Urban smoke concentrations at Kew, London, 1898-2004

Historical smoke concentrations at monthly resolution for the early twentieth century are found for Kew Observatory, London, using the atmospheric electricity proxy technique. Smoke particles modify the electrical properties of urban air: an increase in smoke concentration reduces air's electrical conductivity and increases the Potential Gradient (PG). Calibrated PG data are available from Kew since 1898, and air conductivity was measured routinely between 1909 and 1979 using the technique developed by C.T.R. Wilson. Automated smoke observations at the same site overlap with the atmospheric electrical measurements from 1921, providing an absolute calibration to smoke concentration. This shows that the late nineteenth century winter smoke concentrations at Kew were approximately 100 times greater than contemporary winter smoke concentrations. Following smoke emission regulations reducing the smoke concentration, the electrical parameters of the urban air did not change dramatically. This is suggested to be due to a composition change, with an increase in the abundance of small aerosol compensating for the decrease in smoke. (c) 2006 Elsevier Ltd. All rights reserved.

Observational constraints on past attributable warming and predictions of future global warming

This paper investigates the impact of aerosol forcing uncertainty on the robustness of estimates of the twentieth-century warming attributable to anthropogenic greenhouse gas emissions. Attribution analyses on three coupled climate models with very different sensitivities and aerosol forcing are carried out. The Third Hadley Centre Coupled Ocean - Atmosphere GCM (HadCM3), Parallel Climate Model (PCM), and GFDL R30 models all provide good simulations of twentieth-century global mean temperature changes when they include both anthropogenic and natural forcings. Such good agreement could result from a fortuitous cancellation of errors, for example, by balancing too much ( or too little) greenhouse warming by too much ( or too little) aerosol cooling. Despite a very large uncertainty for estimates of the possible range of sulfate aerosol forcing obtained from measurement campaigns, results show that the spatial and temporal nature of observed twentieth-century temperature change constrains the component of past warming attributable to anthropogenic greenhouse gases to be significantly greater ( at the 5% level) than the observed warming over the twentieth century. The cooling effects of aerosols are detected in all three models. Both spatial and temporal aspects of observed temperature change are responsible for constraining the relative roles of greenhouse warming and sulfate cooling over the twentieth century. This is because there are distinctive temporal structures in differential warming rates between the hemispheres, between land and ocean, and between mid- and low latitudes. As a result, consistent estimates of warming attributable to greenhouse gas emissions are obtained from all three models, and predictions are relatively robust to the use of more or less sensitive models. The transient climate response following a 1% yr(-1) increase in CO2 is estimated to lie between 2.2 and 4 K century(-1) (5-95 percentiles).

Boundary layer structure and decoupling from synoptic scale flow during NAMBLEX

This paper presents an overview of the meteorology and planetary boundary layer structure observed during the NAMBLEX field campaign to aid interpretation of the chemical and aerosol measurements. The campaign has been separated into five periods corresponding to the prevailing synoptic condition. Comparisons between meteorological measurements ( UHF wind profiler, Doppler sodar, sonic aneometers mounted on a tower at varying heights and a standard anemometer) and the ECMWF analysis at 10 m and 1100 m identified days when the internal boundary layer was decoupled from the synoptic flow aloft. Generally the agreement was remarkably good apart from during period one and on a few days during period four when the diurnal swing in wind direction implies a sea/land breeze circulation near the surface. During these periods the origin of air sampled at Mace Head would not be accurately represented by back trajectories following the winds resolved in ECMWF analyses. The wind profiler observations give a detailed record of boundary layer structure including an indication of its depth, average wind speed and direction. Turbulence statistics have been used to assess the height to which the developing internal boundary layer, caused by the increased surface drag at the coast, reaches the sampling location under a wide range of marine conditions. Sampling conducted below 10 m will be impacted by emission sources at the shoreline in all wind directions and tidal conditions, whereas sampling above 15 m is unlikely to be affected in any of the wind directions and tidal heights sampled during the experiment.

