bluuebunny/crossref_metadata_2025 huggingface dataset:
Influence of entrainment of CCN on microphysical properties of warm cumulus
Authors: Derksen J. W. B. , Roelofs G.-J. H. , Röckmann T.
Published: April 2010

Abstract. We use a 1-D cloud model with explicit microphysics and a binned representation of the aerosol size distribution to investigate the influence of entrainment of cloud condensation nuclei (CCN) on the microphysical development of warm cumulus clouds. For a more realistic representation of cloud drop spectral width, the model separates droplets that grow on aerosol that is initially present in the cloud from droplets growing on entrained aerosol. Model results are compared with observations of trade wind cumulus microphysics from the Rain in Cumulus over the Ocean experiment (RICO, 2004–2005). The results indicate that CCN are entrained throughout the entire cloud depth, and inside the cloud part of these may be activated. Compared to a simulation where entrainment of ambient CCN is neglected this leads to higher cloud droplet number concentrations (CDNC) and a continuous presence of droplets in the range smaller than ~5 μm that is consistent with the observations. Cloud dynamics are sensitive to the entrainment parameter as well as to the applied initial vertical velocity, as expressed by the liquid water content and cloud top height. However, simulated cloud drop spectra remain relatively unaffected for the specific conditions during RICO.
Impact of prescribed SSTs on climatologies and long-term trends in CCM simulations
Authors: Garny H. , Dameris M. , Stenke A.
Published: April 2010

Abstract. Chemistry-Climate Model (CCM) simulations are commonly used to project the past and future development of the dynamics and chemistry of the stratosphere, and in particular the ozone layer. So far, CCMs are usually not interactively coupled to an ocean model, so that sea surface temperatures (SSTs) and sea ice coverage are prescribed in the simulations. While for future integrations SSTs have to be taken from precalculated climate model projections, for CCM experiments resembling the past either modelled or observed SSTs can be used. This study addresses the question to which extent atmospheric climatologies and long-term trends for the recent past simulated in the CCM E39C-A differ when choosing either observed or modelled SSTs. Furthermore, the processes of how the SST signal is communicated to the atmosphere, and in particular to the stratosphere are examined. Two simulations that differ only with respect to the prescribed SSTs and that span years 1960 to 1999 are used. Significant differences in temperature and ozone climatologies between the model simulations are found. The differences in ozone are attributed to differences in the meridional circulation, which are in turn driven by weaker wave forcing in the simulation with generally lower SSTs. The long-term trends over 40 years in annual mean temperature and ozone differ only in the troposphere, where temperatures are directly influenced by the local SST trends. Differences in temperature and ozone trends are only found on shorter time scales. The trends in tropical upwelling, as a measure of the strength of the Brewer-Dobson circulation (BDC), differ strongly between the simulations. A reverse from negative to positive trends is found in the late 1970s in the simulation using observed SSTs while trends are positive throughout the simulation when using modelled SSTs. The increase in the BDC is a robust feature of the simulations only after about 1980 and is evident mainly in the tropics in the lower stratosphere.
Monitoring of atmospheric composition using the thermal infrared IASI/MetOp sounder
Authors: Clerbaux C. , Boynard A. , Clarisse L. , George M. , Hadji-Lazaro J. , Herbin H. , Hurtmans D. , Pommier M. , Razavi A. , Turquety S. , Wespes C. , Coheur P.-F.
Published: April 2010

Abstract. Atmospheric remote sounding from satellites is an essential component of the observational strategy deployed to monitor atmospheric pollution and changing composition. The IASI nadir looking thermal infrared sounder onboard MetOp will provide 15 years of global scale observations for a series of key atmospheric species, with unprecedented spatial sampling and coverage. This paper gives an overview of the instrument's capability for measuring atmospheric composition in the perspective of chemistry and air quality. The assessment is made in terms of species, accuracy and vertical information. Global distributions are presented for CO, CH4, O3 (total and tropospheric), HNO3, NH3, and volcanic SO2. Local distributions of organic species measured during fire events, such as C2H4, CH3OH, HCOOH, and PAN are also shown. For each species or process, the link is made to specialized papers in this issue.
Evolution of stratospheric ozone and water vapour time series studied with satellite measurements
Authors: Jones A. , Urban J. , Murtagh D. P. , Eriksson P. , Brohede S. , Haley C. , Degenstein D. , Bourassa A. , von Savigny C. , Sonkaew T. , Rozanov A. , Bovensmann H. , Burrows J.
Published: April 2010

