Items

Advanced search

Parameterization of subgrid plume dilution for use in large-scale atmospheric simulations

A new model of plume dynamics has been developed for use as a subgrid model of plume dilution in a large-scale atmospheric simulation. The model uses mean wind, shear, and diffusion parameters derived from the local large-scale variables to advance the plume cross-sectional shape and area in time. Comparisons with a large eddy simulation of aircraft emission plume dynamics, with an analytical solution to the dynamics of a sheared Gaussian plume, and with measurements of aircraft exhaust plume dilution at cruise altitude show good agreement with these previous studies. We argue that the model also provides a reasonable approximation of line-shaped contrail dilution and give an example of how it can be applied in a global climate model.
Widening the gap between measurement and modelling of secondary organic aerosol properties?

The link between measured sub-saturated hygroscopicity and cloud activation potential of secondary organic aerosol particles produced by the chamber photo-oxidation of α-pinene in the presence or absence of ammonium sulphate seed aerosol was investigated using two models of varying complexity. A simple single hygroscopicity parameter model and a more complex model (incorporating surface effects) were used to assess the detail required to predict the cloud condensation nucleus (CCN) activity from the sub-saturated water uptake. Sub-saturated water uptake measured by three hygroscopicity tandem differential mobility analyser (HTDMA) instruments was used to determine the water activity for use in the models. The predicted CCN activity was compared to the measured CCN activation potential using a continuous flow CCN counter. Reconciliation using the more complex model formulation with measured cloud activation could be achieved widely different assumed surface tension behavior of the growing droplet; this was entirely determined by the instrument used as the source of water activity data. This unreliable derivation of the water activity as a function of solute concentration from sub-saturated hygroscopicity data indicates a limitation in the use of such data in predicting cloud condensation nucleus behavior of particles with a significant organic fraction. Similarly, the ability of the simpler single parameter model to predict cloud activation behaviour was dependent on the instrument used to measure sub-saturated hygroscopicity and the relative humidity used to provide the model input. However, agreement was observed for inorganic salt solution particles, which were measured by all instruments in agreement with theory. The difference in HTDMA data from validated and extensively used instruments means that it cannot be stated with certainty the detail required to predict the CCN activity from sub-saturated hygroscopicity. In order to narrow the gap between measurements of hygroscopic growth and CCN activity the processes involved must be understood and the instrumentation extensively quality assured. It is impossible to say from the results presented here due to the differences in HTDMA data whether: i) Surface tension suppression occurs ii) Bulk to surface partitioning is important iii) The water activity coefficient changes significantly as a function of the solute concentration.
Sources of uncertainties in modelling black carbon at the global scale

Our understanding of the global black carbon (BC) cycle is essentially qualitative due to uncertainties in our knowledge of its properties. This work investigates two source of uncertainties in modelling black carbon: those due to the use of different schemes for BC ageing and its removal rate in the global Transport-Chemistry model TM5 and those due to the uncertainties in the definition and quantification of the observations, which propagate through to both the emission inventories, and the measurements used for the model evaluation. The schemes for the atmospheric processing of black carbon that have been tested with the model are (i) a simple approach considering BC as bulk aerosol and a simple treatment of the removal with fixed 70% of in-cloud black carbon concentrations scavenged by clouds and removed when rain is present and (ii) a more complete description of microphysical ageing within an aerosol dynamics model, where removal is coupled to the microphysical properties of the aerosol, which results in a global average of 40% in-cloud black carbon that is scavenged in clouds and subsequently removed by rain, thus resulting in a longer atmospheric lifetime. This difference is reflected in comparisons between both sets of modelled results and the measurements. Close to the sources, both anthropogenic and vegetation fire source regions, the model results do not differ significantly, indicating that the emissions are the prevailing mechanism determining the concentrations and the choice of the aerosol scheme does not influence the levels. In more remote areas such as oceanic and polar regions the differences can be orders of magnitude, due to the differences between the two schemes. The more complete description reproduces the seasonal trend of the black carbon observations in those areas, although not always the magnitude of the signal, while the more simplified approach underestimates black carbon concentrations by orders of magnitude. The sensitivity to wet scavenging has been tested by varying in-cloud and below-cloud removal. BC lifetime increases by 10% when large scale and convective scale precipitation removal efficiency are reduced by 30%, while the variation is very small when below-cloud scavenging is zero. Since the emission inventories are representative of elemental carbon-like substance, the model output should be compared to elemental carbon measurements and if known, the ratio of black carbon to elemental carbon mass should be taken into account when the model is compared with black carbon observations.
On the seasonal dependence of tropical lower-stratospheric temperature trends

