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Single-particle compositional analysis of filter samples collected on-board the FAAM BAe-146 aircraft is presented for six flights during the springtime Aerosol-Cloud Coupling and Climate Interactions in the Arctic (ACCACIA) campaign (March-April 2013). Scanning electron microscopy was utilised to derive size distributions and sizesegregated particle compositions. These data were compared to corresponding data from wing-mounted optical particle counters and reasonable agreement between the calculated number size distributions was found. Significant variability in composition was observed, with differing external and internal mixing identified, between air mass trajectory cases based on HYSPLIT analyses. Dominant particle classes were silicatebased dusts and sea salts, with particles notably rich in K and Ca detected in one case. Source regions varied from the Arctic Ocean and Greenland through to northern Russia and the European continent. Good agreement between the back trajectories was mirrored by comparable compositional trends between samples. Silicate dusts were identified in all cases, and the elemental composition of the dust was consistent for all samples except one. It is hypothesised that long-range, high-altitude transport was primarily responsible for this dust, with likely sources including the Asian arid regions. [ABSTRACT FROM AUTHOR]

The Fennec climate program aims to improve understanding of the Saharan climate system through a synergy of observations and modelling. We present a description of the Fennec airborne observations during 2011 and 2012 over the remote Sahara (Mauritania and Mali) and the advances in the understanding of mineral dust and boundary layer processes they have provided. Aircraft instrumentation aboard the UK FAAM BAe146 and French SAFIRE Falcon 20 is described, with specific focus on instrumentation specially developed and relevant to Saharan meteorology and dust. Flight locations, aims and associated meteorology are described. Examples and applications of aircraft measurements from the Fennec flights are presented, highlighting new scientific results delivered using a synergy of different instruments and aircraft. These include: (1) the first airborne measurement of dust particles sized up to 300 microns and associated dust fluxes in the Saharan atmospheric boundary layer (SABL), (2) dust uplift from the breakdown of the nocturnal low-level jet before becoming visible in SEVIRI satellite imagery, (3) vertical profiles of the unique vertical structure of turbulent fluxes in the SABL, (4) in-situ observations of processes in SABL clouds showing dust acting as CCN and IN at -15 °C, (5) dual-aircraft observations of the SABL dynamics, thermodynamics and composition in the Saharan heat low region (SHL), (6) airborne observations of a dust storm associated with a cold-pool (haboob) issued from deep convection over the Atlas, (7) the first airborne chemical composition measurements of dust in the SHL region with differing composition, sources (determined using Lagrangian backward trajectory calculations) and absorption properties between 2011 and 2012, (8) coincident ozone and dust surface area measurements suggest coarser particles provide a route for ozone depletion, (9) discrepancies between airborne coarse mode size distributions and AERONET sunphotometer retrievals under light dust loadings. These results provide insights into boundary layer and dust processes in the SHL region -- a region of substantial global climatic importance. [ABSTRACT FROM AUTHOR]

New in-situ aircraft measurements of Saharan dust originating from Mali, Mauritania and Algeria taken during the Fennec 2011 aircraft campaign over a remote part of the Sahara Desert are presented. Size distributions extending to 300 µm are shown, representing measurements extending further into the coarse mode than previously published for airborne Saharan dust. A significant coarse mode was present in the size distribution measurements with effective diameter (deff) from 2.3 to 19.4 µm and coarse mode volume median diameter (dvc) from 5.8 to 45.3 µm. The mean size distribution had a larger relative proportion of coarse mode particles than previous aircraft measurements. The largest particles (with deff > 12 µm, or dvc > 25 µm) were only encountered within 1 km of the ground. Number concentration, mass loading and extinction coefficient showed inverse relationships to dust age since uplift. Dust particle size showed a weak exponential relationship to dust age. Two cases of freshly uplifted dust showed quite different characteristics of size distribution and number concentration. SSA values at 550 nm calculated from the measured size distributions revealed high absorption ranging from 0.70 to 0.97 depending on the refractive index. SSA was found to be strongly related to deff. New instrumentation revealed that direct measurements, behind Rosemount inlets, overestimate SSA by up to 0.11 when deff is greater than 2 µm. This is caused by aircraft inlet inefficiencies and sampling losses. Previous measurements of SSA from aircraft measurements may also have been overestimates for this reason. Radiative transfer calculations indicate that the range of SSAs during Fennec 2011 can lead to underestimates in shortwave atmospheric heating rates by 2.0 to 2.9 times if the coarse mode is neglected. This will have an impact on Saharan atmospheric dynamics and circulation, which should be taken into account by numerical weather prediction and climate models. [ABSTRACT FROM AUTHOR]

