bluuebunny/crossref_metadata_2025 huggingface dataset:
Geochemical perspectives from a new aerosol chemical mass closure
Authors: Guinot B. , Cachier H. , Oikonomou K.
Published: April 2010

Abstract. The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC) and the black carbon (BC). Atmospheric particles are separated into coarse (AD>2 μm) and fine (AD<2 μm) fractions and are treated separately. For the coarse fraction the carbonaceous component is minor and assumption is made for the conversion factor k of OC-to-POM (Particulate Organic Matter) which is fixed to the value of 1.8 accounting for secondary species. The coarse soluble calcium is shown to display a correlation (regression coefficient f, y axis intercept b) with the missing mass. Conversely, the fine fraction is dominated by organic species and assumption is made for dust which is assumed to have the same f factor as the coarse mode dust. The fine mode mass obtained from chemical analyses is then adjusted to the actual weighed mass by tuning the k conversion factor. The k coefficient is kept different in the two modes due to the expected different origins of the organic particles. Using the f and k coefficient obtained from the data set, the mass closure is reached for each individual sample with an undetermined fraction less than 10%. The procedure has been applied to different urban and peri-urban environments in Europe and in Beijing and its efficiency and uncertainties on f and k values are discussed. The f and k coefficients are shown to offer consistent geochemical indications on aerosol origin and transformations. f allows to retrieve dust mass and its value accounting for Ca abundance in dust at the site of investigation may serve as an indicator of dust origin and aerosol interactions with anthropogenic acids. f values were found to vary in the 0.08–0.12 range in European urban areas, and a broader range in Beijing (0.01–0.16). As expected, k appears to be a relevant proxy for particle origin and ageing and varies in the 1.4–1.8 range. For Beijing, k exhibits high values of about 1.7 in winter and summer. Winter values suggest that fresh coal aerosol might be responsible for such a high k value, which was not taken into account in previous works.
Solar cycle variations of stratospheric ozone and temperature in simulations of a coupled chemistry-climate model
Authors: Austin J. , Hood L. L. , Soukharev B. E.
Published: April 2010

Abstract. The results from three 45-year simulations of a coupled chemistry climate model are analysed for solar cycle influences on ozone and temperature. The simulations include UV forcing at the top of the atmosphere, which includes a generic 27-day solar rotation effect as well as the observed monthly values of the solar fluxes. The results are analysed for the 27-day and 11-year cycles in temperature and ozone. In accordance with previous results, the 27-day cycle results are in good qualitative agreement with observations, particularly for ozone. However, the results show significant variations, typically a factor of two or more in sensitivity to solar flux, depending on the solar cycle. In the lower and middle stratosphere we show good agreement also between the modelled and observed 11-year cycle results for the ozone vertical profile averaged over low latitudes. In particular, the minimum in solar response near 20 hPa is well simulated. In comparison, experiments of the model with fixed solar phase (solar maximum/solar mean) and climatological sea surface temperatures lead to a poorer simulation of the solar response in the ozone vertical profile, indicating the need for variable phase simulations in solar sensitivity experiments. The role of sea surface temperatures and tropical upwelling in simulating the ozone minimum response are also discussed.
Evaluation of organic markers for chemical mass balance source apportionment at the Fresno Supersite
Authors: Chow J. C. , Watson J. G. , Lowenthal D. H. , Chen L. W. A. , Zielinska B. , Mazzoleni L. R. , Magliano K. L.
Published: April 2010

Abstract. Sources of PM2.5 at the Fresno Supersite during high PM2.5 episodes occurring from 15 December 2000–3 February 2001 were estimated with the Chemical Mass Balance (CMB) receptor model. The ability of source profiles with organic markers to distinguish motor vehicle, residential wood combustion (RWC), and cooking emissions was evaluated with simulated data. Organics improved the distinction between gasoline and diesel vehicle emissions and allowed a more precise estimate of the cooking source contribution. Sensitivity tests using average ambient concentrations showed that the gasoline vehicle contribution was not resolved without organics. Organics were not required to estimate hardwood contributions. The most important RWC marker was the water-soluble potassium ion. The estimated cooking contribution did not depend on cholesterol because its concentrations were below the detection limit in most samples. Winter time source contributions were estimated by applying the CMB model to individual and average sample concentrations. RWC was the largest source, contributing 29–31% of measured PM2.5. Hardwood and softwood combustion accounted for 16–17% and 12–15%, respectively. Secondary ammonium nitrate and motor vehicle emissions accounted for 31–33% and 9–15%, respectively. The gasoline vehicle contribution (3–10%) was comparable to the diesel vehicle contribution (5–6%). The cooking contribution was 5–19% of PM2.5. Fresno source apportionment results were consistent with those estimated in previous studies.
The Assimilation of Envisat data (ASSET) project
Authors: Lahoz W. A. , Geer A. J. , Bekki S. , Bormann N. , Ceccherini S. , Elbern H. , Errera Q. , Eskes H. J. , Fonteyn D. , Jackson D. R. , Khattatov B. , Marchand M. , Massart S. , Peuch V.-H. , Rharmili S. , Ridolfi M. , Segers A. , Talagrand O. , Thornton H. E. , Vik A. F. , von Clarmann T.
Published: April 2010