This study examines the seasonality of tropical lower-stratospheric temperature trends using the Microwave Sounding Unit lower-stratospheric channel (T4) for 1980–2008. We present evidence that this seasonality is largely a response to changes in the Brewer-Dobson circulation (BDC) driven by extratropical wave forcing. We show how the tropical T4 trend can be used as an indicator of changes in the BDC, and find that the BDC is strengthening for 1980–2008 in June–November related to the Southern Hemisphere (SH) and in December–February to the Northern Hemisphere (NH). In marked contrast, we find that the BDC is weakening in March–May, apparently because of a weakening of its northern cell. The novel observational evidence on the seasonal dependence of the BDC trends presented in this study has important implications for the understanding of climate change in the stratosphere as well as testing climate model simulations.
The global SF6 source inferred from long-term high precision atmospheric measurements and its comparison with emission inventories

Emissions of sulphur hexafluoride (SF6), one of the strongest greenhouse gases on a per molecule basis, are targeted to be collectively reduced under the Kyoto Protocol. Because of its long atmospheric lifetime (estimated as 800 to 3200 years), the accumulation of SF6 in the atmosphere is a direct measure of its global emissions. Examination of our extended data set of globally distributed high-precision SF6 observations shows an increase in SF6 abundance from near zero in the 1970s to a global mean of 6.7 ppt by the end of 2008. In-depth evaluation of our long-term data records shows that the global source of SF6 decreased after 1995, most likely due to SF6 emission reductions in industrialised countries, but increased again after 1998. By subtracting those emissions reported by Annex I countries to the United Nations Framework Convention of Climatic Change (UNFCCC) from our observation-inferred SF6 source leaves a surprisingly large gap of more than 70–80% of non-reported SF6 emissions in the last decade. This suggests a strong under-estimation of emissions in Annex I countries and underlines the urgent need for independent atmospheric verification of greenhouse gases emissions accounting.
Homogeneous nucleation of sulfuric acid and water mixture: experimental setup and first results

In this study we introduce a new flow tube suitable for binary and ternary homogeneous nucleation studies. The production of sulfuric acid and water vapor mixture, the experimental setup and the method of sulfuric acid concentration determination are discussed in detail. Wall losses were estimated from the measured sulfuric acid concentration profiles along the flow tube and compared to a theoretical prediction. In this investigation the experimental evidence of new particle formation was observed at a concentration of 109 molecules cm−3 of sulfuric acid and the nucleation rates measured at three relative humidities (RH) 10, 30 and 50%, cover six orders of magnitude, from 10−3 to 103 particles cm−3. Particle free air was used as a carrier gas. Our initial results are compared to the theoretical prediction of binary homogeneous nucleation, to results obtained by other investigators, and to atmospheric nucleation.
Corrigendum to "Estimates of biomass burning emissions in tropical Asia based on satellite-derived data" published in Atmos. Chem. Phys., 10, 2335–2351, 2010
Molecular characterization of urban organic aerosol in tropical India: contributions of primary emissions and secondary photooxidation

Organic molecular composition of PM10 samples, collected at Chennai in tropical India, was studied using capillary gas chromatography/mass spectrometry. Fourteen organic compound classes were detected in the aerosols, including aliphatic lipids, sugar compounds, lignin products, terpenoid biomarkers, sterols, aromatic acids, hydroxy-/polyacids, phthalate esters, hopanes, Polycyclic Aromatic Hydrocarbons (PAHs), and photooxidation products from biogenic Volatile Organic Compounds (VOCs). At daytime, phthalate esters were found to be the most abundant compound class; however, at nighttime, fatty acids were the dominant one. Di-(2-ethylhexyl) phthalate, C16 fatty acid, and levoglucosan were identified as the most abundant single compounds. The nighttime maxima of most organics in the aerosols indicate a land/sea breeze effect in tropical India, although some other factors such as local emissions and long-range transport may also influence the composition of organic aerosols. However, biogenic VOC oxidation products (e.g., 2-methyltetrols, pinic acid, 3-hydroxyglutaric acid and β-caryophyllinic acid) showed diurnal patterns with daytime maxima. Interestingly, terephthalic acid was maximized at nighttime, which is different from those of phthalic and isophthalic acids. A positive relation was found between 1,3,5-triphenylbenzene (a tracer for plastic burning) and terephthalic acid, suggesting that the field burning of municipal solid wastes including plastics is a significant source of terephthalic acid. Organic compounds were further categorized into several groups to clarify their sources. Fossil fuel combustion (24–43%) was recognized as the most significant source for the total identified compounds, followed by plastic emission (16–33%), secondary oxidation (8.6–23%), and microbial/marine sources (7.2–17%). In contrast, the contributions of terrestrial plant waxes (5.9–11%) and biomass burning (4.2–6.4%) were relatively small. This study demonstrates that, in addition to fossil fuel combustion and biomass burning, the open-burning of plastics in urban area also contributes to the organic aerosols in South Asia.
Atmospheric nitrogen budget in Sahelian dry savannas