Abstract. The long term evolution of stratospheric ozone and water vapour has been investigated by extending satellite time series to April 2008. For ozone, we examine monthly average ozone values from various satellite data sets for nine latitude and altitude bins covering 60° S to 60° N and 20–45 km and covering the time period of 1979–2008. Data are from the Stratospheric Aerosol and Gas Experiment (SAGE I+II), the HALogen Occultation Experiment (HALOE), the Solar BackscatterUltraViolet-2 (SBUV/2) instrument, the Sub-Millimetre Radiometer (SMR), the Optical Spectrograph InfraRed Imager System (OSIRIS), and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartograpY (SCIAMACHY). Monthly ozone anomalies are calculated by utilising a linear regression model, which also models the solar, quasi-biennial oscillation (QBO), and seasonal cycle contributions. Individual instrument ozone anomalies are combined producing an all instrument average. Assuming a turning point of 1997 and that the all instrument average is represented by good instrumental long term stability, the largest statistically significant ozone declines (at two sigma) from 1979–1997 are seen at the mid-latitudes between 35 and 45 km, namely −7.2%±0.9%/decade in the Northern Hemisphere and −7.1%±0.9%/in the Southern Hemisphere. Furthermore, for the period 1997 to 2008 we find that the same locations show the largest ozone recovery (+1.4% and +0.8%/decade respectively) compared to other global regions, although the estimated trend model errors indicate that the trend estimates are not significantly different from a zero trend at the 2 sigma level. An all instrument average is also constructed from water vapour anomalies during 1991–2008, using the SAGE II, HALOE, SMR, and the Microwave Limb Sounder (Aura/MLS) measurements. We report that the decrease in water vapour values after 2001 slows down around 2004–2005 in the lower tropical stratosphere (20–25 km) and has even shown signs of increasing until present. We show that a similar correlation is also seen with the temperature measured at 100 hPa during this same period.
Effect of regional precursor emission controls on long-range ozone transport – Part 2: Steady-state changes in ozone air quality and impacts on human mortality
Authors: West J. J. , Naik V. , Horowitz L. W. , Fiore A. M.
Published: April 2010

Abstract. Large-scale changes in ozone precursor emissions affect ozone directly in the short term, and also affect methane, which in turn causes long-term changes in ozone that affect surface ozone air quality. Here we assess the effects of changes in ozone precursor emissions on the long-term change in surface ozone via methane, as a function of the emission region, by modeling 10% reductions in anthropogenic nitrogen oxide (NOx) emissions from each of nine world regions. Reductions in NOx emissions from all world regions increase methane and long-term surface ozone. While this long-term increase is small compared to the intra-regional short-term ozone decrease, it is comparable to or larger than the short-term inter-continental ozone decrease for some source-receptor pairs. The increase in methane and long-term surface ozone per ton of NOx reduced is greatest in tropical and Southern Hemisphere regions, exceeding that from temperate Northern Hemisphere regions by roughly a factor of ten. We also assess changes in premature ozone-related human mortality associated with regional precursor reductions and long-range transport, showing that for 10% regional NOx reductions, the strongest inter-regional influence is for emissions from Europe affecting mortalities in Africa. Reductions of NOx in North America, Europe, the Former Soviet Union, and Australia are shown to reduce more mortalities outside of the source regions than within. Among world regions, NOx reductions in India cause the greatest number of avoided mortalities per ton, mainly in India itself. Finally, by increasing global methane, NOx reductions in one hemisphere tend to cause long-term increases in ozone concentration and mortalities in the opposite hemisphere. Reducing emissions of methane, and to a lesser extent carbon monoxide and non-methane volatile organic compounds, alongside NOx reductions would avoid this disbenefit.
Factors controlling the distribution of ozone in the West African lower troposphere during the AMMA (African Monsoon Multidisciplinary Analysis) wet season campaign
Authors: Saunois M. , Reeves C. E. , Mari C. H. , Murphy J. G. , Stewart D. J. , Mills G. P. , Oram D. E. , Purvis R. M.
Published: April 2010

Abstract. Ozone and its precursors were measured on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 Atmospheric Research Aircraft during the monsoon season 2006 as part of the African Monsoon Multidisciplinary Analysis (AMMA) campaign. One of the main features observed in the west African boundary layer is the increase of the ozone mixing ratios from 25 ppbv over the forested area (south of 12° N) up to 40 ppbv over the Sahelian area. We employ a two-dimensional (latitudinal versus vertical) meteorological model coupled with an O3-NOx-VOC chemistry scheme to simulate the distribution of trace gases over West Africa during the monsoon season and to analyse the processes involved in the establishment of such a gradient. Including an additional source of NO over the Sahelian region to account for NO emitted by soils we simulate a mean NOx concentration of 0.7 ppbv at 16° N versus 0.3 ppbv over the vegetated region further south in reasonable agreement with the observations. As a consequence, ozone is photochemically produced with a rate of 0.25 ppbv h−1 over the vegetated region whilst it reaches up to 0.75 ppbv h−1 at 16° N. We find that the modelled gradient is due to a combination of enhanced deposition to vegetation, which decreases the ozone levels by up to 11 pbbv, and the aforementioned enhanced photochemical production north of 12° N. The peroxy radicals required for this enhanced production in the north come from the oxidation of background CO and CH4 as well as from VOCs. Sensitivity studies reveal that both the background CH4 and partially oxidised VOCs, produced from the oxidation of isoprene emitted from the vegetation in the south, contribute around 5–6 ppbv to the ozone gradient. These results suggest that the northward transport of trace gases by the monsoon flux, especially during nighttime, can have a significant, though secondary, role in determining the ozone gradient in the boundary layer. Convection, anthropogenic emissions and NO produced from lightning do not contribute to the establishment of the discussed ozone gradient.
Increasing surface ozone concentrations in the background atmosphere of Southern China, 1994–2007
Authors: Wang T. , Wei X. L. , Ding A. J. , Poon C. N. , Lam K. S. , Li Y. S. , Chan L. Y. , Anson M.
Published: April 2010