Abstract. This paper discusses the highlights of the EU-funded "Assimilation of Envisat data" (ASSET) project, which has involved assimilation of Envisat atmospheric constituent and temperature data into systems based on Numerical Weather Prediction (NWP) models and chemical transport models (CTMs). Envisat was launched in 2002 and is one of the largest Earth Observation (EO) satellites ever built. It carries several sophisticated EO instruments providing insights into chemistry and dynamics of the atmosphere. In this paper we focus on the assimilation of temperature and constituents from Envisat. The overarching theme of the ASSET project has been to bring together experts from all aspects of the data assimilation problem. This has allowed ASSET to address several themes comprehensively: enhancement of NWP analyses by assimilation of research satellite data; studies of the distribution of stratospheric chemical species by assimilation of research satellite data into CTM systems; objective assessment of the quality of ozone analyses; studies of the spatial and temporal evolution of tropospheric pollutants; enhanced retrievals of Envisat data; and data archival and dissemination. Among the results from the ASSET project, many of which are firsts in their field, we can mention: a positive impact on NWP analyses from assimilation of height-resolved stratospheric humidity and temperature data, and assimilation of limb radiances; the extraction of temperature information from the assimilation of chemical species into CTMs; a first intercomparison between ozone assimilation systems; the extraction of information on tropospheric pollution from assimilation of Envisat data; and the large potential of the Envisat MIPAS dataset. This paper discusses these, often novel, developments and results. Finally, achievements of, and recommendations from, the ASSET project are presented.
Observations of total peroxy nitrates and aldehydes: measurement interpretation and inference of OH radical concentrations
Authors: Cleary P. A. , Wooldridge P. J. , Millet D. B. , McKay M. , Goldstein A. H. , Cohen R. C.
Published: April 2010

Abstract. We describe measurements of total peroxy nitrates (ΣPNs), NO2, O3 and several aldehydes at Granite Bay, California, during the Chemistry and Transport of the Sacramento Urban Plume-2001 (CATSUP 2001) campaign, from 19 July–16 September 2001. We observed a strong photochemically driven variation of ΣPNs during the day with the median of 1.2 ppb at noon. Acetaldehyde, pentanal, hexanal and methacrolein had median abundances in the daytime of 1.2 ppb, 0.093 ppb, 0.14 ppb, and 0.27 ppb, respectively. We compare steady state and time dependent calculations of the dependence of ΣPNs on aldehydes, OH, NO and NO2 showing that the steady state calculations are accurate to ±30% between 10:00 and 18:00 h. We use the steady state calculation to investigate the composition of ΣPNs and the concentration of OH at Granite Bay. We find that PN molecules that have never been observed before make up an unreasonably large fraction of the ΣPNs unless we assume that there exists a PAN source that is much larger than the acetaldehyde source. We calculate that OH at the site varied between 2 and 7×106 molecule cm−3 at noon during the 8 weeks of the experiment.
Atmospheric effects and societal consequences of regional scale nuclear conflicts and acts of individual nuclear terrorism
Authors: Toon O. B. , Turco R. P. , Robock A. , Bardeen C. , Oman L. , Stenchikov G. L.
Published: April 2010

Abstract. We assess the potential damage and smoke production associated with the detonation of small nuclear weapons in modern megacities. While the number of nuclear warheads in the world has fallen by about a factor of three since its peak in 1986, the number of nuclear weapons states is increasing and the potential exists for numerous regional nuclear arms races. Eight countries are known to have nuclear weapons, 2 are constructing them, and an additional 32 nations already have the fissile material needed to build substantial arsenals of low-yield (Hiroshima-sized) explosives. Population and economic activity worldwide are congregated to an increasing extent in megacities, which might be targeted in a nuclear conflict. We find that low yield weapons, which new nuclear powers are likely to construct, can produce 100 times as many fatalities and 100 times as much smoke from fires per kt yield as previously estimated in analyses for full scale nuclear wars using high-yield weapons, if the small weapons are targeted at city centers. A single "small" nuclear detonation in an urban center could lead to more fatalities, in some cases by orders of magnitude, than have occurred in the major historical conflicts of many countries. We analyze the likely outcome of a regional nuclear exchange involving 100 15-kt explosions (less than 0.1% of the explosive yield of the current global nuclear arsenal). We find that such an exchange could produce direct fatalities comparable to all of those worldwide in World War II, or to those once estimated for a "counterforce" nuclear war between the superpowers. Megacities exposed to atmospheric fallout of long-lived radionuclides would likely be abandoned indefinitely, with severe national and international implications. Our analysis shows that smoke from urban firestorms in a regional war would rise into the upper troposphere due to pyro-convection. Robock et al. (2007) show that the smoke would subsequently rise deep into the stratosphere due to atmospheric heating, and then might induce significant climatic anomalies on global scales. We also anticipate substantial perturbations of global ozone. While there are many uncertainties in the predictions we make here, the principal unknowns are the type and scale of conflict that might occur. The scope and severity of the hazards identified pose a significant threat to the global community. They deserve careful analysis by governments worldwide advised by a broad section of the world scientific community, as well as widespread public debate.
Identification and classification of the formation of intermediate ions measured in boreal forest
Authors: Hirsikko A. , Bergman T. , Laakso L. , Dal Maso M. , Riipinen I. , Hõrrak U. , Kulmala M.
Published: April 2010

