemistry involving sea-salt aerosol is also necessary to account for the vertical profile of BrO. Iodine chemistry causes a large increase (typically more than 3-fold) in the rate of O3 depletion in the BL, compared with bromine chemistry alone. Rapid entrainment of O3 from the free troposphere appears to be required to account for the observation that on occasion there is little O3 depletion at the surface in the presence of high concentrations of IO and BrO. The halogens also cause significant changes to the vertical profiles of OH and HO2 and the NO2/NO ratio. The average Hg0 lifetime against oxidation is also predicted to be about 10 h during springtime. An important result from the model is that very large fluxes of iodine precursors into the boundary layer are required to account for the observed levels of IO. The mechanisms which cause these emissions are unknown. Overall, our results show that halogens profoundly influence the oxidizing capacity of the Antarctic troposphere.
A case of extreme particulate matter concentrations over Central Europe caused by dust emitted over the southern Ukraine
Authors: Birmili W. , Schepanski K. , Ansmann A. , Spindler G. , Tegen I. , Wehner B. , Nowak A. , Reimer E. , Mattis I. , Müller K. , Brüggemann E. , Gnauk T. , Herrmann H. , Wiedensohler A. , Althausen D. , Schladitz A. , Tuch T. , Löschau G.
Published: April 2010

Abstract. On 24 March 2007, an extraordinary dust plume was observed in the Central European troposphere. Satellite observations revealed its origins in a dust storm in Southern Ukraine, where large amounts of soil were resuspended from dried-out farmlands at wind gusts up to 30 m s−1. Along the pathway of the plume, maximum particulate matter (PM10) mass concentrations between 200 and 1400 μg m−3 occurred in Slovakia, the Czech Republic, Poland, and Germany. Over Germany, the dust plume was characterised by a volume extinction coefficient up to 400 Mm−1 and a particle optical depth of 0.71 at wavelength 0.532 μm. In-situ size distribution measurements as well as the wavelength dependence of light extinction from lidar and Sun photometer measurements confirmed the presence of a coarse particle mode with diameters around 2–3 μm. Chemical particle analyses suggested a fraction of 75% crustal material in daily average PM10 and up to 85% in the coarser fraction PM10–2.5. Based on the particle characteristics as well as a lack of increased CO and CO2 levels, a significant impact of biomass burning was ruled out. The reasons for the high particle concentrations in the dust plume were twofold: First, dust was transported very rapidly into Central Europe in a boundary layer jet under dry conditions. Second, the dust plume was confined to a relatively stable boundary layer of 1.4–1.8 km height, and could therefore neither expand nor dilute efficiently. Our findings illustrate the capacity of combined in situ and remote sensing measurements to characterise large-scale dust plumes with a variety of aerosol parameters. Although such plumes from Southern Eurasia seem to occur rather infrequently in Central Europe, its unexpected features highlights the need to improve the description of dust emission, transport and transformation processes needs, particularly when facing the possible effects of further anthropogenic desertification and climate change.
Sensitivity of satellite observations for freshly produced lightning NOx
Authors: Beirle S. , Salzmann M. , Lawrence M. G. , Wagner T.
Published: April 2010

Abstract. In this study, we analyse the sensitivity of nadir viewing satellite observations in the visible range to freshly produced lightning NOx. This is a particular challenge due to the complex and highly variable conditions of meteorology, (photo-) chemistry, and radiative transfer in and around cumulonimbus clouds. For the first time, such a study is performed accounting for photo-chemistry, dynamics, and radiative transfer in a consistent way: A one week episode in the TOGA COARE/CEPEX region (Pacific) in December 1992 is simulated with a 3-D cloud resolving chemistry model. The simulated hydrometeor mixing ratios are fed into a Monte Carlo radiative transfer model to calculate box-Air Mass Factors (box-AMFs) for NO2. From these box-AMFs, together with model NOx profiles, slant columns of NO2 (SNO2), i.e. synthetic satellite measurements, are calculated and set in relation to the actual model NOx vertical column (VNOx), yielding the "sensitivity" SNO2/VNOx. From this study, we find a mean sensitivity of 0.46. NOx below the cloud bottom is mostly present as NO2, but shielded from the satellites' view, whereas NOx at the cloud top or above is shifted to NO due to high photolysis and low temperature, and hence not detectable from space. However, a significant fraction of the lightning produced NOx in the middle part of the cloud is present as NO2 and has a good visibility from space. Due to the resulting total sensitivity being quite high, nadir viewing satellites provide a valuable additional platform to quantify NOx production by lightning; strong lightning events over "clean" regions should be clearly detectable in satellite observations. Since the observed enhancement of NO2 column densities over mesoscale convective systems are lower than expected for current estimates of NOx production per flash, satellite measurements can in particular constrain the upper bound of lightning NOx production estimates.
Total and partial cloud amount detection during summer 2005 at Westerland (Sylt, Germany)
Authors: Schade N. H. , Macke A. , Sandmann H. , Stick C.
Published: April 2010

