bluuebunny/crossref_metadata_2025 huggingface dataset:
The ASSET intercomparison of stratosphere and lower mesosphere humidity analyses
Authors: Thornton H. E. , Jackson D. R. , Bekki S. , Bormann N. , Errera Q. , Geer A. J. , Lahoz W. A. , Rharmili S.
Published: April 2010

Abstract. This paper presents results from the first detailed intercomparison of stratosphere-lower mesosphere water vapour analyses; it builds on earlier results from the EU funded framework V "Assimilation of ENVISAT Data" (ASSET) project. Stratospheric water vapour plays an important role in many key atmospheric processes and therefore an improved understanding of its daily variability is desirable. With the availability of high resolution, good quality Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) water vapour profiles, the ability of four different atmospheric models to assimilate these data is tested. MIPAS data have been assimilated over September 2003 into the models of the European Centre for Medium Range Weather Forecasts (ECMWF), the Belgian Institute for Space and Aeronomy (BIRA-IASB), the French Service d'Aéronomie (SA-IPSL) and the UK Met Office. The resultant middle atmosphere humidity analyses are compared against independent satellite data from the Halogen Occultation Experiment (HALOE), the Polar Ozone and Aerosol Measurement (POAM III) and the Stratospheric Aerosol and Gas Experiment (SAGE II). The MIPAS water vapour profiles are generally well assimilated in the ECMWF, BIRA-IASB and SA systems, producing stratosphere-mesosphere water vapour fields where the main features compare favourably with the independent observations. However, the models are less capable of assimilating the MIPAS data where water vapour values are locally extreme or in regions of strong humidity gradients, such as the southern hemisphere lower stratosphere polar vortex. Differences in the analyses can be attributed to the choice of humidity control variable, how the background error covariance matrix is generated, the model resolution and its complexity, the degree of quality control of the observations and the use of observations near the model boundaries. Due to the poor performance of the Met Office analyses the results are not included in the intercomparison, but are discussed separately. The Met Office results highlight the pitfalls in humidity assimilation, and provide lessons that should be learnt by developers of stratospheric humidity assimilation systems. In particular, they underline the importance of the background error covariances in generating a realistic troposphere to mesosphere water vapour analysis.
Nitrous oxide emissions from the Arabian Sea: A synthesis
Authors: Bange H. W. , Andreae M. O. , Lal S. , Law C. S. , Naqvi S. W. A. , Patra P. K. , Rixen T. , Upstill-Goddard R. C.
Published: April 2010

Abstract. We computed high-resolution (1o latitude × 1o longitude) seasonal and annual nitrous oxide (N2O) concentration fields for the Arabian Sea surface layer using a database containing more than 2400 values measured between December 1977 and July 1997. N2O concentrations are highest during the southwest (SW) monsoon along the southern Indian continental shelf. Annual emissions range from 0.33 to 0.70 Tg N2O and are dominated by fluxes from coastal regions during the SW and northeast monsoons. However, the tendency to focus on measurements in locally restricted features in combination with insufficient seasonal data coverage leads to considerable uncertainties of the concentration fields and thus in the flux estimates, especially in the coastal zones of the northern and eastern Arabian Sea.
Field measurements of hygroscopic properties and state of mixing of nucleation mode particles
Authors: Väkevä M. , Kulmala M. , Stratmann F. , Hämeri K.
Published: April 2010

Abstract. An Ultrafine Tandem Differential Mobility Analyser (UF-TDMA) has been used in several field campaigns over the last few years. The investigations were focused on the origin and properties of nucleation event aerosols, which are observed frequently in various environments. This paper gives a summary of the results of 10 nm and 20 nm particle hygroscopic properties from different measurement sites: an urban site, an urban background site and a forest site in Finland and a coastal site in western Ireland. The data can be classified in four hygroscopic growth classes: hydrofobic, less-hygroscopic, more-hygroscopic and sea-salt. Similar classification has been earlier presented for Aitken and accumulation mode particles. In urban air, the summertime 10 nm particles showed varying less-hygroscopic growth behaviour, while winter time 10 nm and 20 nm particles were externally mixed with two different hygroscopic growth modes. The forest measurements revealed diurnal behaviour of hygroscopic growth, with high growth factors at day time and lower during night. The urban background particles had growth behaviour similar to the urban and forest measurement sites depending on the origin of the observed particles. The coastal measurements were strongly affected by air mass history. Both 10 nm and 20 nm particles were hygroscopic in marine background air. The 10 nm particles produced during clean nucleation burst periods were hydrofobic. Diurnal variation and higher growth factors of 10 nm particles were observed in air affected by other source regions. External mixing was occasionally observed at all the sites, but incidents with more than two growth modes were extremely rare.
Oxidation of SO2 by H2O2 on ice surfaces at 228 K: a sink for SO2 in ice clouds
Authors: Clegg S. M. , Abbatt J. P. D.
Published: April 2010