Abstract. We have measured the size distributions of air ions (0.42–7.5 nm in diameter) with the Balanced Scanning Mobility Analyzer in boreal forest, in Southern Finland since spring 2003. The size range covers the size range of cluster ions (approximately 0.42–1.6 nm) and naturally charged nanometre aerosol particles (1.6–7.5 nm) or intermediate air ions. Based on the measurements from April 2003 to March 2006 we studied the characteristics of charged aerosol particle formation by classifying each day either as a particle formation event, undefined or non-event day. The principal of the classification, as well as the statistical description of the charged aerosol particle formation events are given. We found in total 270 (26% of the analysed days) and 226 (22% of the analysed days) particle formation days for negative and positive intermediate ions, respectively. For negatively charged particles we classified 411 (40% of the analysed days) undefined and 348 (34% of the analysed days) non-event days whereas for positively charged particles 343 (33% of the analysed days) undefined and 460 (45% of the analysed days) non-event days. The results were compared with the ordinary classification based on the Differential Mobility Particle Sizer (DMPS) measurements carried out at the same place. The above-presented values differed slightly from that found from the DMPS data, with a lower particle diameter of 3 nm. In addition, we have found the rain-induced intermediate ion bursts frequently. The rain effect was detected on 163 days by means of negative ions and on 105 days by positive ones. Another interesting phenomenon among the charged aerosol particles was the appearance and existence of intermediate ions during the snowfall. We observed this phenomenon 24 times with negatively charged particles and 21 times with positively charged ones during winter months (October–April). These intermediate air ions were seen during the snowfall and may be caused by ice crystals, although the origin of these intermediate ions is unclear at the moment.
Evaluation of a global aerosol microphysics model against size-resolved particle statistics in the marine atmosphere
Authors: Spracklen D. V. , Pringle K. J. , Carslaw K. S. , Mann G. W. , Manktelow P. , Heintzenberg J.
Published: April 2010

Abstract. A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP). We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed sub-micrometre size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10–30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the marine boundary layer (MBL). Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic MBL aerosol, with typically 60–90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of >120 h away from land. However, anthropogenic primary black carbon and organic carbon particles (at the emission size and quantity assumed here) do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the observed and modelled particle persistence at Cape Grim in the Southern Ocean, does not reveal a diurnal cycle consistent with a photochemically driven local particle source. We also show that a physically based cloud drop activation scheme better explains the observed change in accumulation mode geometric mean diameter with particle number.
Near-real time retrieval of tropospheric NO2 from OMI
Authors: Boersma K. F. , Eskes H. J. , Veefkind J. P. , Brinksma E. J. , van der A R. J. , Sneep M. , van den Oord G. H. J. , Levelt P. F. , Stammes P. , Gleason J. F. , Bucsela E. J.
Published: April 2010

Abstract. We present a new algorithm for the near-real time retrieval – within 3 h of the actual satellite measurement – of tropospheric NO2 columns from the Ozone Monitoring Instrument (OMI). The retrieval is based on the combined retrieval-assimilation-modelling approach developed at KNMI for off-line tropospheric NO2 from the GOME and SCIAMACHY satellite instruments. We have adapted the off-line system such that the required a priori information – profile shapes and stratospheric background NO2 – is now immediately available upon arrival (within 80 min of observation) of the OMI NO2 slant columns and cloud data at KNMI. Slant columns for NO2 are retrieved using differential optical absorption spectroscopy (DOAS) in the 405–465 nm range. Cloud fraction and cloud pressure are provided by a new cloud retrieval algorithm that uses the absorption of the O2-O2 collision complex near 477 nm. On-line availability of stratospheric slant columns and NO2 profiles is achieved by running the TM4 chemistry transport model (CTM) forward in time based on forecast ECMWF meteo and assimilated NO2 information from all previously observed orbits. OMI NO2 slant columns, after correction for spurious across-track variability, show a random error for individual pixels of approximately 0.7×1015 molec cm−2. Cloud parameters from OMI's O2-O2 algorithm have similar frequency distributions as retrieved from SCIAMACHY's Fast Retrieval Scheme for Cloud Observables (FRESCO) for August 2006. On average, OMI cloud fractions are higher by 0.011, and OMI cloud pressures exceed FRESCO cloud pressures by 60 hPa. A sequence of OMI observations over Europe in October 2005 shows OMI's capability to track changeable NOx air pollution from day to day in cloud-free situations.
Hygroscopic properties of ultrafine aerosol particles in the boreal forest: diurnal variation, solubility and the influence of sulfuric acid
Authors: Ehn M. , Petäjä T. , Aufmhoff H. , Aalto P. , Hämeri K. , Arnold F. , Laaksonen A. , Kulmala M.
Published: April 2010