Abstract. The detection of cloudiness is investigated by means of partial and total cloud amount estimations from pyrgeometer radiation measurements and visible all-sky imager observations. The measurements have been performed in Westerland, a seaside resort on the North Sea island of Sylt, Germany, during summer 2005. An improvement to previous studies on this subject resulting in the first time partial cloud amounts (PCAs), defined as cloud amounts without high clouds calculated from longwave downward radiation (LDR) according to the APCADA algorithm (Dürr and Philipona, 2004), are validated against both human observations from the National Meteorological Servive DWD at the nearby airport of Sylt and digital all-sky imaging. The aim is to establish the APCADA scheme at a coastal midlatitude site for longterm observations of cloud cover and to quantify errors resulting from the different methods of detecting cloudiness. Differences between the resulting total cloud amounts (TCAs), defined as cloud amount for all-cloud situations, derived from the camera images and from human observations are within ±1 octa in 72% and within ±2 octa in 85% of the cases. Compared to human observations, PCA measurements, according to APCADA, underestimate the observed cloud cover in 47% of all cases and the differences are within ±1 octa in 60% and ±2 octa in 74% of all cases. Since high cirrus clouds can not be derived from LDR, separate comparisons for all cases without high clouds have been performed showing an agreement within ±1(2) octa in 73(90)% for PCA and also for camera-derived TCA. For this coastal mid-latitude site under investigation, we find similar though slightly smaller agreements to human observations as reported by Dürr and Philipona (2004). Though limited to daytime, the cloud cover retrievals from the sky imager are not really affected by cirrus clouds and provide a more reliable cloud climatology for all-cloud conditions than APCADA.
Saharan dust transport and deposition towards the tropical northern Atlantic
Authors: Schepanski K. , Tegen I. , Macke A.
Published: April 2010

Abstract. We present a study of Saharan dust export towards the tropical North Atlantic using the regional dust emission, transport and deposition model LM-MUSCAT. Horizontal and vertical distribution of dust optical thickness, concentration, and dry and wet deposition rates are used to describe seasonality of dust export and deposition towards the eastern Atlantic for three typical months in different seasons. Deposition rates strongly depend on the vertical dust distribution, which differs with seasons. Furthermore the contribution of dust originating from the Bodélé Depression to Saharan dust over the Atlantic is investigated. A maximum contribution of Bodélé dust transported towards the Cape Verde Islands is evident in winter when the Bodélé source area is most active and dominant with regard to activation frequency and dust emission. Limitations of using satellite retrievals to estimate dust deposition are highlighted.
Transitional dispersive scenarios driven by mesoscale flows on complex terrain under strong dry convective conditions
Authors: Palau J. L. , Pérez-Landa G. , Millán M. M.
Published: April 2010

Abstract. By experimentation and modelling, this paper analyses the atmospheric dispersion of the SO2 emissions from a power plant on complex terrain under strong convective conditions, describing the main dispersion features as an ensemble of "stationary dispersive scenarios" and reformulating some "classical" dispersive concepts to deal with the systematically monitored summer dispersive scenarios in inland Spain. The results and discussions presented arise from a statistically representative study of the physical processes associated with the multimodal distribution of pollutants aloft and around a 343-m-tall chimney under strong dry convective conditions in the Iberian Peninsula. This paper analyses the importance of the identification and physical implications of transitional periods for air quality applications. The indetermination of a transversal plume to the preferred transport direction during these transitional periods implies a small (or null) physical significance of the classical definition of horizontal standard deviation of the concentration distribution.
Increasing ozone in marine boundary layer inflow at the west coasts of North America and Europe
Authors: Parrish D. D. , Millet D. B. , Goldstein A. H.
Published: April 2010