The atmospheric nitrogen budget depends on emission and deposition fluxes both as reduced and oxidized nitrogen compounds. In this study, a first attempt at estimating the Sahel nitrogen budget for the year 2006 is made, through measurements and simulations at three stations from the IDAF network situated in dry savanna ecosystems. Dry deposition fluxes are estimated from measurements of NO2, HNO3 and NH3 gaseous concentrations and from simulated dry deposition velocities, and wet deposition fluxes are calculated from NH4+ and NO3− concentrations in samples of rain. Emission fluxes are estimated including biogenic emission of NO from soils (an Artificial Neural Network module has been inserted into the ISBA-SURFEX surface model), emission of NOx and NH3 from domestic fires and biomass burning, and volatilization of NH3 from animal excreta. Uncertainties are calculated for each contribution of the budget. This study uses original and unique data from remote and hardly-ever-explored regions.The monthly evolution of oxidized N compounds shows that emission and deposition increase at the beginning of the rainy season because of large emissions of biogenic NO (pulse events). Emission of oxidized compounds is dominated by biogenic emission from soils (domestic fires and biomass burning of oxidized compounds account for 0 to 13% at the most at the annual scale, depending on the station), whereas emission of NH3 is dominated by the process of volatilization from soils. At the annual scale, the average gaseous dry deposition accounts for 47% of the total estimated deposition flux, for both oxidized and reduced compounds. The average estimated wet plus dry deposition flux in dry savanna ecosystems is 7.5±1.8 kgN ha−1 yr−1, with approximately 30% attributed to oxidized compounds, and the rest attributed to NHx. The average estimated emission flux ranges from 8.4(±3.8) to 12.4(±5.9) kgN ha−1 yr−1, dominated by NH3 volatilization (72–82%) and biogenic emission from soils (11–17%), depending on the applied volatilization rate of NH3. While larger, emission fluxes are on the same order of magnitude as deposition fluxes. The main uncertainties are linked to the NH3 emission from volatilization. When scaled up from the 3 measurement sites to the Sahelian region (12° N:18° N, 15° W:10° E), the estimated total emission ranges from 2(±0.9) to 3(±1.4) TgN yr−1, depending on the applied volatilization rate of NH3 and estimated total deposition is 1.8(±0.4) TgN yr−1. The dry savanna ecosystems of the Sahel contribute around 2% to the global (biogenic + anthropogenic) nitrogen budget.
First climatology of polar mesospheric clouds from GOMOS/ENVISAT stellar occultation instrument

GOMOS (Global Ozone Monitoring by Occultation of Stars), on board the European platform ENVISAT launched in 2002, is a stellar occultation instrument combining four spectrometers and two fast photometers which measure light at 1 kHz sampling rate in the two visible channels 470–520 nm and 650–700 nm. On the day side, GOMOS does not measure only the light from the star, but also the solar light scattered by the atmospheric molecules. In the summer polar days, Polar Mesospheric Clouds (PMC) are clearly detected using the photometers signals, as the solar light scattered by the cloud particles in the instrument field of view. The sun-synchronous orbit of ENVISAT allows observing PMC in both hemispheres and the stellar occultation technique ensures a very good geometrical registration. Four years of data, from 2002 to 2006, are analyzed up to now. GOMOS data set consists of approximately 10 000 cloud observations all over the eight PMC seasons studied. The first climatology obtained by the analysis of this data set is presented, focusing on the seasonal and latitudinal coverage, represented by global maps. GOMOS photometers allow a very sensitive PMC detection, showing a frequency of occurrence of 100% in polar regions during the middle of the PMC season. According to this work mesospheric clouds seem to be more frequent in the Northern Hemisphere than in the Southern Hemisphere. The PMC altitude distribution was also calculated. The obtained median values are 82.7 km in the North and 83.2 km in the South.