Quasi-biennial oscillation and tracer distributions in a coupled chemistry-climate model

[ 1] We have used a fully coupled chemistry-climate model (CCM), which generates its own wind and temperature quasi-biennial oscillation (QBO), to study the effect of coupling on the QBO and to examine the QBO signals in stratospheric trace gases, particularly ozone. Radiative coupling of the interactive chemistry to the underlying general circulation model tends to prolong the QBO period and to increase the QBO amplitude in the equatorial zonal wind in the lower and middle stratosphere. The model ozone QBO agrees well with Stratospheric Aerosol and Gas Experiment II and Total Ozone Mapping Spectrometer satellite observations in terms of vertical and latitudinal structure. The model captures the ozone QBO phase change near 28 km over the equator and the column phase change near +/- 15 degrees latitude. Diagnosis of the model chemical terms shows that variations in NOx are the main chemical driver of the O-3 QBO around 35 km, i.e., above the O-3 phase change.

Krakatoa lives: The effect of volcanic eruptions on ocean heat content and thermal expansion

A suite of climate model experiments indicates that 20th Century increases in ocean heat content and sea-level ( via thermal expansion) were substantially reduced by the 1883 eruption of Krakatoa. The volcanically-induced cooling of the ocean surface is subducted into deeper ocean layers, where it persists for decades. Temporary reductions in ocean heat content associated with the comparable eruptions of El Chichon ( 1982) and Pinatubo ( 1991) were much shorter lived because they occurred relative to a non-stationary background of large, anthropogenically-forced ocean warming. Our results suggest that inclusion of the effects of Krakatoa ( and perhaps even earlier eruptions) is important for reliable simulation of 20th century ocean heat uptake and thermal expansion. Inter-model differences in the oceanic thermal response to Krakatoa are large and arise from differences in external forcing, model physics, and experimental design. Systematic experimentation is required to quantify the relative importance of these factors. The next generation of historical forcing experiments may require more careful treatment of pre-industrial volcanic aerosol loadings.

Changes in the global sulfate burden due to perturbations in global CO2 concentrations

A large ensemble of general circulation model (GCM) integrations coupled to a fully interactive sulfur cycle scheme were run on the climateprediction.net platform to investigate the uncertainty in the climate response to sulfate aerosol and carbon dioxide (CO2) forcing. The sulfate burden within the model (and the atmosphere) depends on the balance between formation processes and deposition (wet and dry). The wet removal processes for sulfate aerosol are much faster than dry removal and so any changes in atmospheric circulation, cloud cover, and precipitation will feed back on the sulfate burden. When CO2 is doubled in the Hadley Centre Slab Ocean Model (HadSM3), global mean precipitation increased by 5%; however, the global mean sulfate burden increased by 10%. Despite the global mean increase in precipitation, there were large areas of the model showing decreases in precipitation (and cloud cover) in the Northern Hemisphere during June–August, which reduced wet deposition and allowed the sulfate burden to increase. Further experiments were also undertaken with and without doubling CO2 while including a future anthropogenic sulfur emissions scenario. Doubling CO2 further enhanced the increases in sulfate burden associated with increased anthropogenic sulfur emissions as observed in the doubled CO2-only experiment. The implications are that the climate response to doubling CO2 can influence the amount of sulfate within the atmosphere and, despite increases in global mean precipitation, may act to increase it.

The development of a new dust uplift scheme in the Met Office Unified Model

Aeolian mineral dust aerosol is an important consideration in the Earth's radiation budget as well as a source of nutrients to oceanic and land biota. The modelling of aeolian mineral dust has been improving consistently despite the relatively sparse observations to constrain them. This study documents the development of a new dust emissions scheme in the Met Office Unified ModelTM (MetUM) based on the Dust Entrainment and Deposition (DEAD) module. Four separate case studies are used to test and constrain the model output. Initial testing was undertaken on a large dust event over North Africa in March 2006 with the model constrained using AERONET data. The second case study involved testing the capability of the model to represent dust events in the Middle East without being re-tuned from the March 2006 case in the Sahara. While the model is unable to capture some of the daytime variation in AERONET AOD there is good agreement between the model and observed dust events. In the final two case studies new observations from in situ aircraft data during the Dust Outflow and Deposition to the Ocean (DODO) campaigns in February and August 2006 were used. These recent observations provided further data on dust size distributions and vertical profiles to constrain the model. The modelled DODO cases were also compared to AERONET data to make sure the radiative properties of the dust were comparable to observations. Copyright © 2009 Royal Meteorological Society and Crown Copyright