Abstract. An effective method is presented for determining the ozone (O3) mixing ratio in the onshore flow of marine air at the North American west coast. By combining the data available from all marine boundary layer (MBL) sites with simultaneous wind data, decadal temporal trends of MBL O3 in all seasons are established with high precision. The average springtime temporal trend over the past two decades is 0.46 ppbv/yr with a 95% confidence limit of 0.13 ppbv/yr, and statistically significant trends are found for all seasons except autumn, which does have a significantly smaller trend than other seasons. The average trend in mean annual ozone is 0.34±0.09 ppbv/yr. These decadal trends at the North American west coast present a striking comparison and contrast with the trends reported for the European west coast at Mace Head, Ireland. The trends in the winter, spring and summer seasons compare well at the two locations, while the Mace Head trend is significantly greater in autumn. Even though the trends are similar, the absolute O3 mixing ratios differ markedly, with the marine air arriving at Europe in all seasons containing 7±2 ppbv higher ozone than marine air arriving at North America. Further, the ozone mixing ratios at the North American west coast show no indication of stabilizing as has been reported for Mace Head. In a larger historical context the background boundary layer O3 mixing ratios over the 130 years covered by available data have increased substantially (by a factor of two to three), and this increase continues at present, at least in the MBL of the Pacific coast region of North America. The reproduction of the increasing trends in MBL O3 over the past two decades, as well as the difference in the O3 mixing ratios between the two coastal regions will present a significant challenge for global chemical transport models. Further, the ability of the models to at least semi-quantitatively reproduce the longer-term, historical trends may an even greater challenge.
Intensification of tropical cyclones in the GFS model
Authors: Marín J. C. , Raymond D. J. , Raga G. B.
Published: April 2010

Abstract. Special forecasts from the Global Forecast System (GFS) model were used in this study to evaluate how the intensification process in a tropical cyclone is represented in this model. Several tropical cyclones that developed in 2005 were analyzed in terms of the storm-scale circulation rather than more traditional measures such as maximum wind or minimum central pressure. The primary balance governing the circulation in the planetary boundary layer is between the convergence of environmental vorticity, which tends to spin up the storm, and surface friction, which tends to spin it down. In addition, we employ recently developed ideas about the relationship between precipitation and the saturation fraction of the environment to understand the factors controlling mass, and hence vorticity convergence. The budget of moist entropy is central to this analysis. Two well-known governing factors for cyclone intensification emerge from this study; surface moist entropy fluxes, dependent in the model on sea surface temperature and cyclone-generated surface winds, and ventilation of the system by dry environmental air. Quantitative expressions for the role of these factors in cyclone intensification are presented in this paper.
Physical interpretation of the spectral radiative signature in the transition zone between cloud-free and cloudy regions
Authors: Chiu J. C. , Marshak A. , Knyazikhin Y. , Pilewski P. , Wiscombe W. J.
Published: April 2010

Abstract. One-second-resolution zenith radiance measurements from the Atmospheric Radiation Measurement program's new shortwave spectrometer (SWS) provide a unique opportunity to analyze the transition zone between cloudy and cloud-free air, which has considerable bearing on the aerosol indirect effect. In the transition zone, we find a remarkable linear relationship between the sum and difference of radiances at 870 and 1640 nm wavelengths. The intercept of the relationship is determined primarily by aerosol properties, and the slope by cloud properties. We then show that this linearity can be predicted from simple theoretical considerations and furthermore that it supports the hypothesis of inhomogeneous mixing, whereby optical depth increases as a cloud is approached but the effective drop size remains unchanged.
Organic nitrate and secondary organic aerosol yield from NO3 oxidation of β-pinene evaluated using a gas-phase kinetics/aerosol partitioning model
Authors: Fry J. L. , Kiendler-Scharr A. , Rollins A. W. , Wooldridge P. J. , Brown S. S. , Fuchs H. , Dubé W. , Mensah A. , dal Maso M. , Tillmann R. , Dorn H.-P. , Brauers T. , Cohen R. C.
Published: April 2010