Abstract. The hygroscopic growth of aerosol particles present in a boreal forest was measured at a relative humidity of 88%. Simultaneously the gas phase concentration of sulfuric acid, a very hygroscopic compound, was monitored. The focus was mainly on days with new particle formation by nucleation. The measured hygroscopic growth factors (GF) correlated positively with the gaseous phase sulfuric acid concentrations. The smaller the particles, the stronger the correlation, with r=0.20 for 50 nm and r=0.50 for 10 nm particles. The increase in GF due to condensing sulfuric acid is expected to be larger for particles with initially smaller masses. During new particle formation, the changes in solubility of the new particles were calculated during their growth to Aitken mode sizes. As the modal diameter increased, the solubility of the particles decreased. This indicated that the initial particle growth was due to more hygroscopic compounds, whereas the later growth during the evening and night was mainly caused by less hygroscopic or even hydrophobic compounds. For all the measured sizes, a diurnal variation in GF was observed both during days with and without particle formation. The GF was lowest at around midnight, with a mean value of 1.12–1.24 depending on particle size and if new particle formation occurred during the day, and increased to 1.25–1.34 around noon. This can be tentatively explained by day- and nighttime gas-phase chemistry; different vapors will be present depending on the time of day, and through condensation these compounds will alter the hygroscopic properties of the particles in different ways.
The atmospheric cycling of radiomethane and the "fossil fraction" of the methane source
Authors: Lassey K. R. , Lowe D. C. , Smith A. M.
Published: April 2010

Abstract. The cycling of 14CH4 ("radiomethane") through the atmosphere has been strongly perturbed in the industrial era by the release of 14C-free methane from geologic reservoirs ("fossil methane" emissions), and in the nuclear era, especially since ca 1970, by the direct release of nucleogenic radiomethane from nuclear power facilities. Contemporary measurements of atmospheric radiomethane have been used to estimate the proportion of fossil methane in the global methane source (the "fossil fraction"), but such estimates carry high uncertainty due to the ill-determined nuclear-power source. Guided by a mass-balance formulation in a companion paper, we apply a contemporary time series of atmospheric radiomethane to quantify both the fossil fraction and the strength of the nuclear power source. We deduce that 30.0±2.3% (1 s.d.) of the global methane source for 1986–2000 has fossil origin, a fraction which may include some 14C-depleted refractory carbon such as from aged peat deposits. Since this estimate depends upon the validity of assumptions underlying a linear regression model, it should be seen as providing a plausible re-estimate rather than a definitive revision. Such a fossil fraction would be much larger (by 50%) than is commonly accepted, with implications for inventory compilation. The co-estimated strength of the global nuclear-power source of radiomethane is consistent with values inferred independently from local nuclear facilities.
Observations and analysis of polar stratospheric clouds detected by POAM III and SAGE III during the SOLVE II/VINTERSOL campaign in the 2002/2003 Northern Hemisphere winter
Authors: Alfred J. , Fromm M. , Bevilacqua R. , Nedoluha G. , Strawa A. , Poole L. , Wickert J.
Published: April 2010

Abstract. The Polar Ozone and Aerosol Measurement and Stratospheric Aerosol and Gas Experiment instruments both observed high numbers of polar stratospheric clouds (PSCs) in the polar region during the second SAGE Ozone Loss and Validation (SOLVE II) and Validation of INTERnational Satellites and Study of Ozone Loss (VINTERSOL) campaign, conducted during the 2002/2003 Northern Hemisphere winter. Between 15 November 2002 (14 November 2002) and 18 March 2003 (21 March 2003) SAGE (POAM) observed 122 (151) aerosol extinction profiles containing PSCs. PSCs were observed on an almost daily basis, from early December through 15 January, in both instruments. No PSCs were observed from either instrument from 15 January until 4 February, and from then only sparingly in three periods in mid- and late February and mid-March. In early December, PSCs were observed in the potential temperature range from roughly 375 K to 750 K. Throughout December the top of this range decreases to near 600 K. In February and March, PSC observations were primarily constrained to potential temperatures below 500 K. The PSC observation frequency as a function of ambient temperature relative to the nitric acid-trihydrate saturation point (using a nitric acid profile prior to denitrification) was used to infer irreversible denitrification. By late December 38% denitrification was inferred at both the 400–475 K and 475–550 K potential temperature ranges. By early January extensive levels of denitrification near 80% were inferred at both potential temperature ranges, and the air remained denitrified at least through early March.
Comparison of measurements of peroxyacyl nitrates and primary carbonaceous aerosol concentrations in Mexico City determined in 1997 and 2003
Authors: Marley N. A. , Gaffney J. S. , Ramos-Villegas R. , Cárdenas González B.
Published: April 2010