Direct radiative effect of aerosols emitted by transport from road, shipping and aviation

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 consist of a positive direct radiative forcing for aerosols emitted by road traffic of +20±11 mW m−2 for an externally mixed aerosol, and of +32±13 mW m−2 when BC is internally mixed. These direct radiative forcings are much higher than the previously published estimate of +3±11 mW m−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 mW m−2. These estimates are in very good agreement with the range of a previously published one (from −46 to −13 mW m−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 mW m−2.

Overview of observations from the RADAGAST experiment in Niamey, Niger: 2. Radiative fluxes and divergences

Broadband shortwave and longwave radiative fluxes observed both at the surface and from space during the Radiative Atmospheric Divergence using ARM Mobile Facility, GERB data and AMMA Stations (RADAGAST) experiment in Niamey, Niger, in 2006 are presented. The surface fluxes were measured by the Atmospheric Radiation Measurement (ARM) Program Mobile Facility (AMF) at Niamey airport, while the fluxes at the top of the atmosphere (TOA) are from the Geostationary Earth Radiation Budget (GERB) instrument on the Meteosat-8 satellite. The data are analyzed as daily averages, in order to minimize sampling differences between the surface and top of atmosphere instruments, while retaining the synoptic and seasonal changes that are the main focus of this study. A cloud mask is used to identify days with cloud versus those with predominantly clear skies. The influence of temperature, water vapor, aerosols, and clouds is investigated. Aerosols are ubiquitous throughout the year and have a significant impact on both the shortwave and longwave fluxes. The large and systematic seasonal changes in temperature and column integrated water vapor (CWV) through the dry and wet seasons are found to exert strong influences on the longwave fluxes. These influences are often in opposition to each other, because the highest temperatures occur at the end of the dry season when the CWV is lowest, while in the wet season the lowest temperatures are associated with the highest values of CWV. Apart from aerosols, the shortwave fluxes are also affected by clouds and by the seasonal changes in CWV. The fluxes are combined to provide estimates of the divergence of radiation across the atmosphere throughout 2006. The longwave divergence shows a relatively small variation through the year, because of a partial compensation between the seasonal variations in the outgoing longwave radiation (OLR) and surface net longwave radiation. A simple model of the greenhouse effect is used to interpret this result in terms of the dependence of the normalized greenhouse effect at the TOA and of the effective emissivity of the atmosphere at the surface on the CWV. It is shown that, as the CWV increases, the atmosphere loses longwave energy to the surface with about the same increasing efficiency with which it traps the OLR. When combined with the changes in temperature, this maintains the atmospheric longwave divergence within the narrow range that is observed. The shortwave divergence is mainly determined by the CWV and aerosol loadings and the effect of clouds is much smaller than on the component fluxes.

Hydrolysis of N2O5 on submicron sulfuric acid aerosols

The kinetics of reactive uptake of gaseous N2O5 on submicron sulfuric acid aerosol particles has been investigated using a laminar flow reactor coupled with a differential mobility analyzer (DMA) to characterize the aerosol. The particles were generated by homogeneous nucleation of SO3/H2O mixtures. In the H2SO4 concentration range 26.3−64.5 wt % the uptake coefficient was γ = 0.033 ± 0.004, independent of acid strength. For an acid strength of 45 wt % γ was found to decrease with increasing temperature over the range 263−298 K. From this, temperature dependence values of −115 ± 30 kJ/mol and −25.5 ± 8.4 J/K mol were determined for the changes in enthalpy and entropy of the uptake process, respectively. The results are consistent with a previous model of N2O5 hydrolysis involving both a direct and an acid catalyzed mechanism, with uptake under the experimental conditions limited by mass accommodation.