The Emissions around the M25 motorway (EM25) campaign took place over the megacity of London in the United Kingdom in June 2009 with the aim of characterising trace gas and aerosol composition and properties entering and emitted from the urban region. It featured two mobile platforms, the UK BAe-146 Facility for Airborne Atmospheric Measurements (FAAM) research aircraft and a ground-based mobile lidar van, both travelling in circuits around London, roughly following the path of the M25 motorway circling the city. We present an overview of findings from the project, which took place during typical UK summertime pollution conditions. Emission ratios of volatile organic compounds (VOCs) emitted from the London region were consistent with measurements in and downwind of other large urban areas and indicated traffic and associated fuel evaporation were major sources. Sub-micron aerosol composition was dominated by secondary species including sulphate (24% of sub-micron mass in the London plume and 30% in the background aerosol), nitrate (24% plume; 18% background) and organic aerosol (30% plume; 30% background). The primary submicron aerosol emissions from London were minor compared to the larger regional background, with only limited increases in aerosol mass in the urban plume compared to the background (15% mass increase on average). Black carbon mass was the major exception, which more than doubled in the urban plume and lead to a decrease in the single scattering albedo from 0.91 in the background aerosol to 0.86 in the London plume, on average. Our observations indicated that regional aerosol appeared to dominate urban sources, at least during typical summertime conditions, meaning future efforts to reduce PM levels in London must account for regional as well as local aerosol sources. [ABSTRACT FROM AUTHOR]

OH and HO2 aircraft measurements made over West Africa during the AMMA field campaign in summer 2006 have been investigated using a box model constrained to observations of long-lived species and physical parameters. "Good" agreement was found for HO2 (modelled to observed gradient of 1.23±0.11). However, the model significantly overpredicts OH concentrations. The reasons for this are not clear, but may reflect instrumental instabilities affecting the OH measurements. Within the model HOx concentrations in West Africa are controlled by relatively simple photochemistry, with production dominated by ozone photolysis and reaction of O(1D) with water vapour, and loss processes dominated by HO2+HO2 and HO2+RO2. Isoprene chemistry was found to influence forested regions. In contrast to several recent field studies in very low NOx and high isoprene environments we do not observe any dependence of model success for HO2 on isoprene and attribute this to efficient recycling of HOx through RO2+NO reactions under the moderate NOx concentrations (5-300 ppt NO in the boundary layer) encountered during AMMA. This suggests that some of the problems with understanding the impact of isoprene on atmospheric composition may be limited to the extreme low range of NOx concentrations. [ABSTRACT FROM AUTHOR]

Pollutant plumes with enhanced levels 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 both the origin of these pollutant plumes and their potential to produce O3 downwind over the Atlantic Ocean. Runs using the BOLAM mesoscale model including biomass burning CO tracers were used to confirm an origin from central African fires. The plumes in the mid troposphere had significantly higher pollutant concentrations due to the fact that transport occurred from a region nearer or even over the fire region. In contrast, plumes transported into the upper troposphere over West Africa had been transported to the north-east of the fire region before being uplifted. Modelled tracer results showed that pollutants resided for between 9 and 12 days over Central Africa before being transported for 4 days, in the case of the mid-troposphere plume and 2 days in the case of the upper tropospheric plume to the measurement location over the southern part of West Africa. Around 35% of the biomass burning tracer was transported into the upper troposphere compared to that remaining in the mid troposphere. Runs using a photochemical trajectory model, CiTTyCAT, were used to estimate the net photochemical O3 production potential of these plumes. The mid tropospheric plume was still very photochemically active (up to 7 ppbv/day) especially during the first few days of transport westward over the Atlantic Ocean. The upper tropospheric plume was also still photochemically active, although at a slower rate (1-2 ppbv/day). Trajectories show this plume being recirculated around an upper tropospheric anticyclone back towards the African continent (around 20°S). The potential of theses plumes to produce O3 supports the hypothesis that biomass burning population are contributing to the observed O3 maxima over the southern Atlantic at this time of year. [ABSTRACT FROM AUTHOR]