Abstract. The concentrations of peroxyacetyl nitrate (PAN) in ambient air can be a good indicator of air quality and the effectiveness of control strategies for reducing ozone levels in urban areas. As PAN is formed by the oxidation of reactive hydrocarbons in the presence of nitrogen dioxide (NO2), it is a direct measure of the peroxyacyl radical levels produced from reactive organic emissions in the urban air shed. Carbon soot, known as black carbon (BC) or elemental carbon (EC), is a primary atmospheric aerosol species and is a good indicator of the levels of combustion emissions, particularly from diesel engines, in major cities. Mexico City is the second largest megacity in the world and has long suffered from poor air quality. Reported here are atmospheric measurements of PAN and BC obtained in Mexico City during the Mexico Megacity 2003 field study. These results are compared with measurements obtained earlier during the Investigación sobre Materia Particulada y Deterioro Atmosférico – Aerosol and Visibility Research (IMADA-AVER) campaign in 1997 to obtain an estimate of the changes in emissions in Mexico City and the effectiveness of control strategies adopted during that time. Concentrations of PAN in 1997 reached a maximum of 34 ppb with an average daily maximum of 15 ppb. The PAN levels recorded in 2003 were quite different, with an average daily maximum of 3 ppb. This dramatic reduction in PAN levels observed in 2003 indicate that reactive hydrocarbon emissions have been reduced in the city due to controls on olefins in liquefied petroleum gas (LPG) and also due to the significant number of newer vehicles with catalytic converters that have replaced older higher emission vehicles. In contrast, black/elemental carbon levels were similar in 1997 and 2003 indicating little improvement likely due to the lack of controls on diesel vehicles in the city. Thus, while air quality and ozone production have improved, Mexico City and other megacities continue to be a major source of black carbon aerosols, which can be an important species in determining regional radiative balance and climate.
Dangerous human-made interference with climate: a GISS modelE study
Authors: Hansen J. , Sato M. , Ruedy R. , Kharecha P. , Lacis A. , Miller R. , Nazarenko L. , Lo K. , Schmidt G. A. , Russell G. , Aleinov I. , Bauer S. , Baum E. , Cairns B. , Canuto V. , Chandler M. , Cheng Y. , Cohen A. , Del Genio A. , Faluvegi G. , Fleming E. , Friend A. , Hall T. , Jackman C. , Jonas J. , Kelley M. , Kiang N. Y. , Koch D. , Labow G. , Lerner J. , Menon S. , Novakov T. , Oinas V. , Perlwitz Ja. , Perlwitz Ju. , Rind D. , Romanou A. , Schmunk R. , Shindell D. , Stone P. , Sun S. , Streets D. , Tausnev N. , Thresher D. , Unger N. , Yao M. , Zhang S.
Published: April 2010

Abstract. We investigate the issue of "dangerous human-made interference with climate" using simulations with GISS modelE driven by measured or estimated forcings for 1880–2003 and extended to 2100 for IPCC greenhouse gas scenarios as well as the "alternative" scenario of Hansen and Sato (2004). Identification of "dangerous" effects is partly subjective, but we find evidence that added global warming of more than 1°C above the level in 2000 has effects that may be highly disruptive. The alternative scenario, with peak added forcing ~1.5 W/m2 in 2100, keeps further global warming under 1°C if climate sensitivity is ~3°C or less for doubled CO2. The alternative scenario keeps mean regional seasonal warming within 2σ (standard deviations) of 20th century variability, but other scenarios yield regional changes of 5–10σ, i.e. mean conditions outside the range of local experience. We conclude that a CO2 level exceeding about 450 ppm is "dangerous", but reduction of non-CO2 forcings can provide modest relief on the CO2 constraint. We discuss three specific sub-global topics: Arctic climate change, tropical storm intensification, and ice sheet stability. We suggest that Arctic climate change has been driven as much by pollutants (O3, its precursor CH4, and soot) as by CO2, offering hope that dual efforts to reduce pollutants and slow CO2 growth could minimize Arctic change. Simulated recent ocean warming in the region of Atlantic hurricane formation is comparable to observations, suggesting that greenhouse gases (GHGs) may have contributed to a trend toward greater hurricane intensities. Increasing GHGs cause significant warming in our model in submarine regions of ice shelves and shallow methane hydrates, raising concern about the potential for accelerating sea level rise and future positive feedback from methane release. Growth of non-CO2 forcings has slowed in recent years, but CO2 emissions are now surging well above the alternative scenario. Prompt actions to slow CO2 emissions and decrease non-CO2 forcings are required to achieve the low forcing of the alternative scenario.
Mid-latitude ozone changes: studies with a 3-D CTM forced by ERA-40 analyses
Authors: Feng W. , Chipperfield M. P. , Dorf M. , Pfeilsticker K. , Ricaud P.
Published: April 2010