Abstract. The yields of organic nitrates and of secondary organic aerosol (SOA) particle formation were measured for the reaction NO3+β-pinene under dry and humid conditions in the atmosphere simulation chamber SAPHIR at Research Center Jülich. These experiments were conducted at low concentrations of NO3 (NO3+N2O5<10 ppb) and β-pinene (peak~15 ppb), with no seed aerosol. SOA formation was observed to be prompt and substantial (~50% mass yield under both dry conditions and at 60% RH), and highly correlated with organic nitrate formation. The observed gas/aerosol partitioning of organic nitrates can be simulated using an absorptive partitioning model to derive an estimated vapor pressure of the condensing nitrate species of pvap~5×10−6 Torr (6.67×10−4 Pa), which constrains speculation about the oxidation mechanism and chemical identity of the organic nitrate. Once formed the SOA in this system continues to evolve, resulting in measurable aerosol volume decrease with time. The observations of high aerosol yield from NOx-dependent oxidation of monoterpenes provide an example of a significant anthropogenic source of SOA from biogenic hydrocarbon precursors. Estimates of the NO3+β-pinene SOA source strength for California and the globe indicate that NO3 reactions with monoterpenes are likely an important source (0.5–8% of the global total) of organic aerosol on regional and global scales.
Airborne observations of total RONO2: new constraints on the yield and lifetime of isoprene nitrates
Authors: Perring A. E. , Bertram T. H. , Wooldridge P. J. , Fried A. , Heikes B. G. , Dibb J. , Crounse J. D. , Wennberg P. O. , Blake N. J. , Blake D. R. , Brune W. H. , Singh H. B. , Cohen R. C.
Published: April 2010

Abstract. Formation of isoprene nitrates (INs) is an important free radical chain termination step ending production of ozone and possibly affecting formation of secondary organic aerosol. Isoprene nitrates also represent a potentially large, unmeasured contribution to OH reactivity and are a major pathway for the removal of nitrogen oxides from the atmosphere. Current assessments indicate that formation rates of isoprene nitrates are uncertain to a factor of 2–3 and the subsequent fate of isoprene nitrates remains largely unconstrained by laboratory, field or modeling studies. Measurements of total alkyl and multifunctional nitrates (ΣANs), NO2, total peroxy nitrates (ΣPNs), HNO3, CH2O, isoprene and other VOC were obtained from the NASA DC-8 aircraft during summer 2004 over the continental US during the INTEX-NA campaign. These observations represent the first characterization of ΣANs over a wide range of land surface types and in the lower free troposphere. ΣANs were a significant, 12–20%, fraction of NOy throughout the experimental domain and ΣANs were more abundant when isoprene was high. We use the observed hydrocarbon species to calculate the relative contributions of ΣAN precursors to their production. These calculations indicate that isoprene represents at least three quarters of the ΣAN source in the summertime continental boundary layer of the US. An observed correlation between ΣANs and CH2O is used to place constraints on nitrate yields from isoprene oxidation, atmospheric lifetimes of the resulting nitrates and recycling efficiencies of nitrates during subsequent oxidation. We find reasonable fits to the data using sets of production rates, lifetimes and recycling efficiencies of INs as follows (4.4%, 16 h, 97%), (8%, 2.5 h, 79%) and (12%, 95 min, 67%). The analysis indicates that the lifetime of ΣANs as a pool of compounds is considerably longer than the lifetime of the individual isoprene nitrates to reaction with OH, implying that the organic nitrate functionality is at least partially maintained through a second oxidation cycle.
Aerosol and thermodynamic effects on tropical cloud systems during TWPICE and ACTIVE
Authors: May P. T. , Allen G. , Vaughan G. , Connolly P.
Published: April 2010

Abstract. Regularly occurring storms over the Tiwi Islands, north of Darwin, Australia are used as a laboratory for investigating the relative importance of thermodynamic parameters, shear and aerosols on the amount and intensity of convection over the islands during the pre-monsoon and monsoon break periods of the 2005–2006 summer wet season. Storm systems on individual days are characterised by simple metrics derived from polarimetric radar data. The analysis shows clear dependencies on thermodynamic and shear parameters. The shear dependence was unexpected, as high shear implied less activity, but this is likely an island effect. There are some indications of a dependence of storm intensity on aerosol, but mid-level moisture differences may also play a role.
The Tropical Tropopause Layer 1960–2100
Authors: Gettelman A. , Birner T. , Eyring V. , Akiyoshi H. , Bekki S. , Brühl C. , Dameris M. , Kinnison D. E. , Lefevre F. , Lott F. , Mancini E. , Pitari G. , Plummer D. A. , Rozanov E. , Shibata K. , Stenke A. , Struthers H. , Tian W.
Published: April 2010

