C. E. Reeves

Evaluation and intercomparison of global atmospheric transport models using 222Rn and other short‐lived tracers

Simulations of 222Rn and other short-lived tracers are used to evaluate and intercompare the representations of convective and synoptic processes in 20 global atmospheric transport models. Results show that most established three-dimensional models simulate vertical mixing in the troposphere to within the constraints offered by the observed mean 222Rn concentrations and that subgrid parameterization of convection is essential for this purpose. However, none of the models captures the observed variability of 222Rn concentrations in the upper troposphere, and none reproduces the high 222Rn concentrations measured at 200 hPa over Hawaii. The established three-dimensional models reproduce the frequency and magnitude of high-222Rn episodes observed at Crozet Island in the Indian Ocean, demonstrating that they can resolve the synoptic-scale transport of continental plumes with no significant numerical diffusion. Large differences between models are found in the rates of meridional transport in the upper troposphere (interhemispheric exchange, exchange between tropics and high latitudes). The four two-dimensional models which participated in the intercomparison tend to underestimate the rate of vertical transport from the lower to the upper troposphere but show concentrations of 222Rn in the lower troposphere that are comparable to the zonal mean values in the three-dimensional models.

Nitrogen management is essential to prevent tropical oil palm plantations from causing ground-level ozone pollution

More than half the worlds rainforest has been lost to agriculture since the Industrial Revolution. Among the most widespread tropical crops is oil palm (Elaeis guineensis): global production now exceeds 35 million tonnes per year. In Malaysia, for example, 13% of land area is now oil palm plantation, compared with 1% in 1974. There are enormous pressures to increase palm oil production for food, domestic products, and, especially, biofuels. Greater use of palm oil for biofuel production is predicated on the assumption that palm oil is an “environmentally friendly” fuel feedstock. Here we show, using measurements and models, that oil palm plantations in Malaysia directly emit more oxides of nitrogen and volatile organic compounds than rainforest. These compounds lead to the production of ground-level ozone (O3), an air pollutant that damages human health, plants, and materials, reduces crop productivity, and has effects on the Earths climate. Our measurements show that, at present, O3 concentrations do not differ significantly over rainforest and adjacent oil palm plantation landscapes. However, our model calculations predict that if concentrations of oxides of nitrogen in Borneo are allowed to reach those currently seen over rural North America and Europe, ground-level O3 concentrations will reach 100 parts per billion (109) volume (ppbv) and exceed levels known to be harmful to human health. Our study provides an early warning of the urgent need to develop policies that manage nitrogen emissions if the detrimental effects of palm oil production on air quality and climate are to be avoided.

The effect of aircraft emissions on tropospheric ozone in the northern hemisphere

Abstract The effect of aircraft emissions on tropospheric ozone was studied using a two-dimensional zonal model, of longitude vs altitude, extending between 30°–60°N. An emission inventory for the 1987 civil aircraft fleet was constructed based on fuel usage and civil aviation statistics. The addition of the 1987 civil emissions to a modelled standard atmosphere caused increases in concentrations of O3 (12%; 10 ppbv), NOx (40%; 20 pptv) and OH (10%) between 8 and 12 km altitude. A doubling and tripling of the emissions corresponding to a present day inclusion of military aircraft and a future scenario, respectively, caused the increase in O3 to double (19%) and almost triple (25%). The lightning source of NOx was found to be an important parameter. When this source was ommitted the change in O3 at the cruise flight altitude increased to 16%, with respect to a standard atmosphere not containing a lightning source of NOx.

Measurements of HCFC-142b and HCFC-141b in the Cape Grim air Archive: 1978–1993

Stored air samples collected at Cape Grim, Tasmania since 1978, have been analyzed by GC-MS to investigate the change in the tropospheric concentration of HCFC-142b and HCFC-141b over the past 15 years. Between April 1978 and September 1993 the concentration of HCFC-142b rose from 0.20±0.02 pptv to 3.0±0.3 pptv, with the majority of this increase occurring from 1989 onwards. By mid-1993 the rate of increase had reached 0.9±0.1 pptv/yr. From 1982 to 1991 the average concentration of HCFC-141b was 0.08±0.01 pptv. A very sharp increase in concentration began in 1992 however, such that it reached 0.46±0.05 pptv by September 1993. Using a 2-D model of atmospheric chemistry, constrained by these observations, global emissions of these two compounds have been calculated and found to differ from other estimates. This is partly due to the background concentration levels which existed prior to the start of the other estimated emissions.