Hydrolysis of N2O5 on sub-micron mineral salt aerosols

The kinetics of reactive uptake of gaseous N2O5 on sub-micron aerosol particles composed of aqueous ammonium sulfate, ammonium hydrogensulfate and sodium nitrate has been investigated. Uptake was measured in a laminar flow reactor, coupled with a differential mobility analyser (DMA) to obtain the aerosol size distribution, with N2O5 detection using NO chemiluminescence. FTIR spectroscopy was used to obtain information about the composition and water content of the aerosol particles under the conditions used in the kinetic measurements. The aerosols were generated by the nebulisation of aqueous salt solutions. The uptake coefficient on the sulfate salts was in the range [gamma]=0.0015 to 0.033 depending on temperature, humidity and phase of the aerosol. On sodium nitrate aerosols the values were much lower, [gamma]<0.001, confirming the inhibition of N2O5 hydrolysis by nitrate ions. At high humidity (>50% r.h.) the uptake coefficient on liquid sulfate aerosols is independent of water content, but at lower humidity, especially below the efflorescence point, the reactivity of the aerosol declines, correlating with the lower water content. The lower uptake rate on solid aerosols may be due to limitations imposed by the liquid volume in the particles. Uptake on sulfate aerosols showed a negative temperature dependence at T>290 K but no significant temperature dependence at lower temperatures. The results are generally consistent with previous models of N2O5 hydrolysis where the reactive intermediate is NO2+ produced by autoionisation of nitrogen pentoxide in the condensed phase.

Cross-hemispheric transport of Central African biomass burning pollutants: Implications for downwind ozone production

Pollutant plumes with enhanced concentrations of trace gases and aerosols were observed over the southern coast of West Africa during August 2006 as part of the AMMA wet season field campaign. Plumes were observed both in the mid and upper troposphere. In this study we examined the origin of these pollutant plumes, and their potential to photochemically produce ozone (O3) downwind over the Atlantic Ocean. Their possible contribution to the Atlantic O3 maximum is also discussed. Runs using the BOLAM mesoscale model including biomass burning carbon monoxide (CO) tracers were used to confirm an origin from central African biomass burning fires. The plumes measured in the mid troposphere (MT) had significantly higher pollutant concentrations over West Africa compared to the upper tropospheric (UT) plume. The mesoscale model reproduces these differences and the two different pathways for the plumes at different altitudes: transport to the north-east of the fire region, moist convective uplift and transport to West Africa for the upper tropospheric plume versus north-west transport over the Gulf of Guinea for the mid-tropospheric plume. Lower concentrations in the upper troposphere are mainly due to enhanced mixing during upward transport. Model simulations suggest that MT and UT plumes are 16 and 14 days old respectively when measured over West Africa. The ratio of tracer concentrations at 600 hPa and 250 hPa was estimated for 14–15 August in the region of the observed plumes and compares well with the same ratio derived from observed carbon dioxide (CO2) enhancements in both plumes. It is estimated that, for the period 1–15 August, the ratio of Biomass Burning (BB) tracer concentration transported in the UT to the ones transported in the MT is 0.6 over West Africa and the equatorial South Atlantic. Runs using a photochemical trajectory model, CiTTyCAT, initialized with the observations, were used to estimate in-situ net photochemical O3 production rates in these plumes during transport downwind of West Africa. The mid-troposphere plume spreads over altitude between 1.5 and 6 km over the Atlantic Ocean. Even though the plume was old, it was still very photochemically active (mean net O3 production rates over 10 days of 2.6 ppbv/day and up to 7 ppbv/day during the first days) above 3 km especially during the first few days of transport westward. It is also shown that the impact of high aerosol loads in the MT plume on photolysis rates serves to delay the peak in modelled O3 concentrations. These results suggest that a significant fraction of enhanced O3 in mid-troposphere over the Atlantic comes from BB sources during the summer monsoon period. According to simulated occurrence of such transport, BB may be the main source for O3 enhancement in the equatorial south Atlantic MT, at least in August 2006. The upper tropospheric plume was also still photochemically active, although mean net O3 production rates were slower (1.3 ppbv/day). The results suggest that, whilst the transport of BB pollutants to the UT is variable (as shown by the mesoscale model simulations), pollution from biomass burning can make an important contribution to additional photochemical production of O3 in addition to other important sources such as nitrogen oxides (NOx) from lightning.