Abstract. Tropospheric ozone is of great importance with regard to air quality, atmospheric chemistry, and climate change. In this paper we report the first continuous record of surface ozone in the background atmosphere of South China. The data were obtained from 1994 to 2007 at a coastal site in Hong Kong, which is strongly influenced by the outflow of Asian continental air during the winter and the inflow of maritime air from the subtropics in the summer. Three methods are used to derive the rate of change in ozone. A linear fit to the 14-year record shows that the ozone concentration increased by 0.58 ppbv/yr, whereas comparing means in years 1994–2000 and 2001–2007 gives an increase of 0.87 ppbv/yr for a 7-year period. The ozone changes in air masses from various source regions are also examined. Using local wind and carbon monoxide (CO) data to filter out local influence, we find that ozone increased by 0.94 ppbv/yr from 1994–2000 to 2001–2007 in air masses from Eastern China, with similar changes in the other two continent-influenced air-mass groups, but no statistically significant change in the marine air. An examination of the nitrogen dioxide (NO2) column obtained from GOME and SCIAMACHY reveals an increase in atmospheric NO2 in China's three fastest developing coastal regions, whereas NO2 in other parts of Asia decreased during the same period, and no obvious trend over the main shipping routes in the South China Sea was indicated. Thus the observed increase in background ozone in Hong Kong is most likely due to the increased emissions of NO2 (and possibly volatile organic compounds (VOCs) as well) in the upwind coastal regions of mainland China. The CO data at Hok Tsui showed less definitive changes compared to the satellite NO2 column. The increase in background ozone likely made a strong contribution (81%) to the rate of increase in "total ozone" at an urban site in Hong Kong, suggesting the need to consider distant sources when developing long-term strategies to mitigate local ozone pollution.
Factors controlling contrail cirrus optical depth
Authors: Kärcher B. , Burkhardt U. , Unterstrasser S. , Minnis P.
Published: April 2010

Abstract. Aircraft contrails develop into contrail cirrus by depositional growth and sedimentation of ice particles and horizontal spreading due to wind shear. Factors controlling this development include temperature, ice supersaturation, thickness of ice-supersaturated layers, and vertical gradients in the horizontal wind field. An analytical microphysical cloud model is presented and validated that captures these processes. Many individual contrail cirrus are simulated that develop differently owing to the variability in the controlling factors, resulting in large samples of cloud properties that are statistically analyzed. Contrail cirrus development is studied over the first four hours past formation, similar to the ages of line-shaped contrails that were tracked in satellite imagery on regional scales. On these time scales, contrail cirrus optical depth and microphysical variables exhibit a marked variability, expressed in terms of broad and skewed probability distribution functions. Simulated mean optical depths at a wavelength of 0.55 μm range from 0.05-0.5 and a substantial fraction 20-50% of contrail cirrus stay subvisible (optical depth <0.02), depending on meteorological conditions. A detailed analysis based on an observational case study over the continental USA suggests that previous satellite measurements of line-shaped persistent contrails have missed about 89%, 50%, and 11% of contrails with optical depths 0-0.05, 0.05-0.1, and 0.1-0.2, respectively, amounting to 65% of contrail coverage of all optical depths. When comparing observations with simulations and when estimating the contrail cirrus climate impact, not only mean values but also the variability in optical depth and microphysical properties need to be considered.
Comparative study of the effect of water on the heterogeneous reactions of carbonyl sulfide on the surface of α-Al2O3 and MgO
Authors: Liu Y. , Ma Q. , He H.
Published: April 2010

Abstract. Here we compared the heterogeneous reactions of carbonyl sulfide (OCS) on the surface of α-Al2O3 and MgO and the effect of water on the reactions at 300 K using Knudsen cell–mass spectrometry, diffuse reflectance infrared Fourier transform spectroscopy, and temperature programmed reactions. H2S and CO2 were found to be hydrolysis products of OCS on both α–Al2O3 and MgO at ambient temperature. At low water vapor pressure (<6.8×10−6 Torr), when water vapor pressure in the Knudsen cell reactor increased from 2.3×10−6 to 6.8×10−6 Torr, the initial true uptake coefficient of OCS on α-Al2O3 decreased from 4.70±0.45×10−7 to 3.59±0.34×10−7; while it increased from 5.19±0.49×10−7 to 6.48±0.62×10−7 on MgO under the same conditions. At high relative humidity (0.07–0.67), the observed uptake coefficients of OCS on α-Al2O3 and MgO, which were measured using an in situ DRIFTS, decreased from 4.63±0.22×10−6 to 1.00±0.47×10−6 and from 9.72±0.46×10−5 to 7.68±0.36×10−5, respectively, when RH increased from 0.07 to 0.67 corresponding to 1.7–15.9 Torr of water vapor pressure. In the RH region of 0.17–0.67, the average observed uptake coefficient of OCS on α-Al2O3 and MgO was equal to 8.34±2.19×10−7 and 8.19±0.48×10−5, respectively. The restrictive effect of water on the heterogeneous reaction of OCS on the surface of α-Al2O3 and MgO was found to be related to competitive adsorption between water and OCS molecules; while the promotive effect of water on the heterogeneous reaction of OCS on the surface of MgO at low coverage was ascribed to the formation of surface hydroxyl groups. When the environmental RH was greater than the RH of the monolayer, which occurred readily at the atmospherically relevant humidity in the troposphere, thick water layer formed on the mineral dusts, especially, the basic thick water layer formed on the basic component of mineral dusts may be the primary contributor to the heterogeneous hydrolysis of OCS in the troposphere.
Evaluation of mobile emissions contributions to Mexico City's emissions inventory using on-road and cross-road emission measurements and ambient data
Authors: Zavala M. , Herndon S. C. , Wood E. C. , Onasch T. B. , Knighton W. B. , Marr L. C. , Kolb C. E. , Molina L. T.
Published: April 2010