Abstract. The heterogeneous reaction SO2 + H2O2 to H2SO4 on ice at 228 K has been studied in a low temperature coated-wall flow tube. With H2O2 in excess of SO2, the loss of SO2 on an ice surface is time dependent with the reaction most efficient on a freshly exposed surface. The deactivation of the surface arises because the protons formed in the reaction inhibit the dissociation of adsorbed SO2. This lowers the surface concentrations of HSO3-, a participant in the rate-determining step of the oxidation mechanism. For a fixed SO2 partial pressure of 1.4 × 10-4 Pa, the reaction probabilities for SO2 loss on a freshly exposed surface scale linearly with H2O2 partial pressures between 2.7 × 10-3 and 2.7 × 10-2 Pa because the H2O2 surface coverage is unsaturated in this regime. Conversely, the reaction probabilities decrease as the partial pressure of SO2 is raised from 2.7 × 10-5 to 1.3 × 10-3 Pa, for a fixed H2O2 partial pressure of 8.7 × 10-3 Pa. This is expected if the rate determining step for the mechanism involves HSO3- rather than SO2. It may also arise to some degree if there is competition between gas phase SO2 and H2O2 for adsorption sites. The reaction is sufficiently fast that the lifetime of SO2 within ice clouds could be controlled by this heterogeneous reaction and not by the gas-phase reaction with OH.
Temperature variability and trend estimates at tropopause and UT-LS over a subtropical site: Reunion (20.8° S, 55.5° E)
Authors: Bègue N. , Bencherif H. , Sivakumar V. , Kirgis G. , Mzé N. , Leclair de Bellevue J.
Published: April 2010

Abstract. This paper mainly focuses on the trends and variability of the tropopause and UT-LS temperature using radiosonde observations carried out over 16 years (January 1993 to December 2008) from a southern subtropical site, Reunion Island (20.8° S, 55.5° E), using a linear-regression fitting model. Two kinds of tropopause definitions, namely, cold point tropopause (CPT) and lapse rate tropopause (LRT) are used. In the purpose to characterize and quantify the relationship between the regional oceanic forcing and temperature at tropopause and UT-LS, we take into account the Indian Ocean Dipole (IOD) for the estimation of temperature trends. Results show that the main component is the Annual Oscillation (AO), particularly at tropopause (CPT, LRT) and in the lower stratosphere (LS) where more than 26% of the variability of temperature can be explained by AO. As a result, the influence of IOD on the variability of the temperature is at highest ratio at CPT and LS, with respectively 12.3% and 13.1%. The results show a low correlation between IOD and the temperature anomalies at tropopause (LRT, CPT) and UT-LS, in the range of 0.08–0.15, with the maximum of correlation at CPT (0.15). In addition, trend estimates at CPT and in the LS suggests that the IOD forcing contributes enhancing the rate of cooling of about 0.1 K per decade. Indeed a trend analysis reveals a cooling of about 0.90±0.40 K per decade at LS and a cooling trend of about 0.36±0.48 K per decade at CPT. The cooling trend at LS is found to be in good agreement with the others studies. These results support the assumption that the Indian Ocean may have a slight impact on temperature variability and on temperature change at CPT and in the LS over Reunion.
Review and parameterisation of bi-directional ammonia exchange between vegetation and the atmosphere
Authors: Massad R.-S. , Nemitz E. , Sutton M. A.
Published: April 2010

Abstract. Current deposition schemes used in atmospheric chemical transport models do not generally account for bi-directional exchange of ammonia (NH3). Bi-directional exchange schemes, which have so far been applied at the plot scale, can be included in transport models, but need to be parameterised with appropriate values of the stomatal compensation point (χs) and cuticular resistance (Rw). We here review existing measurements of χs as well as Rw and compile a comprehensive dataset from which we then propose generalised parameterisations. χs is related to Γs, the non-dimensional ratio of [NH4+]apo and [H+]apo in the apoplast, through the temperature dependence of the combined Henry and solubility equilibrium. The meta-analysis suggests that the nitrogen (N) input is the main driver of the apoplastic and bulk leaf concentrations of ammonium (NH+4 apo, NH+4 bulk). For managed ecosystems, the main source of N is fertilisation which is reflected in a peak value of χs a few days following application, but also alters seasonal values of NH+4 apo and NH+4 bulk. We propose a parameterisation for χs which includes peak values as a function of amount and type of fertiliser application which gradually decreases to a background value. The background χs is set based on total N input to the ecosystem as a yearly fertiliser application and N deposition (Ndep). For non-managed ecosystems, χs is parameterised based solely on the link with Ndep. For Rw we propose a general parameterisation as a function of atmospheric Relative Humidity (RH), incorporating a minimum value (R w(min)), which depends on the ratio of atmospheric acid concentrations (SO2, HNO3 and HCl) to NH3 concentrations. The parameterisations are based mainly on datasets from temperate locations in northern Europe making them most suitable for up-scaling in these regions (Unified EMEP model for example). In principle, the parameterisations should be applicable to other climates, though there is a need for more underpinning data, with the uncertainties being especially large for tropical and subtropical conditions.
Aerosol effects on ice clouds: can the traditional concept of aerosol indirect effects be applied to aerosol-cloud interactions in cirrus clouds?
Authors: Lee S. S. , Penner J. E.
Published: April 2010

Abstract. Cirrus clouds cover approximately 20–25% of the globe and thus play an important role in the Earth's radiation budget. This indicates that aerosol effects on cirrus clouds can have a substantial impact on the variation of global radiative forcing if the ice-water path (IWP) changes. This study examines the aerosol indirect effect (AIE) through changes in the IWP for a cirrus cloud case. We use a cloud-system resolving model (CSRM) coupled with a double-moment representation of cloud microphysics. Intensified interactions among the cloud ice number concentration (CINC), deposition and dynamics play a critical role in the IWP increases due to aerosol increases. Increased aerosols lead to increased CINC, providing increased surface area for water vapor deposition. The increased deposition causes depositional heating which produces stronger updrafts, and leads to the increased IWP. The conversion of ice crystals to aggregates through autoconversion and accretion plays a negligible role in the IWP responses to aerosols, as the sedimentation of aggregates. The sedimentation of ice crystals plays a more important role in the IWP response to aerosol increases than the sedimentation of aggregates, but, not more important than the interactions among the CINC, deposition and dynamics.
Options to accelerate ozone recovery:ozone and climate benefits
Authors: Daniel J. S. , Fleming E. L. , Portmann R. W. , Velders G. J. M. , Jackman C. H. , Ravishankara A. R.
Published: April 2010