Abstract. We have used an off-line three-dimensional (3-D) chemical transport model (CTM) to study long-term changes in stratospheric O3. The model was run from 1977–2004 and forced by ECMWF ERA-40 and operational analyses. Model runs were performed to examine the impact of increasing halogens and additional stratospheric bromine from short-lived source gases. The analyses capture much of the observed interannual variability in column ozone, but there are also unrealistic features. In particular the ERA-40 analyses cause a large positive anomaly in northern hemisphere (NH) column O3 in the late 1980s. Also, the change from ERA-40 to operational winds at the start of 2002 introduces abrupt changes in some model fields (e.g. temperature, ozone) which affect analysis of trends. The model reproduces the observed column increase in NH mid-latitudes from the mid 1990s. Analysis of a run with fixed halogens shows that this increase is not due to a significant decrease in halogen-induced loss, i.e. is not an indication of recovery. The model predicts only a small decrease in halogen-induced loss after 1999. In the upper stratosphere, despite the modelled turnover of chlorine around 1999, O3 does not increase because of the effects of increasing ECMWF temperatures, decreasing modelled CH4 at this altitude, and abrupt changes in the SH temperatures at the end of the ERA-40 period. The impact of an additional 5 pptv stratospheric bromine from short-lived species decreases mid-latitude column O3 by about 10 DU. However, the impact on the modelled relative O3 anomaly is generally small except during periods of large volcanic loading.
Observationally derived transport diagnostics for the lowermost stratosphere and their application to the GMI chemistry and transport model
Authors: Strahan S. E. , Duncan B. N. , Hoor P.
Published: April 2010

Abstract. Transport from the surface to the lowermost stratosphere (LMS) can occur on timescales of a few months or less, making it possible for short-lived tropospheric pollutants to influence stratospheric composition and chemistry. Models used to study this influence must demonstrate the credibility of their chemistry and transport in the upper troposphere and lower stratosphere (UT/LS). Data sets from satellite and aircraft instruments measuring CO, O3, N2O, and CO2 in the UT/LS are used to create a suite of diagnostics for the seasonally-varying transport into and within the lowermost stratosphere, and of the coupling between the troposphere and stratosphere in the extratropics. The diagnostics are used to evaluate a version of the Global Modeling Initiative (GMI) Chemistry and Transport Model (CTM) that uses a combined tropospheric and stratospheric chemical mechanism and meteorological fields from the GEOS-4 general circulation model. The diagnostics derived from N2O and O3 show that the model lowermost stratosphere has realistic input from the overlying high latitude stratosphere in all seasons. Diagnostics for the LMS show two distinct layers. The upper layer begins ~30 K potential temperature above the tropopause and has a strong annual cycle in its composition. The lower layer is a mixed region ~30 K thick near the tropopause that shows no clear seasonal variation in the degree of tropospheric coupling. Diagnostics applied to the GMI CTM show credible seasonally-varying transport in the LMS and a tropopause layer that is realistically coupled to the UT in all seasons. The vertical resolution of the GMI CTM in the UT/LS, ~1 km, is sufficient to realistically represent the extratropical tropopause layer. This study demonstrates that the GMI CTM has the transport credibility required to study the impact of tropospheric emissions on the stratosphere.
Diurnal variation of upper tropospheric humidity and its relations to convective activities over tropical Africa
Authors: Chung E. S. , Sohn B. J. , Schmetz J. , Koenig M.
Published: April 2010

Abstract. Diurnal variations of upper tropospheric humidity (UTH) as well as middle tropospheric humidity (MTH) were examined in conjunction with the diurnal cycle of convection over tropical Africa and the adjacent tropical Atlantic Ocean using Meteosat-8 measurements. Cloud and humidity features were also tracked to document the diurnal variations of humidity and clouds in the Lagrangian framework. A distinct diurnal variation of UTH (and MTH) is noted over regions where tropical deep convective cloud systems are commonly observed. The amplitude of the UTH diurnal variation is larger over land, while its variations over convectively inactive subtropical regions are much smaller. The diurnal variation of UTH tends to reach a maximum during nighttime over land, lagging deep convection and high cloud whose maxima occurred in the late afternoon and evening, respectively. It was revealed that these diurnal variations over the African continent are likely associated with continental-scale daytime solar heating and topography, in which topographically-induced signals develop earlier around the mid-afternoon and merge into stronger and broader continental-scale convection clusters later, forming a precipitation maximum in the late afternoon. It was also revealed that advection effect on the diurnal variation appears to be insignificant.
On the diurnal variability of particle properties related to light absorbing carbon in Mexico City
Authors: Baumgardner D. , Kok G. L. , Raga G. B.
Published: April 2010