Abstract. Mobile emissions represent a significant fraction of the total anthropogenic emissions burden in the Mexico City Metropolitan Area (MCMA) and, therefore, it is crucial to use top-down techniques informed by on-road exhaust measurements to evaluate and improve traditional bottom-up official emissions inventory (EI) for the city. We present the measurements of on-road fleet-average emission factors obtained using the Aerodyne mobile laboratory in the MCMA in March 2006 as part of the MILAGRO/MCMA-2006 field campaign. A comparison of our on-road emission measurements with those obtained in 2003 using essentially the same measurement techniques and analysis methods indicates that, in the three year span, NO emission factors remain within the measured variability ranges whereas emission factors of aldehydes and aromatics species were reduced for all sampled driving conditions. We use a top-down fuel-based approach to evaluate the mobile emissions from the gasoline fleet estimated in the bottom-up official 2006 MCMA mobile sources. Within the range of measurement uncertainties, we found probable slight overpredictions of mean EI estimates on the order of 20–28% for CO and 14–20% for NO. However, we identify a probable EI discrepancy of VOC mobile emissions between 1.4 and 1.9; although estimated benzene and toluene mobile emissions in the inventory seem to be well within the uncertainties of the corresponding emissions estimates. Aldehydes mobile emissions in the inventory, however, seem to be underpredicted by factors of 3 for HCHO and 2 for CH3CHO. Our on-road measurement-based estimate of annual emissions of organic mass from PM1 particles suggests a severe underprediction (larger than a factor of 4) of PM2.5 mobile emissions in the inventory. Analyses of ambient CO, NOx and CO/NOx concentration trends in the MCMA indicate that the early morning ambient CO/NOx ratio has decreased at a rate of about 1.9 ppm/ppm/year over the last two decades due to reductions in CO levels rather than by NOx. These trends, together with the analysis of fuel sales and fleet size, suggest that the relative contribution of diesel vehicles to overall NOx levels has increased over time in the city. Despite the impressive increase in the size of the vehicle fleet between 2000 and 2006, the early morning ambient concentrations of CO and NOx have not increased accordingly, probably due to the reported low removal rates of older vehicles, which do not have emissions control technologies, and partially due to the much lower emissions from newer gasoline vehicles. This indicates that an emission-based air quality improvement strategy targeting large reductions of emissions from mobile sources should be directed towards a significant increase of the removal rate of older, highly-polluting, vehicles.
Gas phase precursors to anthropogenic secondary organic aerosol: detailed observations of 1,3,5-trimethylbenzene photooxidation
Authors: Wyche K. P. , Monks P. S. , Ellis A. M. , Cordell R. L. , Parker A. E. , Whyte C. , Metzger A. , Dommen J. , Duplissy J. , Prevot A. S. H. , Baltensperger U. , Rickard A. R. , Wulfert F.
Published: April 2010

Abstract. A series of photooxidation experiments were conducted in an atmospheric simulation chamber in order to investigate the oxidation mechanism and secondary organic aerosol (SOA) formation potential of the model anthropogenic gas phase precursor, 1,3,5-trimethylbenzene. Alongside specific aerosol measurements, comprehensive gas phase measurements, primarily by Chemical Ionisation Reaction Time-of-Flight Mass Spectrometry (CIR-TOF-MS), were carried out to provide detailed insight into the composition and behaviour of the organic components of the gas phase matrix during SOA formation. An array of gas phase organic compounds was measured during the oxidation process, including several previously unmeasured primary bicyclic compounds possessing various functional groups. Analysis of results obtained during this study implies that these peroxide bicyclic species along with a series of ring opening products and organic acids contribute to SOA growth. The effect of varying the VOC/NOx ratio on SOA formation was explored, as was the effect of acid seeding. It was found that low NOx conditions favour more rapid aerosol formation and a higher aerosol yield, a result that implies a role for organic peroxides in the nucleation process and SOA growth.
The two-day wave in the Antarctic and Arctic mesosphere and lower thermosphere
Authors: Tunbridge V. M. , Mitchell N. J.
Published: April 2010