Abstract. The representation of the Tropical Tropopause Layer (TTL) in 13 different Chemistry Climate Models (CCMs) designed to represent the stratosphere is analyzed. Simulations for 1960–2005 and 1980–2100 are analyzed. Simulations for 1960–2005 are compared to reanalysis model output. CCMs are able to reproduce the basic structure of the TTL. There is a large (10 K) spread in annual mean tropical cold point tropopause temperatures. CCMs are able to reproduce historical trends in tropopause pressure obtained from reanalysis products. Simulated historical trends in cold point tropopause temperatures are not consistent across models or reanalyses. The pressure of both the tropical tropopause and the level of main convective outflow appear to have decreased (increased altitude) in historical runs as well as in reanalyses. Decreasing pressure trends in the tropical tropopause and level of main convective outflow are also seen in the future. Models consistently predict decreasing tropopause and convective outflow pressure, by several hPa/decade. Tropical cold point temperatures are projected to increase by 0.09 K/decade. Tropopause anomalies are highly correlated with tropical surface temperature anomalies and with tropopause level ozone anomalies, less so with stratospheric temperature anomalies. Simulated stratospheric water vapor at 90 hPa increases by up to 0.5–1 ppmv by 2100. The result is consistent with the simulated increase in temperature, highlighting the correlation of tropopause temperatures with stratospheric water vapor.
Evaluation of upper tropospheric humidity forecasts from ECMWF using AIRS and CALIPSO data
Authors: Lamquin N. , Gierens K. , Stubenrauch C. J. , Chatterjee R.
Published: April 2010

Abstract. An evaluation of the upper tropospheric humidity from the European Centre of Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS) is presented. We first make an analysis of the spinup behaviour of ice supersaturation in weather forecasts. It shows that a spinup period of at least 12 h is necessary before using forecast humidity data from the upper troposphere. We compare the forecasted upper tropospheric humidity with coincident relative humidity fields retrieved from the Atmospheric InfraRed Sounder (AIRS) and with cloud vertical profiles from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO). The analysis is made over one year, from October 2006 to September 2007, and we discuss how relative humidity and cloud features appear both in the IFS and in the observations. The comparison with AIRS is made difficult because of the vertical resolution of the sounder and the impossibility to retrieve humidity for high cloudiness. Clear sky relative humidities show a rather good correlation whereas cloudy situations reflect more the effect of a dry bias for AIRS increasing with the relative humidity. The comparison with CALIPSO shows that the IFS predicts high relative humidity where CALIPSO finds high clouds, which supports the good quality of the ECMWF upper tropospheric cloud forecast. In a last part, we investigate the presence of ice supersaturation within low vertical resolution pressure layers by comparing the IFS outputs for high-resolution and low-resolution humidity profiles and by simulating the interpolation of humidity over radiosonde data. A new correction method is proposed and tested with these data.
Homogeneous vs. heterogeneous nucleation in water-dicarboxylic acid systems
Authors: Hienola A. I. , Vehkamäki H. , Riipinen I. , Kulmala M.
Published: April 2010

Abstract. Binary heterogeneous nucleation of water-succinic/glutaric/malonic/adipic acid on nanometer-sized particles is investigated within the frame of classical heterogeneous nucleation theory. Homogeneous nucleation is also included for comparison. It is found that the nucleation probabilities depend on the contact angle and on the size of the seed particles. New thermodynamical properties, such as saturation vapor pressure, density and surface tension for all the dicarboxylic acid aqueous solutions are included in the calculations. While the new surface tension and density formulations do not bring any significant difference in the computed nucleation rate for homogeneous nucleation for succinic and glutaric acids, the use of the newly derived equations for the vapor pressure decrease the acid concentrations in gas phase by 3 orders of magnitude. According to our calculations, the binary heterogeneous nucleation of succinic acid-water and glutaric acid-water – although it requires a 3–4 orders of magnitude lower vapor concentrations than the homogeneous nucleation – cannot take place under atmospheric conditions. On the other hand binary homogeneous nucleation of adipic acid-water systems might be possible under conditions occuring in upper boundary layer. However, a more detailed characterization of the interaction between the surface and the molecules of the nucleating vapor should be considered in the future.