Abstract. The mass of light absorbing carbon (LAC) in individual, internally mixed aerosol particles was measured with the Single Particle Soot Photometer (SP2) in April of 2003 and 2005 and evaluated with respect to concentrations of carbon monoxide (CO), particle bound polycyclic aromatic hydrocarbons (PPAH) and condensation nuclei (CN). The LAC and CO have matching diurnal trends that are linked to traffic patterns and boundary layer growth. The PPAH reaches a maximum at the same time as CO and LAC but returns rapidly back to nighttime values within three hours of the peak. The number of particles containing LAC ranges between 10% to 40% of all particles between 150 nm and 650 nm and the mass is between 5% and 25% of the total mass in this size range. The average LAC equivalent mass diameter varies between 160 and 230 nm and the thinnest coating of non-light absorbing material is observed during periods of maximum LAC mass. The coating varies between 10 nm and 30 nm during the day, but is a strong function of particle size. The mass absorption cross sections, σabs, derived from the SP2, are 5.0±0.2 m2g−1 and 4.8±0.2 m2g−1, dependent on the optical model used to describe LAC mixtures. The LAC contributes up to 50% of the total light extinction in the size range from 100 nm to 400 nm. The estimated emission rate of LAC is 1200 metric tons per year in Mexico City, based upon the SP2 measurements and correlations between LAC and CO.
Size-segregated mass distributions of aerosols over Eastern Mediterranean: seasonal variability and comparison with AERONET columnar size-distributions
Authors: Gerasopoulos E. , Koulouri E. , Kalivitis N. , Kouvarakis G. , Saarikoski S. , Mäkelä T. , Hillamo R. , Mihalopoulos N.
Published: April 2010

Abstract. This work provides long-term (2004–2006) size segregated measurements of aerosol mass at a remote coastal station in the southern Europe, with the use of size-selective samplings (SDI impactor). Seven distinct modes were identified in the range 0–10 µm and the dominant were the "Accumulation 1" (0.25–0.55 µm) and the "Coarse 2" (3–7 µm) modes. The seasonal characteristics of each mode were thoroughly studied and different sources for submicron and supermicron particles were identified, the first being related to local/regional and transported pollution with maximum in summer and the latter to dust from deserted areas in Northern Africa maximizing in spring. On average, PM2.5 and PM1 accounted for 60% and 40% of PM10 mass, respectively.The representativity of the ground-based measurements for the total column was also investigated by comparing the measured aerosol mass distributions with the AERONET volume size distribution data. Similar seasonal patterns were revealed and AERONET was found adequate for the estimation of background levels of both fine and coarse particles near surface, with certain limitations in the case of pollution or dust abrupt episodes due to its low temporal coverage.
Evaluation of ozonesondes, HALOE, SAGE II and III, Odin- OSIRIS and -SMR, and ENVISAT-GOMOS, -SCIAMACHY and -MIPAS ozone profiles in the tropics from SAOZ long duration balloon measurements in 2003 and 2004
Authors: Borchi F. , Pommereau J.-P.
Published: April 2010

Abstract. The performances of satellite and sondes ozone measuring instruments available in the tropics between 10 and 26 km during the southern hemisphere summer in 2003 and 2004, have been investigated by comparison with series of profiles obtained by solar occultation in the visible Chappuis bands using a SAOZ UV-Vis spectrometer carried by long duration balloons. When compared to SAOZ, systematic positive or negative altitude shifts are observed in the satellite profiles, varying from <50 m for the GOMOS v6.0b stellar occultation instrument, followed by +100/200 m for solar occultation systems (SAGE II v6.2, HALOE v19 above 22 km), but as large as −900 m for the OSIRIS limb viewing system. The ozone relative biases are generally limited, between −4% and +4%, for measurements in the visible Chappuis bands (SAGE II and SAGE III moon v3, GOMOS above 22 km and OSIRIS), the near IR (HALOE above 22 km) and the ozonesondes, but increase to +5.5% (SCIAMACHY IUP v1.63) though still in the visible, and +7% in the mid-IR (MIPAS NL v4.61) and the submillimetric range (SMR v222). Regarding precision, evaluated statistically from the zonal variability of ozone concentration, the best measurements are found to be those of SAGE II (2%), followed by HALOE above 22 km (3–4%), then the ozonesondes, SAGE III moon, SCIAMACHY and OSIRIS (4–5%), GOMOS above 22 km (~6%), MIPAS (8.5%) and finally SMR (16%). Overall, all satellite ozone measurements appear to be of little utility in the tropical troposphere except those of SAGE II (and eventually SAGE III), though low biased by 50% and of limited (50%) precision.
Global cloud and precipitation chemistry and wet deposition: tropospheric model simulations with ECHAM5/MESSy1
Authors: Tost H. , Jöckel P. , Kerkweg A. , Pozzer A. , Sander R. , Lelieveld J.
Published: April 2010

Abstract. The representation of cloud and precipitation chemistry and subsequent wet deposition of trace constituents in global atmospheric chemistry models is associated with large uncertainties. To improve the simulated trace gas distributions we apply the new submodel SCAV, which includes detailed cloud and precipitation chemistry and present results of the atmospheric chemistry general circulation model ECHAM5/MESSy1. A good agreement with observed wet deposition fluxes for species causing acid rain is obtained. The new scheme enables prognostic calculations of the pH of clouds and precipitation, and these results are also in accordance with observations. We address the influence of detailed cloud and precipitation chemistry on trace constituents based on sensitivity simulations. The results confirm previous results from regional scale and box models, and we extend the analysis to the role of aqueous phase chemistry on the global scale. Some species are directly affected through multiphase removal processes, and many also indirectly through changes in oxidant concentrations, which in turn have an impact on the species lifetime. While the overall effect on tropospheric ozone is relatively small (<10%), regional effects on O3 can reach ≈20%, and several important compounds (e.g., H2O2, HCHO) are substantially depleted by clouds and precipitation.
Effective UV surface albedo of seasonally snow-covered lands
Authors: Tanskanen A. , Manninen T.
Published: April 2010