Abstract. There have been comparatively few studies reported of the 2-day planetary wave in the middle atmosphere at polar latitudes. Here we report on a study made using high-latitude meteor radars at Rothera in the Antarctic (68° S, 68° W) and Esrange in Arctic Sweden (68° N, 21° E). Observations from 2005–2008 are used for Rothera and from 1999–2008 for Esrange. Measurements were made of horizontal winds at heights of 80–100 km. The radar data revealed distinct summertime and wintertime 2-day waves. The Antarctic summertime wave occurs with significant amplitudes in January – February at heights between about 88–100 km. Horizontal wind monthly variances associated with the wave exceed 160 m2 s−2 and the zonal component has larger amplitudes than the meridional. In contrast, the Arctic summertime wave occurs for a longer duration, June–August and has meridional amplitudes larger than the zonal amplitudes. The Arctic summertime wave is weaker than that in the Antarctic and maximum monthly variances are typically 60 m2 s−2. In both hemispheres the summertime wave reaches largest amplitudes in the strongly sheared eastward zonal flow above the zero-wind line and is largely absent in the westward flow below. The observed differences in the summertime wave are probably due to the differences in the background zonal winds in the two hemispheres. The Antarctic and Arctic wintertime 2-day waves have very similar behaviour. The Antarctic wave has significant amplitudes in May–August and the Arctic wave in November–February. Both are evident across the full height range observed.
Impact of tropospheric nitrogen dioxide on the regional radiation budget
Authors: Vasilkov A. P. , Joiner J. , Oreopoulos L. , Gleason J. F. , Veefkind P. , Bucsela E. , Celarier E. A. , Spurr R. J. D. , Platnick S.
Published: April 2010

Abstract. Following the launch of several satellite ultraviolet and visible spectrometers including the Ozone Monitoring Instrument (OMI), much has been learned about the global distribution of nitrogen dioxide (NO2). NO2, which is mostly anthropogenic in origin, absorbs solar radiation at ultraviolet and visible wavelengths. We parameterized NO2 absorption for fast radiative transfer calculations. Using this parameterization with cloud, surface, and NO2 information from different sensors in the NASA A-train constellation of satellites and NO2 profiles from the Global Modeling Initiative (GMI), we compute the global distribution of net atmospheric heating (NAH) due to tropospheric NO2 for January and July 2005. The globally-averaged NAH values due to tropospheric NO2 are very low: they are about 0.05 W/m2. While the impact of NO2 on the global radiative forcing is small, locally it can produce instantaneous net atmospheric heating of 2–4 W/m2 in heavily polluted areas. We assess the impact of clouds and find that they reduce the globally-averaged NAH values by 5–6% only. However, because most of NO2 is contained in the boundary layer in polluted regions, the cloud shielding effect can significantly reduce the net atmospheric heating due to tropospheric NO2 (up to 50%). We examine the effect of diurnal variations in NO2 emissions and chemistry on net atmospheric heating and find only a small impact of these on the daily-averaged heating (11–14% at the most). We also examine the sensitivity of NO2 absorption to various geophysical conditions. Effects of the vertical distributions of cloud optical depth and NO2 on net atmospheric heating and downwelling radiance are simulated in detail for various scenarios including vertically-inhomogeneous convective clouds observed by CloudSat. The maximum effect of NO2 on downwelling radiance occurs when the NO2 is located in the middle part of the cloud where the optical extinction peaks.
Observations of high rates of NO2-HONO conversion in the nocturnal atmospheric boundary layer in Kathmandu, Nepal
Authors: Yu Y. , Galle B. , Panday A. , Hodson E. , Prinn R. , Wang S.
Published: April 2010

Abstract. Nitrous acid (HONO) plays a significant role in the atmosphere, especially in the polluted troposphere. Its photolysis after sunrise is an important source of hydroxyl free radicals (OH). Measurements of nitrous acid and other pollutants were carried out in the Kathmandu urban atmosphere during January–February 2003, contributing to the sparse knowledge of nitrous acid in South Asia. The results showed average nocturnal levels of HONO (1.7±0.8 ppbv), NO2 (17.9±10.2 ppbv), and PM10 (0.18±0.11 mg m−3) in urban air in Kathmandu. Surprisingly high ratios of chemically formed secondary [HONO] to [NO2] (up to 30%) were found, which indicates unexpectedly efficient chemical conversion of NO2 to HONO in Kathmandu. The ratios of [HONO]/[NO2] at night were found to be much higher than previously reported values from measurements in urban air in Europe, North America and Asia. The influences of aerosol surface, ground reactive surface, and relative humidity on NO2-HONO chemical conversion were discussed. The high humidity, strong and low inversion layer at night, and high aerosol pollution burden in Kathmandu may explain the particularly efficient conversion of NO2 to HONO.
Technical Note: Determination of aerosol optical properties by a calibrated sky imager
Authors: Cazorla A. , Shields J. E. , Karr M. E. , Olmo F. J. , Burden A. , Alados-Arboledas L.
Published: April 2010