Abstract. Hypothetical reductions in future emissions of ozone-depleting substances (ODSs), including N2O, are evaluated in terms of effects on equivalent effective stratospheric chlorine (EESC), globally-averaged total column ozone, and radiative forcing through 2100. Due to the established success of the Montreal Protocol, these actions can have only a fraction of the impact that regulations already in force have had. If all anthropogenic ODS emissions were halted beginning in 2011, ozone is calculated to be higher by about 1–2{%} during the period 2030–2100 compared to a case of no additional ODS restrictions. Radiative forcing by 2100 would be about 0.23 W/m2 lower due to the elimination of N2O emissions and about 0.005 W/m2 lower due to destruction of the chlorofluorocarbon (CFC) bank. The ability of EESC to be a suitable metric for total ozone is also quantified. Responding to the recent suggestion that N2O should be considered an ODS, we provide an approach to incorporate N2O into the EESC formulation.
EUCAARI ion spectrometer measurements at 12 European sites – analysis of new-particle formation events
Authors: Manninen H. E. , Nieminen T. , Asmi E. , Gagné S. , Häkkinen S. , Lehtipalo K. , Aalto P. , Vana M. , Mirme A. , Mirme S. , Hõrrak U. , Plass-Dülmer C. , Stange G. , Kiss G. , Hoffer A. , Tör\\H{o} N. , Moerman M. , Henzing B. , de Leeuw G. , Brinkenberg M. , Kouvarakis G. N. , Bougiatioti A. , Mihalopoulos N. , O'Dowd C. , Ceburnis D. , Arneth A. , Svenningsson B. , Swietlicki E. , Tarozzi L. , Decesari S. , Facchini M. C. , Birmili W. , Sonntag A. , Wiedensohler A. , Boulon J. , Sellegri K. , Laj P. , Gysel M. , Bukowiecki N. , Weingartner E. , Wehrle G. , Laaksonen A. , Hamed A. , Joutsensaari J. , Petäjä T. , Kerminen V.-M. , Kulmala M.
Published: April 2010

Abstract. We present comprehensive results on continuous atmospheric cluster and particle measurements in the size range ~1–42 nm within the European Integrated project on Aerosol Cloud Climate and Air Quality interactions (EUCAARI) project. We focused on characterizing the spatial and temporal variation of new-particle formation events and relevant particle formation parameters across Europe. Different types of air ion and cluster mobility spectrometers were deployed at 12 field sites across Europe from March 2008 to May 2009. The measurements were conducted in a wide variety of environments, including coastal and continental locations as well as sites at different altitudes (both in the boundary layer and the free troposphere). New-particle formation events were detected at all of the 12 field sites during the year-long measurement period. From the data, nucleation and growth rates of newly-formed particles were determined for each environment. In a case of parallel ion and neutral cluster measurements, we could also estimate the relative contribution of ion-induced and neutral nucleation to the total particle formation. The formation rates of charged particles at 2 nm accounted for 1–30% of the respective total particle formation rates. As a significant new result, we found out that the total particle formation rate varied much more between the different sites than the formation rate of charged particles. This work presents, so far, the most comprehensive effort to experimentally characterize nucleation and growth of atmospheric molecular clusters and nanoparticles at ground-based observation sites on a continental scale.
Sunphotometry of the 2006–2007 aerosol optical/radiative properties at the Himalayan Nepal Climate Observatory – Pyramid (5079 m a.s.l.)
Authors: Gobbi G. P. , Angelini F. , Bonasoni P. , Verza G. P. , Marinoni A. , Barnaba F.
Published: April 2010

Abstract. In spite of being located at the heart of the highest mountain range in the world, the Himalayan Nepal Climate Observatory (5079 m a.s.l.) at the Ev-K2-CNR Pyramid is shown to be affected by the advection of pollution aerosols from the populated regions of southern Nepal and the Indo-Gangetic plains. Such an impact is observed along most of the period April 2006–March 2007 addressed here, with a minimum in the monsoon season. Backtrajectory-analysis indicates long-range transport episodes occurring in this period to originate mainly in the West Asian deserts. At this high altitude site, the measured aerosol optical depth is observed to be: 1) about one order of magnitude lower than the one measured at Gandhi College (60 m a.s.l.), in the Indo-Gangetic basin, and 2) maximum during the monsoon period, due to the presence of elevated (cirrus-like) particle layers. Assessment of the aerosol radiative forcing results to be hampered by the persistent presence of these high altitude particle layers, which impede a continuous measurement of both the aerosol optical depth and its radiative properties from sky radiance inversions. Even though the retrieved absorption coefficients of pollution aerosols was rather large (single scattering albedo of the order of 0.6–0.9 were observed in the month of April 2006), the corresponding low optical depths (~0.03 at 500 nm) are expected to limit the relevant radiative forcings. Still, the high specific forcing of this aerosol and its capability of altering snow surface albedo provide good reason for continuous monitoring.
Nocturnal nitrogen oxides at a rural mountain-site in South-Western Germany
Authors: Crowley J. N. , Schuster G. , Pouvesle N. , Parchatka U. , Fischer H. , Bonn B. , Bingemer H. , Lelieveld J.
Published: April 2010