Abstract. At ultraviolet wavelengths the albedo of most natural surfaces is small with the striking exception of snow and ice. Therefore, snow cover is a major challenge for various applications based on radiative transfer modelling. The aim of this work was to determine the characteristic effective UV range surface albedo of various land cover types when covered by snow. First we selected 1 by 1 degree sample regions that met three criteria: the sample region contained dominantly subpixels of only one land cover type according to the 8 km global land cover classification product from the University of Maryland; the average slope of the sample region was less than 2 degrees according to the USGS's HYDRO1K slope data; the sample region had snow cover in March according to the NSIDC Northern Hemisphere weekly snow cover data. Next we generated 1 by 1 degree gridded 360 nm surface albedo data from the Nimbus-7 TOMS Lambertian equivalent reflectivity data, and used them to construct characteristic effective surface albedo distributions for each land cover type. The resulting distributions showed that each land cover type experiences a characteristic range of surface albedo values when covered by snow. The result is explained by the vegetation that extends upward beyond the snow cover and masks the bright snow covered surface.
Evidence for a CO increase in the SH during the 20th century based on firn air samples from Berkner Island, Antarctica
Authors: Assonov S. S. , Brenninkmeijer C. A. M. , Jöckel P. , Mulvaney R. , Bernard S. , Chappellaz J.
Published: April 2010

Abstract. Trends of carbon monoxide (CO) for the past 100 years are reported as derived from Antarctic firn drilling expeditions. Only one of 3 campaigns provided high quality results. The trend was reconstructed using a firn air model in the forward mode to constrain age distributions and assuming the CO increase to be proportional to its major source, namely CH4. The results suggest that CO has increased by ~38%, from 38±7 to 52.5±1.5 ppbv over a period of roughly 100 years. The concentrations are on the volumetric scale which corresponds to ~1.08 of the scale used by NOAA/CMDL. The estimated CO increase is somewhat larger than what is estimated from the CO budget estimations and the CH4 growth alone. The most likely explanation might be an increase in biomass burning emissions. Using CH3Cl as another proxy produces a very similar reconstruction.
Technical Note: The heterogeneous Zeldovich factor
Authors: Vehkamäki H. , Määttänen A. , Lauri A. , Napari I. , Kulmala M.
Published: April 2010

Abstract. In this technical note we present the exact form of the Zeldovich factor for heterogeneous nucleation on spherical pre-existing particles. We study the error caused by planar pre-existing surface approximations, which have been used in our earlier heterogeneous nucleation model and elsewhere in the literature. We also test the significance of widely used approximations for cluster surface area and circumference. We conclude that the approximations do not affect the predicted onset saturation. Especially for small pre-existing particles the nucleation rates calculated with the exact and approximative models differ significantly.
Process-based estimates of terrestrial ecosystem isoprene emissions: incorporating the effects of a direct CO2-isoprene interaction
Authors: Arneth A. , Niinemets Ü. , Pressley S. , Bäck J. , Hari P. , Karl T. , Noe S. , Prentice I. C. , Serça D. , Hickler T. , Wolf A. , Smith B.
Published: April 2010

Abstract. In recent years evidence has emerged that the amount of isoprene emitted from a leaf is affected by the CO2 growth environment. Many – though not all – laboratory experiments indicate that emissions increase significantly at below-ambient CO2 concentrations and decrease when concentrations are raised to above-ambient. A small number of process-based leaf isoprene emission models can reproduce this CO2 stimulation and inhibition. These models are briefly reviewed, and their performance in standard conditions compared with each other and to an empirical algorithm. One of the models was judged particularly useful for incorporation into a dynamic vegetation model framework, LPJ-GUESS, yielding a tool that allows the interactive effects of climate and increasing CO2 concentration on vegetation distribution, productivity, and leaf and ecosystem isoprene emissions to be explored. The coupled vegetation dynamics-isoprene model is described and used here in a mode particularly suited for the ecosystem scale, but it can be employed at the global level as well. Annual and/or daily isoprene emissions simulated by the model were evaluated against flux measurements (or model estimates that had previously been evaluated with flux data) from a wide range of environments, and agreement between modelled and simulated values was generally good. By using a dynamic vegetation model, effects of canopy composition, disturbance history, or trends in CO2 concentration can be assessed. We show here for five model test sites that the suggested CO2-inhibition of leaf-isoprene metabolism can be large enough to offset increases in emissions due to CO2-stimulation of vegetation productivity and leaf area growth. When effects of climate change are considered atop the effects of atmospheric composition the interactions between the relevant processes will become even more complex. The CO2-isoprene inhibition may have the potential to significantly dampen the expected steep increase of ecosystem isoprene emission in a future, warmer atmosphere with higher CO2 levels; this effect raises important questions for projections of future atmospheric chemistry, and its connection to the terrestrial vegetation and carbon cycle.