Abstract. The calibrated ground-based sky imager developed in the Marine Physical Laboratory, the Whole Sky Imager (WSI), has been tested with data from the Atmospheric Radiation Measurement Program (ARM) at the Southern Great Plain site (SGP) to determine optical properties of the atmospheric aerosol. Different neural network-based models calculate the aerosol optical depth (AOD) for three wavelengths using the radiance extracted from the principal plane of sky images from the WSI as input parameters. The models use data from a CIMEL CE318 photometer for training and validation and the wavelengths used correspond to the closest wavelengths in both instruments. The spectral dependency of the AOD, characterized by the Ångström exponent α in the interval 440–870 nm, is also derived using the standard AERONET procedure and also with a neural network-based model using the values obtained with a CIMEL CE318. The deviations between the WSI derived AOD and the AOD retrieved by AERONET are within the nominal uncertainty assigned to the AERONET AOD calculation (±0.01), in 80% of the cases. The explanation of data variance by the model is over 92% in all cases. In the case of α, the deviation is within the uncertainty assigned to the AERONET α (±0.1) in 50% of the cases for the standard method and 84% for the neural network-based model. The explanation of data variance by the model is 63% for the standard method and 77% for the neural network-based model.
A model study of the January 2006 low total ozone episode over Western Europe and comparison with ozone sonde data
Authors: Mangold A. , Grooß J.-U. , De Backer H. , Kirner O. , Ruhnke R. , Müller R.
Published: April 2010

Abstract. Total column and stratospheric ozone levels at mid-latitudes often reveal strong fluctuations on time scales of days caused by dynamic processes. In some cases the total ozone column is distinctly reduced below climatological values. Here, a very low total ozone episode around 19 January 2006 over Western Europe is investigated when the observed total ozone column over Uccle (BE), measured by a Brewer spectrophotometer, reached a daily minimum of 200 DU, the lowest recorded value at this station. In order to investigate the mechanisms leading to the ozone minimum, the present study used data from (i) six ozone sounding stations in Western and Middle Europe, (ii) ECMWF meteorological fields, (iii) a simulation of the CLaMS model for January 2006, (iv) a multi-year run of the chemistry transport model KASIMA, and (v) a six-year run of the climate chemistry model ECHAM5/MESSy1. The ozone decrease at different heights was quantified and it was determined to what extent different transport mechanisms, and instantaneous, in-situ chemical ozone depletion contributed to the event. All three models reproduced the evolution and formation of the event. The ozone column decrease between Θ=300 and 750 K was strongest at Uccle (BE) and De Bilt (NL) with 108 and 103 DU, respectively, and somewhat lower at Hohenpeissenberg (DE), Payerne (CH), Prague (CZ) and Lerwick (UK) with 85, 84, 83 and 74 DU, respectively. This analysis demonstrated that mainly the displacement of the ozone depleted polar vortex contributed to the ozone column decrease. Advection of ozone-poor low-latitude air masses was important in the UTLS region. The vertical displacement of isentropes connected with divergence of air out of the column was found to be of minor importance compared to the horizontal transport processes. Severe low total ozone episodes seem to occur when the mentioned mechanisms are superimposed. Instantaneous, in-situ chemical ozone depletion accounted for only 2±1% of the overall total ozone decrease at the sounding stations.
IASI temperature and water vapor retrievals – error assessment and validation
Authors: Pougatchev N. , August T. , Calbet X. , Hultberg T. , Oduleye O. , Schlüssel P. , Stiller B. , Germain K. St. , Bingham G.
Published: April 2010

Abstract. The METOP-A satellite Infrared Atmospheric Sounding Interferometer (IASI) Level 2 products comprise retrievals of vertical profiles of temperature and water vapor. The error covariance matrices and biases of the most recent version (4.3.1) of the L2 data were assessed, and the assessment was validated using radiosonde data for reference. The radiosonde data set includes dedicated and synoptic time launches at the Lindenberg station in Germany. For optimal validation, the linear statistical Validation Assessment Model (VAM) was used. The VAM uses radiosonde profiles as input and provides optimal estimate of the nominal IASI retrieval by utilizing IASI averaging kernels and statistical characteristics of the ensembles of the reference radiosondes. For temperatures above 900 mb and water retrievals above 700 mb, level expected and assessed errors are in good agreement. Below those levels, noticeable excess in assessed error is observed, possibly due to inaccurate surface parameters and undetected clouds/haze.
Source regions of some persistent organic pollutants measured in the atmosphere at Birkenes, Norway
Authors: Eckhardt S. , Breivik K. , Li Y. F. , Manø S. , Stohl A.
Published: April 2010

Abstract. A key feature of POPs (Persistent Organic Pollutants) is their potential for long-range atmospheric transport. In order to better understand and predict atmospheric source-receptor relationships of POPs, we have modified an existing Lagrangian transport model (FLEXPART) to include some of the key processes that control the atmospheric fate of POPs. We also present four years (2004–2007) of new atmospheric measurement data for polychlorinated biphenyls (PCBs) and hexachlorocyclohexanes (HCHs) obtained at Birkenes, an EMEP (European Monitoring and Evaluation Programme) site in southern Norway. The model overestimates measured PCB-28 and γ-HCH concentrations by factors of 2 and 8, respectively, which is most likely because the emissions used as input to the model are overestimated. FLEXPART captures the temporal variability in the measurements very well and, depending on season, explains 31–67% (14–62%) of the variance of measured PCB-28 (γ-HCH) concentrations. FLEXPART, run in a time-reversed (adjoint) mode, was used to identify the source regions responsible for the POP loading at the Birkenes station. Emissions in Central Europe and Eastern Europe contributed 32% and 24%, respectively, to PCB-28 at Birkenes, while Western Europe was found to be the dominant source (50%) for γ-HCH. Intercontinental transport from North America contributed 13% γ-HCH. While FLEXPART has no treatment of the partitioning of POPs between different surface media, it was found a very useful tool for studying atmospheric source-receptor relationships for POPs and POP-like chemicals that do not sorb strongly to atmospheric particles and whose atmospheric levels are believed to be mainly controlled by primary sources.
Intercomparison of integrated IASI and AATSR calibrated radiances at 11 and 12 μm
Authors: Illingworth S. M. , Remedios J. J. , Parker R. J.
Published: April 2010