Abstract. A new, two-channel instrument for simultaneous NO3 and N2O5 monitoring was used to make the first comprehensive set of nocturnal NOx measurements (NO, NO2, NO3 and N2O5) at the Taunus Observatory, a rural mountain site (Kleiner Feldberg) in South-western Germany. In May 2008, NO3 and N2O5 mixing ratios were well above the instrumental detection limit (a few ppt) on all nights of the campaign and were characterised by large variability resulting from inhomogeneously distributed sinks. The concentrations of NO3, N2O5 and NO2 were consistent with the equilibrium constant, K2, defining the rates of formation and thermal dissociation of N2O5. A steady-state lifetime analysis showed that nocturnal NOx losses were generally dominated by reaction of NO3 with volatile organic compounds in this forested region, with N2O5 uptake to aerosols of secondary importance. Analysis of a limited dataset obtained at high relative humidity indicated that the loss of N2O5 by reaction with water vapour is less efficient (> factor 3) than derived using laboratory kinetic data. The fraction of NOx present as NO3 and N2O5 reached ≈20% on some nights, with night-time losses of NOx competing with daytime losses.
Mercury air-borne emissions from 5 municipal solid waste landfills in Guiyang and Wuhan, China
Authors: Li Z. G. , Feng X. , Li P. , Liang L. , Tang S. L. , Wang S. F. , Fu X. W. , Qiu G. L. , Shang L. H.
Published: April 2010

Abstract. A detailed study on atmospheric mercury emissions from municipal solid waste (MSW) landfills in China is necessary to understand mercury behavior in this source category, simply because China disposes of bulk MSW by landfilling and a large quantity of mercury enters into landfills. Between 2003 and 2006, mercury airborne emissions through different pathways, as well as mercury speciation in landfill gas (LFG) were measured at 5 MSW landfills in Guiyang and Wuhan, China. The results showed that mercury content in the substrate fundamentally affected the magnitude of mercury emissions, resulting in the highest emission rate (as high as 57 651 ng Hg m−2 h−1) at the working face and in un-covered waste areas, and the lowest measured at soil covers and vegetation areas (less than 20 ng Hg m−2 h−1). Meteorological parameters, especially solar radiation, influenced the diurnal pattern of mercury surface-air emissions. Total gaseous mercury (TGM) in LFG varied from 2.0 to 1406.0 ng m−3, monomethyl mercury (MMHg) and dimethyl mercury (DMHg) in LFG averaged at 1.93 and 9.21 ng m−3, and accounted for 0.51% and 1.79% of the TGM in the LFG, respectively. Total mercury emitted from the five landfills ranged from 17 to 3285 g yr−1, with the highest from the working face, then soil covering, and finally the vent pipes.
Climatology and comparison of ozone from ENVISAT/GOMOS and SHADOZ/balloon-sonde observations in the southern tropics
Authors: Mze N. , Hauchecorne A. , Bencherif H. , Dalaudier F. , Bertaux J.-L.
Published: April 2010

Abstract. In this paper, the stellar occultation instrument GOMOS is compared with ozonesondes from the SHADOZ network. We only used nighttime O3 profiles and a requirement selection at 8 Southern Hemisphere stations. 7 years of GOMOS datasets (GOPR 6.0cf and IPF 5.0) and 11 years of balloon-sondes are used in this study. A monthly distribution of GOMOS O3 mixing ratios is performed in the upper-troposphere and in the stratosphere (15–50 km). A comparison with SHADOZ is done in the altitude range from 15 km to 30 km. In the 21–30 km altitude range, a satisfactory agreement is observed between GOMOS and SHADOZ although some differences are observed depending on the station. The range for monthly differences is generally decreasing with increasing height and is within ±15%. It is found that the agreement between GOMOS and SHADOZ degrades below ~20 km. The median differences are nearly within ±5% particularly above 23 km. But a large positive bias is found below 21 km compared to SHADOZ.
Fast two-dimensional GC-MS with thermal extraction for anhydro-sugars in fine aerosols
Authors: Ma Y. , Hays M. D. , Geron C. D. , Walker J. T. , Gatari Gichuru M. J.
Published: April 2010

Abstract. A fast two-dimensional gas chromatography (GC-MS) method that uses heart-cutting and thermal extraction (TE) and requires no chemical derivatization was developed for the determination of anhydro-sugars in fine aerosols. Evaluation of the TE-GC-GC-MS method shows high average relative accuracy (≥90%), reproducibility (≤10% relative standard deviation), detection limits of less than 3 ng/μL, and negligible carryover for levoglucosan, mannosan, and galactosan markers. TE-GC-GC-MS- and solvent extraction (SE)-GC-MS-measured levoglucosan concentrations correlate across several diverse types of biomass burning aerosols. Because the SE-GC-MS measurements were taken 8 years prior to the TE-GC-GC-MS ones, the stability of levoglucosan is established for quartz filter-collected biomass burning aerosol samples stored at ultra-low temperature (–45°C). Levoglucosan concentrations (w/w) in aerosols collected following atmospheric dilution near open fires of varying intensity are similar to those in biomass burning aerosols produced in a laboratory enclosure. An average levoglucosan-mannosan-galactosan ratio of 15:2:1 is observed for these two aerosol sets. TE-GC-GC-MS analysis of atmospheric aerosols from the US and Africa produced levoglucosan concentrations (0.01–1.6 μg/m3) well within those reported for aerosols collected globally and examined using different analytical techniques (0.004–7.6 μg/m3). Further comparisons among techniques suggest that fast TE-GC-GC-MS is among the most sensitive, accurate, and precise methods for compound-specific quantification of anhydro-sugars. In addition, an approximately twofold increase in aerosol sample throughput may be realized when combining TE with fast chromatography for anhydro-sugar determination.
Cluster analysis of midlatitude oceanic cloud regimes – Part 1: Mean cloud and meteorological properties
Authors: Gordon N. D. , Norris J. R.
Published: April 2010