We report here top-down emissions estimate for an African megacity. A boundary-layer circumnavigation of Lagos, Nigeria was completed using the FAAM BAe146 aircraft as part of the AMMA project. These observations together with an inferred boundary-layer 5 height allow the flux of pollutants to be calculated. Extrapolation gives annual emissions for CO, NOx and VOCs of 0.72 TgCyr-1, 0.02 TgNyr-1 and 0.28 TgCyr-1 respectively, consistent with bottom-up estimates for other developing megacities. These emissions are attributed to the evaporation of fuels, mobile combustion and natural gas emissions. [ABSTRACT FROM AUTHOR]

This paper presents measurements of organic aerosols above subtropical West Africa during the wet season using data from the UK Facility for Airborne Atmospheric Measurements (FAAM) aircraft. Measurements of biogenic volatile organic compounds (BVOC) at low altitudes over these subtropical forests were made during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment during July and August 2006 mainly above Benin, Nigeria and Niger. Data from an Aerodyne Quadrupole Aerosol Mass Spectrometer show a median organic aerosol loading of 1.08 μg m-3 over tropical West Africa, which represents the first regionally averaged assessment of organic aerosol mass (OM) in this region during the wet season. This is in good agreement with predictions based on aerosol yields from isoprene and monoterpenes during chamber studies and model predictions based on partitioning schemes, contrasting markedly with the large under representations of OM in similar models when compared with data from mid latitudes. [ABSTRACT FROM AUTHOR]

Chemical and meteorological parameters measured on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe 146 Atmospheric Research Aircraft during the African Monsoon Multidisciplinary Analysis (AMMA) campaign are presented to show the impact of NOx emissions from recently wetted soils in West Africa. NOx emissions from soils have been previously observed in many geographical areas with different types of soil/vegetation cover during small scale studies and have been inferred at large scales from satellite measurements of NOx. This study is the first dedicated to showing the emissions of NOx at an intermediate scale between local surface sites and continental satellite measurements. The measurements reveal pronounced mesoscale variations in NOx concentrations closely linked to spatial patterns of antecedent rainfall. Fluxes required to maintain the NOx concentrations observed by the BAe-146 in a number of cases studies and for a range of assumed OH concentrations (0 to 1 x 107 molecules cm-3) are calculated to be in the range 4.7 to 37.3 ng Nm-2 s-1. These values are comparable to the range of fluxes from 2 to 83 ng Nm-2 s-1 reported from small scale field studies in a variety of tropical and sub-tropical locations reported in the review of Davidson and Kingerlee (1997). The fluxes calculated in the present study have been scaled up to cover the area of the Sahel bounded by 10 to 20 N and 10 E to 20W giving an estimated emission of up to 0.05 TgN from this area for July and August 2006. The observed chemical data also suggest that the NOx emitted from soils is taking part in ozone formation as ozone concentrations exhibit similar fine scale structure to the NOx, with enhancements over the wet soils. Such variability can not be explained on the basis of transport from other areas. [ABSTRACT FROM AUTHOR]