Abstract. The mission objectives of the Infrared Atmospheric Sounding Interferometer (IASI) are driven by the needs of the Numerical Weather Prediction (NWP) and climate monitoring communities. These objectives rely upon the IASI instrument being able to measure top of atmosphere radiances accurately. This paper presents a technique and first results for the validation of the radiometric calibration of radiances for IASI, using a cross-calibration with the Advanced Along Track Scanning Radiometer (AATSR). The AATSR is able to measure Brightness Temperature (BT) to an accuracy of 30 mK, and by applying the AATSR spectral filter functions to the IASI measured radiances we are able to compare AATSR and IASI Brightness Temperatures. By choosing coincident data points that are over the sea and in clear sky conditions, a threshold of homogeneity is derived. It is found that in these homogenous conditions, the IASI BTs agree with those measured by the AATSR to within 0.3 K, with an uncertainty of order 0.1 K. The agreement is particularly good at 11 μm where the difference is less than 0.1 K. These first results indicate that IASI is meeting its target objective of 0.5 K accuracy. It is believed that a refinement of the AATSR spectral filter functions will hopefully permit a tighter error constraint on the quality of the IASI data and hence further assessment of the climate quality of the radiances.
Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B
Authors: Shinozuka Y. , Clarke A. D. , DeCarlo P. F. , Jimenez J. L. , Dunlea E. J. , Roberts G. C. , Tomlinson J. M. , Collins D. R. , Howell S. G. , Kapustin V. N. , McNaughton C. S. , Zhou J.
Published: April 2010

Abstract. Remote sensing of cloud condensation nuclei (CCN) would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100 nm particles decreased with increasing organic fraction of non-refractory mass of submicron particles (OMF) as 0.34–0.20×OMF over Central Mexico and 0.47–0.43×OMF over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(−1/3), within measurement uncertainty (~20%). The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0–0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as −0.70×OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust). Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemical composition and CCN activity over Central Mexico.
Scaling behaviour of the global tropopause
Authors: Varotsos C. , Efstathiou M. , Tzanis C.
Published: April 2010

Abstract. Detrended fluctuation analysis is applied to the time series of the global tropopause height derived from the 1980–2004 daily radiosonde data, in order to detect long-range correlations in its time evolution. Global tropopause height fluctuations in small time-intervals are found to be positively correlated to those in larger time intervals in a power-law fashion. The exponent of this dependence is larger in the tropics than in the middle and high latitudes in both hemispheres. Greater persistence is observed in the tropopause of the Northern than in the Southern Hemisphere. A plausible physical explanation of the fact that long-range correlations in tropopause variability decreases with increasing latitude is that the column ozone fluctuations (that are closely related with the tropopause ones) exhibit long range correlations, which are larger in tropics than in the middle and high latitudes at long time scales. This finding for the tropopause height variability should reduce the existing uncertainties in assessing the climatic characteristics. More specifically the reliably modelled values of a climatic variable (i.e. past and future simulations) must exhibit the same scaling behaviour with that possibly existing in the real observations of the variable under consideration. An effort has been made to this end by applying the detrended fluctuation analysis to the global mean monthly land and sea surface temperature anomalies during the period January 1850–August 2008. The result obtained supports the findings presented above, notably: the correlations between the fluctuations in the global mean monthly land and sea surface temperature display scaling behaviour which must characterizes any projection.
Oxygenated organic functional groups and their sources in single and submicron organic particles in MILAGRO 2006 campaign
Authors: Liu S. , Takahama S. , Russell L. M. , Gilardoni S. , Baumgardner D.
Published: April 2010

Abstract. Fourier Transform Infrared (FTIR) and X-ray Fluorescence (XRF) were used to measure organic functional groups and elements of submicron particles collected during MILAGRO in March 2006 on three platforms: the Mexico City urban area (SIMAT), the high altitude site at 4010 m (Altzomoni), and the NCAR C130 aircraft. Scanning Transmission X-ray Microscopy (STXM) and Near-Edge X-ray Absorption Fine Structure (NEXAFS) were applied to single particle organic functional group abundance analysis of particles simultaneously collected at SIMAT and C130. Correlations of elemental concentrations showed different groups of source-related elements at SIMAT, Altzomoni, and C130, suggesting different processes affecting the air masses sampled at the three platforms. Cluster analysis resulted in seven distinct clusters of FTIR spectra, with the last three clusters consisting of spectra collected almost exclusively on the C130 platform, reflecting the variety of sources contributing to C130 samples. Positive Matrix Factorization (PMF) of STXM-NEXAFS spectra identified three main factors representing soot, secondary, and biomass burning type spectra. PMF of FTIR spectra resulted in two fossil fuel combustion factors and one biomass burning factor, the former representative of source regions to the northeast and southwest of SIMAT. Alkane, carboxylic acid, amine, and alcohol functional groups were mainly associated with combustion related sources, while non-acid carbonyl groups were likely from biomass burning events. The majority of OM and O/C was attributed to combustion sources, although no distinction between direct emissions and atmospherically processed OM could be identified.
Modelling of cirrus clouds – Part 1a: Model description and validation
Authors: Spichtinger P. , Gierens K. M.
Published: April 2010