Abstract. Clouds play an important role in the climate system by reducing the amount of shortwave radiation reaching the surface and the amount of longwave radiation escaping to space. Although dependent on type and location, clouds produce more cooling than warming in the global average. Accurate simulation of clouds in computer models remains elusive, however, pointing to a lack of understanding of the connection between large-scale dynamics and cloud properties. This study uses a k-means clustering algorithm to group 21-years of satellite cloud data over midlatitude oceans into seven clusters and demonstrates that the cloud clusters are associated with distinct large-scale dynamical conditions. Three clusters correspond to low-level cloud regimes with different cloud fraction and cumuliform or stratiform characteristics, but all occur under large-scale descent and a relatively dry free troposphere. The "small cumulus" regime is most prevalent equatorward of 40° in all seasons; the "large cumulus" regime is associated with a relatively cold troposphere and primarily occurs during winter; and the "stratocumulus/stratus" regime occurs under a temperature inversion and relatively warm free troposphere and predominates during summer. Three clusters correspond to vertically extensive cloud regimes with tops in the middle or upper troposphere. They differ according to the strength of large-scale ascent and enhancement of tropospheric temperature and humidity: "deep altostratus" has the smallest forcing, "weak frontal" is in the middle, and "strong frontal" has the largest forcing. The frontal cloud regimes occur most frequently in storm track regions. The final cluster, "cirrus" is associated with a lower troposphere that is dry and an upper troposphere that is moist and experiencing weak ascent and horizontal moist advection. This information builds a foundation for producing an observational estimate of the midlatitude ocean cloud response to warming that is independent of confounding meteorological influences.
Direct radiative effect of aerosols emitted by transport: from road, shipping and aviation
Authors: Balkanski Y. , Myhre G. , Gauss M. , Rädel G. , Highwood E. J. , Shine K. P.
Published: April 2010

Abstract. Aerosols and their precursors are emitted abundantly by transport activities. Transportation constitutes one of the fastest growing activities and its growth is predicted to increase significantly in the future. Previous studies have estimated the aerosol direct radiative forcing from one transport sub-sector, but only one study to our knowledge estimated the range of radiative forcing from the main aerosol components (sulphate, black carbon (BC) and organic carbon) for the whole transportation sector. In this study, we compare results from two different chemical transport models and three radiation codes under different hypothesis of mixing: internal and external mixing using emission inventories for the year 2000. The main results from this study is a positive direct radiative forcing for aerosols emitted by road traffic of +20±11 mWm−2 for an externally mixed aerosol, and of +32±13 mWm−2 when BC is internally mixed . These direct radiative forcings are much higher than the previously published estimate of +3±11 mWm−2. For transport activities from shipping, the net direct aerosol radiative forcing is negative. This forcing is dominated by the contribution of the sulphate. For both an external and an internal mixture, the radiative forcing from shipping is estimated at −26±4 mWm−2. These estimates are in very good agreement with the range of a previously published one (from −46 to −13 mWm−2) but with a much narrower range. By contrast, the direct aerosol forcing from aviation is estimated to be small, and in the range −0.9 to +0.3 mWm−2.
On condensational growth of clusters and nanoparticles in sub-10 nm size range
Authors: Nieminen T. , Lehtinen K. E. J. , Kulmala M.
Published: April 2010

Abstract. The growth of freshly formed nanoparticles has been investigated. A new analytical expression based on a recently developed exact solution for the condensational growth rate has been derived. Based on the new growth rate, a new approximate but accurate analytical expression for growth time has been derived. The expression includes transition regime effects on growth, molecule size effects on the collision cross section and particle mobility effects on the relative collisional speeds – the last two of which are typically neglected, but may have significant effects when dealing with the growth of freshly nucleated particles. To demonstrate the use of the derived expressions, the contribution of sulphuric acid and organic compounds on sub 3 nm and sub 10 nm particle growth rates has been studied. For sulphuric acid also the effect of hydration as function of relative humidity has been taken into account. According to the new expression the needed sulphuric acid concentration for 1 nm/h growth in sub 3 nm range is ca. 7×106 cm−3, which is a factor of two smaller than values typically used in aerosol physics based on standard model in kinetic regime.
Ozone reservoir layers in a coastal environment – a case study in Southern Taiwan
Authors: Lin C.-H. , Wu Y.-L. , Lai C.-H.
Published: April 2010