An automated, ground-based instrument was used to measure gas-phase hydroperoxides at the Jungfraujoch High Altitude Research Station as part of the Free Tropospheric EXperiment (FREETEX) during February/March 2003. A nebulising reflux concentrator sampled ambient air twice hourly, prior to on-site analysis by HPLC speciation, coupled with post-column peroxidase derivatisation and fluorescence detection. Hydrogen peroxide (H2O2) concentrations reached up to 1420 pptv over the 13-day period with a mean of 206±261 pptv (± one standard deviation). Methyl hydroperoxide (CH3OOH) reached up to 921 pptv with a mean of 76±96 pptv. No other organic hydroperoxides were detected. The lack of an explicit diurnal cycle suggests that hydroperoxide concentrations are chiefly influenced by transport processes rather than local photochemistry at this mountainous site. We find elevated concentrations of H2O2 in air masses originating from the south-west indicative of higher concentrations of HOx due to more active photochemistry. Air which has been recently polluted exhibits low H2O2 concentration due to a combination of suppression of HO2 by NOx and deposition. We also conclude that despite being at a high alpine site, the vast majority of the air observed was extensively influence by the boundary layer during our campaign (diagnosed from high CO concentrations and the high NOx to NOy ratio) resulting in deposition of H2O2 to the surface and hence reduced H2O2 concentrations. The concentrations of H2O2 sampled here are consistent with previous box modelling studies of hydroperoxides which invoked a depositional sink. [ABSTRACT FROM AUTHOR]

The distribution of trace gases upwind and above the Mace Head Atmospheric Research Station, Ireland has been determined using measurements made from aircraft. The observations indicate excellent agreement between most non-methane hydrocarbons, dimethyl sulphide (DMS) and ozone measured at the surface, at 390m overhead and in upwind boundary layer regions of the coastal Atlantic. Vertical profiles above the observatory indicated that local convective events result in a marine influence being detected at 3 km and above. The observation of isoprene from maritime sources at these levels was indicative of very rapid uplift on the hour timescale. Measurements of trace gases were also made directly upwind of the observatory over coastal regions and as far as the deep open ocean beyond the continental shelf. A maximum of 240 pptV DMS was observed in the boundary layer near to the shelf region, declining to a concentration of around 40 pptV at the coastline. The upwelling of nutrient rich waters at the ocean shelf location may be a possible explanation for the high abundance of DMS in these regions. The observations suggest that this region, some 150-200 km from the observatory, would under these environmental conditions have a major influence in the determining the DMS observed on-shore. The spatial distribution of ethene within boundary layer over coastal and deep waters differed significantly from DMS with an almost uniform abundance over all ocean regions. [ABSTRACT FROM AUTHOR]

The North Atlantic Marine Boundary Layer Experiment (NAMBLEX), involving over 50 scientists from 12 institutions, took place at Mace Head, Ireland (53.32° N, 9.90° W), between 23 July and 4 September 2002. A wide range of state-of-the-art instrumentation enabled detailed measurements of the boundary layer structure and atmospheric composition in the gas and aerosol phase to be made, providing one of the most comprehensive in situ studies of the marine boundary layer to date. This overview paper describes the aims of the NAMBLEX project in the context of previous field campaigns in the Marine Boundary Layer (MBL), the overall layout of the site, a summary of the instrumentation deployed, the temporal coverage of the measurement data, and the numerical models used to interpret the field data. Measurements of some trace species were made for the first time during the campaign, which was characterised by predominantly clean air of marine origin, but more polluted air with higher levels of NOx originating from continental regions was also experienced. This paper provides a summary of the meteorological measurements and Planetary Boundary Layer (PBL) structure measurements, presents time series of some of the longer-lived trace species (O3, CO, H2, DMS, CH4, NMHC, NOx, NOy, PAN) and summarises measurements of other species that are described in more detail in other papers within this special issue, namely oxygenated VOCs, HCHO, peroxides, organo-halogenated species, a range of shorter lived halogen species (I2, OIO, IO, BrO), NO3 radicals, photolysis frequencies, the free radicals OH, HO2 and (HO2+ΣRO2), as well as a summary of the aerosol measurements. NAMBLEX was supported by measurements made in the vicinity of Mace Head using the NERC Dornier-228 aircraft. Using ECMWF wind-fields, calculations were made of the air-mass trajectories arriving at Mace Head during NAMBLEX, and were analysed together with both meteorological and trace-gas measurements. In this paper a chemical climatology is presented to interpret the distribution of air-mass origins and emission sources, and to provide a convenient framework of air-mass classification that is used by other papers in this issue for the interpretation of observed variability in levels of trace gases and aerosols. [ABSTRACT FROM AUTHOR]