Abstract. A double-moment bulk microphysics scheme for modelling cirrus clouds including explicit impact of aerosols on different types of nucleation mechanism is described. Process rates are formulated in terms of generalised moments of the underlying a priori size distributions in order to allow simple switching between various distribution types. The scheme has been implemented into a simple box model and into the anelastic non-hydrostatic model EULAG. The new microphysics is validated against simulations with detailed microphysics for idealised process studies and for a well documented case of arctic cirrostratus. Additionally, the formation of ice crystals with realistic background aerosol concentration is modelled and the effect of ambient pressure on homogeneous nucleation is investigated in the box model. The model stands all tests and is thus suitable for cloud-resolving simulations of cirrus clouds.
Aerosol- and updraft-limited regimes of cloud droplet formation: influence of particle number, size and hygroscopicity on the activation of cloud condensation nuclei (CCN)
Authors: Reutter P. , Su H. , Trentmann J. , Simmel M. , Rose D. , Gunthe S. S. , Wernli H. , Andreae M. O. , Pöschl U.
Published: April 2010

Abstract. We have investigated the formation of cloud droplets under pyro-convective conditions using a cloud parcel model with detailed spectral microphysics and with the κ-Köhler model approach for efficient and realistic description of the cloud condensation nucleus (CCN) activity of aerosol particles. Assuming a typical biomass burning aerosol size distribution (accumulation mode centred at 120 nm), we have calculated initial cloud droplet number concentrations (NCD) for a wide range of updraft velocities (w=0.25–20 m s−1) and aerosol particle number concentrations (NCN=200–105 cm−3) at the cloud base. Depending on the ratio between updraft velocity and particle number concentration (w/NCN), we found three distinctly different regimes of CCN activation and cloud droplet formation: (1) An aerosol-limited regime that is characterized by high w/NCN ratios (>≈10−3 m s−1 cm3), high maximum values of water vapour supersaturation (Smax>≈0.5%), and high activated fractions of aerosol particles (NCN/NCN>≈90%). In this regime NCD is directly proportional to NCN and practically independent of w. (2) An updraft-limited regime that is characterized by low w/NCN ratios (
Cloud processing, cloud evaporation and Angström exponent
Authors: Roelofs G.-J. , Kamphuis V.
Published: April 2010

Abstract. With a cloud parcel model we investigate how cloud processing and cloud evaporation modify the size distribution and the Angström exponent of an aerosol population. Our study provides a new explanation for the observed variability of the aerosol optical thickness and Angström exponent in the vicinity of clouds. Cloud processing causes a decrease of aerosol particle concentrations, relatively most efficiently in the coarse mode, and reduces the relative dispersion of the aerosol distribution. As a result the Angström exponent of the aerosol increases. The Angström exponent is very sensitive for changes in relative humidity during cloud evaporation, especially between 90% and 100%. In addition, kinetic limitations delay evaporation of relatively large cloud drops, especially in clean and mildly polluted environments where the coarse mode fraction is relatively large. This hampers a direct relation between the aerosol optical thickness, the Angström exponent and the ambient relative humidity, which may severely complicate interpretation of these parameters in terms of aerosol properties, such as the fine mode fraction.
Regional modelling of tracer transport by tropical convection – Part 2: Sensitivity to model resolutions
Authors: Arteta J. , Marécal V. , Rivière E. D.
Published: April 2010

Abstract. The general objective of this series of two papers is to evaluate long duration limited-area simulations with idealised tracers as a possible tool to assess the tracer transport in chemistry-transport models (CTMs). In this second paper we analyse the results of three simulations using different horizontal and vertical resolutions. The goal is to study the impact of the model spatial resolution on convective transport of idealized tracer in the tropics. The reference simulation (REF) uses a 60 km horizontal resolution and 300 m vertically in the upper troposphere/lower stratosphere (UTLS). A 20 km horizontal resolution simulation (HR) is run as well as a simulation with 850 m vertical resolution in the UTLS (CVR). The simulations are run for one month during the SCOUT-O3 field campaign. Aircraft data, TRMM rainrate estimates and radiosoundings have been used to evaluate the simulations. They show that the HR configuration gives generally a better agreement with the measurements than the REF simulation. The CVR simulation gives generally the worst results. The vertical distribution of the tropospheric tracers for the simulations has a similar shape with a ~15 km altitude maximum for the 6h-lifetime tracer of 0.4 ppbv for REF, 1.2 for HR and 0.04 for CVR. These differences are related to the dynamics produced by the three simulations that leads to larger values of the upward velocities on average for HR and lower for CVR compared to REF. HR simulates more frequent and stronger convection leading to enhanced fluxes compared to REF and higher detrainment levels compared to CVR. HR provides also occasional overshoots over the cold point dynamical barrier. For the stratospheric tracers the differences between the three simulations are small. The diurnal cycle of the fluxes of all tracers in the Tropical Tropopause Layer exhibits a maximum linked to the maximum of convective activity.