Abstract. The air layer between the nocturnal boundary layer and the top of the daily mixing layer in an ozone-polluted area is known to serve as an ozone reservoir since the ozone that is produced in the previous daytime mixing layer can be well preserved throughout the night in the air layer. Ozone reservoir layers are capable of enhancing surface ozone accumulation on the following day. However, our knowledge of the characteristics of ozone reservoir layers and their effects on the daily ozone accumulations is limited. In this work, ozone reservoir layers were experimentally investigated at a coastal, near-mountain site in Southern Taiwan, 30 km away from the coastlines. Tethered ozone soundings were performed to obtain vertical profiles of ozone and meteorological variables during a four-day ozone episode in November 2006. Observation-based methods are adopted to evaluate the influences of the ozone reservoir layers on the surface ozone accumulation during the four-day ozone episode. Ozone reservoir layers were found to develop every evening with a depth of 1200–1400 m. Ozone concentrations within the reservoir layers reached over 140 parts per billion (ppb). From each evening to midnight, the size of the ozone reservoir layer and the ozone concentration inside dramatically changed. As a result, a concentrated, elevated ozone reservoir layer formed with a depth of 400 m at 800–1200 m every midnight. For the rest of each night, the elevated ozone reservoir layer gradually descended until it reached 500–900 m in the next morning. Local circulations and nocturnal subsidence are responsible for the observed evolution. The ozone concentration at the study site was maximal at 15:00–17:00 LT daily because of the addition of the daily produced ozone on the preceding day. Hourly downward mixing ozone concentrations due to the ozone reservoir layers can be as high as 35–45 ppb/h in the late morning. The contribution of the ozone carried over from the preceding day can be 75–85 ppb, which contributes over 50% to the daily ozone pollution as compared with ozone produced on the study day.
Modeling natural emissions in the Community Multiscale Air Quality (CMAQ) model – Part 1: Building an emissions data base
Authors: Smith S. N. , Mueller S. F.
Published: April 2010

Abstract. A natural emissions inventory for the continental United States and surrounding territories is needed in order to use the US Environmental Protection Agency Community Multiscale Air Quality (CMAQ) Model for simulating natural air quality. The CMAQ air modeling system (including the Sparse Matrix Operator Kernel Emissions (SMOKE) emissions processing system) currently estimates volatile organic compound (VOC) emissions from biogenic sources, nitrogen oxide (NOx) emissions from soils, ammonia from animals, several types of particulate and reactive gas emissions from fires, as well as windblown dust and sea salt emissions. However, there are several emission categories that are not commonly treated by the standard CMAQ Model system. Most notable among these are nitrogen oxide emissions from lightning, reduced sulfur emissions from oceans, geothermal features and other continental sources, and reactive chlorine gas emissions linked with sea salt chloride. A review of past emissions modeling work and existing global emissions data bases provides information and data necessary for preparing a more complete natural emissions data base for CMAQ applications. A model-ready natural emissions data base is developed to complement the anthropogenic emissions inventory used by the VISTAS Regional Planning Organization in its work analyzing regional haze based on the year 2002. This new data base covers a modeling domain that includes the continental United States plus large portions of Canada, Mexico and surrounding oceans. Comparing July 2002 source data reveals that natural emissions account for 16% of total gaseous sulfur (sulfur dioxide, dimethylsulfide and hydrogen sulfide), 44% of total NOx, 80% of reactive carbonaceous gases (VOCs and carbon monoxide), 28% of ammonia, 96% of total chlorine (hydrochloric acid, nitryl chloride and sea salt chloride), and 84% of fine particles (i.e., those smaller than 2.5 μm in size) released into the atmosphere. The seasonality and relative importance of the various natural emissions categories are described.
Patterns of mercury dispersion from local and regional emission sources, rural Central Wisconsin, USA
Authors: Kolker A. , Olson M. L. , Krabbenhoft D. P. , Tate M. T. , Engle M. A.
Published: April 2010

Abstract. Simultaneous real-time changes in mercury (Hg) speciation – reactive gaseous Hg (RGM), elemental Hg (Hg°), and fine particulate Hg (Hg-PM2.5), were determined from June to November 2007, in ambient air at three locations in rural Central Wisconsin. Known Hg emission sources within the airshed of the monitoring sites include: 1) a 1114 megawatt (MW) coal-fired electric utility generating station; 2) a Hg-bed chlor-alkali plant; and 3) a smaller (465 MW) coal-burning electric utility. Monitoring sites, showing sporadic elevation of RGM, Hg° and Hg-PM2.5, were positioned at distances of 25, 50 and 100 km northward of the larger electric utility. A series of RGM events were recorded at each site. The largest, on 23 September, occurred under prevailing southerly winds, with a maximum RGM value (56.8 pg m−3) measured at the 100 km site, and corresponding elevated SO2 (10.41 ppbv; measured at 50 km site). The finding that RGM, Hg°, and Hg-PM2.5 are not always highest at the 25 km site, closest to the large generating station, contradicts the idea that RGM decreases with distance from a large point source. This may be explained if: 1) the 100 km site was influenced by emissions from the chlor-alkali facility or by RGM from regional urban sources; 2) the emission stack height of the larger power plant promoted plume transport at an elevation where the Hg is carried over the closest site; or 3) RGM was being generated in the plume through oxidation of Hg°. Operational changes at each emitter since 2007 should reduce their Hg output, potentially allowing quantification of the environmental benefit in future studies.
Daytime ozone and temperature variations in the mesosphere: a comparison between SABER observations and HAMMONIA model
Authors: Dikty S. , Schmidt H. , Weber M. , von Savigny C. , Mlynczak M. G.
Published: April 2010

Abstract. The scope of this paper is to investigate the latest version 1.07 SABER (Sounding of the Atmosphere using Broadband Emission Radiometry) tropical ozone from the 1.27 μm as well as from the 9.6 μm retrieval and temperature data with respect to daytime variations in the upper mesosphere. For a better understanding of the processes involved we compare these daytime variations to the output of the three-dimensional general circulation and chemistry model HAMMONIA (Hamburg Model of the Neutral and Ionized Atmosphere). The results show good agreement for ozone. The amplitude of daytime variations is in both cases approximately 60% of the daytime mean. During equinox the daytime maximum ozone abundance is for both, the observations and the model, higher than during solstice, especially above 80 km. We also use the HAMMONIA output of daytime variation patterns of several other different trace gas species, e.g., water vapor and atomic oxygen, to discuss the daytime pattern in ozone. In contrast to ozone, temperature data show little daytime variations between 65 and 90 km and their amplitudes are on the order of less than 1.5%. In addition, SABER and HAMMONIA temperatures show significant differences above 80 km.
Hydrochlorofluorocarbon and hydrofluorocarbon emissions in East Asia determined by inverse modeling
Authors: Stohl A. , Kim J. , Li S. , O'Doherty S. , Salameh P. K. , Saito T. , Vollmer M. K. , Wan D. , Yao B. , Yokouchi Y. , Zhou L. X.
Published: April 2010

Abstract. The emissions of three hydrochlorofluorocarbons, HCFC-22 (CHClF2), HCFC-141b (CH3CCl2F) and HCFC-142b (CH3CClF2) and three hydrofluorocarbons, HFC-23 (CHF3), HFC-134a (CH2FCF3) and HFC-152a (CH3CHF2) from five East Asian countries for the year 2008 are determined by inverse modeling. The inverse modeling is based on in-situ measurements of these halocarbons at the Japanese stations Cape Ochi-ishi and Hateruma, the Chinese station Shangdianzi and the South Korean station Gosan. For every station and every 3 h, 20-day backward calculations were made with the Lagrangian particle dispersion model FLEXPART. The model output, the measurement data, bottom-up emission information and corresponding uncertainties were fed into an inversion algorithm to determine the regional emission fluxes. The model captures the observed variation of halocarbon mixing ratios very well for the two Japanese stations but has difficulties explaining the large observed variability at Shangdianzi, which is partly caused by small-scale transport from Beijing that is not adequately captured by the model. Based on HFC-23 measurements, the inversion algorithm could successfully identify the locations of factories known to produce HCFC-22 and emit HFC-23 as an unintentional byproduct. This lends substantial credibility to the inversion method. We report national emissions for China, North Korea, South Korea and Japan, as well as emissions for the Taiwan region. Halocarbon emissions in China are much larger than the emissions in the other countries together and contribute a substantial fraction to the global emissions. Our estimates of Chinese emissions for the year 2008 are 65.3±6.6 kt/yr for HCFC-22 (17% of global emissions extrapolated from Montzka et al., 2009), 12.1±1.6 kt/yr for HCFC-141b (22%), 7.3±0.7 kt/yr for HCFC-142b (17%), 6.2±0.7 kt/yr for HFC-23 (>50%), 12.9±1.7 kt/yr for HFC-134a (9% of global emissions estimated from Velders et al., 2009) and 3.4±0.5 kt/yr for HFC-152a (7%).
Cloud albedo increase from carbonaceous aerosol
Authors: Leaitch W. R. , Lohmann U. , Russell L. M. , Garrett T. , Shantz N. C. , Toom-Sauntry D. , Strapp J. W. , Hayden K. L. , Marshall J. , Worsnop D. , Jayne J.
Published: April 2010

Abstract. Atmospheric cooling from the effect of anthropogenic carbonaceous aerosol particles on the reflectivity of sunlight by water clouds remains an uncertainty for climate prediction. Airborne measurements of aerosol and cloud properties as well as light extinction were made below, in and above stratocumulus over the Northwest Atlantic Ocean on consecutive days. On the first day, the history of the below-cloud fine particle aerosol was marine and the fine particle sulphate and organic carbon mass concentrations measured at cloud base were 2.4 μg m−3 and 0.9 μg m−3, respectively. On the second day, the below-cloud aerosol was continentally influenced and the fine particle sulphate and organic carbon mass concentrations were 2.3 μg m−3 and 2.6 μg m−3, respectively. Correspondingly, the number concentrations of aerosol particles below cloud were approximately a factor of two higher on the second day, while the below-cloud size distributions were similar on both days. The cloud droplet number concentrations (CDNC) on the second day were approximately three times higher than the CDNC measured on the first day, and the vertically integrated cloud light extinction measurements indicate a 6% increase in the cloud albedo principally due to the increase in the carbonaceous components on the second day. Locally, this albedo increase translates to a daytime radiative cooling of ~12 W m−2. This result provides observational evidence that the role of anthropogenic carbonaceous components in the cloud albedo effect can be much larger than that of anthropogenic sulphate, as some global simulations have indicated.
First ground-based FTIR-observations of methane in the tropics
Authors: Petersen A. K. , Warneke T. , Frankenberg C. , Bergamaschi P. , Gerbig C. , Notholt J. , Buchwitz M. , Schneising O. , Schrems O.
Published: April 2010

Abstract. Total column concentrations and volume mixing ratio profiles of methane have been retrieved from ground-based solar absorption FTIR spectra in the near-infrared recorded in Paramaribo (Suriname). The methane FTIR observations are compared with TM5 model simulations and satellite observations from SCIAMACHY, and represent the first validation of SCIAMACHY retrievals in the tropics using ground-based remote sensing techniques. Apart from local biomass burning features, our methane FTIR observations agree well with the SCIAMACHY retrievals and TM5 model simulations.
Probabilistic description of ice-supersaturated layers in low resolution profiles of relative humidity
Authors: Dickson N. C. , Gierens K. M. , Rogers H. L. , Jones R. L.
Published: April 2010

Abstract. The global observation, assimilation and prediction in numerical models of ice super-saturated (ISS) regions (ISSR) are crucial if the climate impact of aircraft condensations trails (contrails) is to be fully understood, and if, for example, contrail formation is to be avoided through aircraft operational measures. A robust assessment of the global distribution of ISSR will further this debate, and ISS event occurrence, frequency and spatial scales have recently attracted significant attention. The mean horizontal path length through ISSR as observed by MOZAIC aircraft is 150 km (±250 km). The average vertical thickness of ISS layers is 600–800 m (±575 m) but layers ranging from 25 m to 3000 m have been observed, with up to one third of ISS layers thought to be less than 100 m deep. Given their small scales compared to typical atmospheric model grid sizes, statistical representations of the spatial scales of ISSR are required, in both horizontal and vertical dimensions, if global occurrence of ISSR is to be adequately represented in climate models. This paper uses radiosonde launches made by the UK Meteorological Office, from the British Isles, Gibraltar, St. Helena and the Falkland Islands between January 2002 and December 2006, to investigate the probabilistic occurrence of ISSR. Specifically each radiosonde profile is divided into 50- and 100-hPa pressure layers, to emulate the coarse vertical resolution of some atmospheric models. Then the high resolution observations contained within each thick pressure layer are used to calculate an average relative humidity and an ISS fraction for each individual thick pressure layer. These relative humidity pressure layer descriptions are then linked through a probability function to produce an s-shaped curve describing the ISS fraction in any average relative humidity pressure layer. An empirical investigation has shown that this one curve is statistically valid for mid-latitude locations, irrespective of season and altitude, however, pressure layer depth is an important variable. Using this empirical understanding of the s-shaped relationship a mathematical model was developed to represent the ISS fraction within any arbitrary thick pressure layer. Here the statistical distributions of actual high resolution RHi observations in any thick pressure layer, along with an error function, are used to mathematically describe the s-shape. Two models were developed to represent both 50- and 100-hPa pressure layers with each reconstructing their respective s-shapes within 8–10% of the empirical curves. These new models can be used, to represent the small scale structures of ISS events, in modelled data where only low vertical resolution is available. This will be useful in understanding, and improving the global distribution, both observed and forecasted, of ice super-saturation.
Investigation of the sources and processing of organic aerosol over the Central Mexican Plateau from aircraft measurements during MILAGRO
Authors: DeCarlo P. F. , Ulbrich I. M. , Crounse J. , de Foy B. , Dunlea E. J. , Aiken A. C. , Knapp D. , Weinheimer A. J. , Campos T. , Wennberg P. O. , Jimenez J. L.
Published: April 2010

Abstract. Organic aerosol (OA) represents approximately half of the submicron aerosol in Mexico City and the Central Mexican Plateau. This study uses the high time resolution measurements performed onboard the NCAR/NSF C-130 aircraft during the MILAGRO/MIRAGE-Mex field campaign in March 2006 to investigate the sources and chemical processing of the OA in this region. An examination of the OA/ΔCO ratio evolution as a function of photochemical age shows distinct behavior in the presence or absence of substantial open biomass burning (BB) influence, with the latter being consistent with other studies in polluted areas. In addition, we present results from Positive Matrix Factorization (PMF) analysis of 12-s High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) OA spectra. Four components were resolved. Three of the components contain substantial organic oxygen and are termed semivolatile oxygenated OA (SV-OOA), low-volatility OOA (LV-OOA), and biomass burning OA (BBOA). A reduced "hydrocarbon-like OA" (HOA) component is also resolved. LV-OOA is highly oxygenated (atomic O/C~1) and is aged organic aerosol linked to regional airmasses, with likely contributions from pollution, biomass burning, and other sources. SV-OOA is strongly correlated with ammonium nitrate, Ox, and the Mexico City Basin. We interpret SV-OOA as secondary OA which is nearly all (>90%) anthropogenic in origin. In the absence of biomass burning it represents the largest fraction of OA over the Mexico City basin, consistent with other studies in this region. BBOA is identified as arising from biomass burning sources due to a strong correlation with HCN, and the elevated contribution of the ion C2H4O2+ (m/z 60, a marker for levoglucosan and other primary BB species). WRF-FLEXPART calculated fire impact factors (FIF) show good correlation with BBOA mass concentrations within the basin, but show location offsets in the far field due to model transport errors. This component is small or absent when forest fires are suppressed by precipitation. Since PMF factors represent organic species grouped by chemical similarity, and this study spans a very large and continuous range of OA ages, additional postprocessing is needed to more directly apportion OA amounts to sources, which is done here based on correlations and regressions to key tracers. The postprocessed AMS results are similar to those from an independent source apportionment based on multiple linear regression with gas-phase tracers. During a flight with very high forest fire intensity near the basin OA arising from open BB represents ~66% of the OA mass in the basin and contributes similarly OA mass in the outflow. Aging and SOA formation of BB emissions is estimated to add OA mass equivalent to about ~32–42% of the primary BBOA over several hours to a day.