Chemical composition observed over the mid-atlantic and the detection of pollution signatures far from source regions

The atmospheric composition of the central North Atlantic region has been sampled using the FAAM BAe146 instrumented aircraft during the Intercontinental Transport of Ozone and Precursors (ITOP) campaign, part of the wider International Consortium for Atmospheric Research on Transport and Transformation (ICARTT). This paper presents an overview of the ITOP campaign. Between late July and early August 2004, twelve flights comprising 72 hours of measurement were made in a region from approximately 20 to 40°W and 33 to 47°N centered on Faial Island, Azores, ranging in altitude from 50 to 9000 m. The vertical profiles of O3 and CO are consistent with previous observations made in this region during 1997 and our knowledge of the seasonal cycles within the region. A cluster analysis technique is used to partition the data set into air mass types with distinct chemical signatures. Six clusters provide a suitable balance between cluster generality and specificity. The clusters are labeled as biomass burning, low level outflow, upper level outflow, moist lower troposphere, marine and upper troposphere. During this summer, boreal forest fire emissions from Alaska and northern Canada were found to provide a major perturbation of tropospheric composition in CO, PAN, organic compounds and aerosol. Anthropogenic influenced air from the continental boundary layer of the USA was clearly observed running above the marine boundary layer right across the mid-Atlantic, retaining high pollution levels in VOCs and sulfate aerosol. Upper level outflow events were found to have far lower sulfate aerosol, resulting from washout on ascent, but much higher PAN associated with the colder temperatures. Lagrangian links with flights of other aircraft over the USA and Europe show that such signatures are maintained many days downwind of emission regions. Some other features of the data set are highlighted, including the strong perturbations to many VOCs and OVOCs in this remote region.

Recent tropospheric growth rate and distribution of HFC‐134a (CF3CH2F)

Air samples collected at Cape Grim, Tasmania (41°S) between 1978 and 1995, and at Mace Head, Ireland (53°N) between July 1994 and May 1995, have been analysed by GC-MS to determine recent trends of HFC-134a, an important CFC replacement, in the background atmosphere. Until 1990, the concentration of HFC-134a at Cape Grim was below detection limits, the first quantifiable level (0.01 pptv) appearing in May 1990. Between 1992 and mid-1995 the concentration grew exponentially at ∼200% yr¹, with the concentration at the end of 1994 reaching 0.43 pptv. At Mace Head, HFC-134a grew at a rate of 1.24±0.11 pptv yr¹ between July 1994 and May 1995, with the concentration at the end of 1994 being 1.48 pptv. hi the absence of industrial production and release estimates for HFC-134a, the observations have been used in conjunction with a 2-D global model to estimate recent emissions. The model indicates that significant emissions (250 tonnes) began in 1991, increasing rapidly to a level of ∼8 ktonnes in 1994.

Biological production of methyl bromide in the coastal waters of the North Sea and open ocean of the northeast Atlantic

Two separate studies in different oceanic regions provide evidence for the production of methyl bromide (CH3Br) by the prymnesiophyte Phaeocystis. A sampling program to study the seasonal cycle of CH3Br in a coastal area demonstrated that the seawater was supersaturated with respect to CH3Br for over 3 months of the year. The greatest saturation was observed during a bloom of Phaeocystis. Also, in situ field measurements demonstrated that CH3Br was supersaturated over a large region of the northeast Atlantic. A positive correlation was observed between CH3Br and dimethylsulphoniopropionate (DMSP), indicating that there was a source common to both compounds. An accessory pigment, hexanoyloxyfucoxanthin, which indicates the presence of prymnesiophytes, also correlated positively with CH3Br.

Forest fire plumes over the North Atlantic: p‐TOMCAT model simulations with aircraft and satellite measurements from the ITOP/ICARTT campaign

[1] Intercontinental Transport of Ozone and Precursors (ITOP) (part of International Consortium for Atmospheric Research on Transport and Transformation (ICARTT)) was an intense research effort to measure long-range transport of pollution across the North Atlantic and its impact on O3 production. During the aircraft campaign plumes were encountered containing large concentrations of CO plus other tracers and aerosols from forest fires in Alaska and Canada. A chemical transport model, p-TOMCAT, and new biomass burning emissions inventories are used to study the emissions long-range transport and their impact on the troposphere O3 budget. The fire plume structure is modeled well over long distances until it encounters convection over Europe. The CO values within the simulated plumes closely match aircraft measurements near North America and over the Atlantic and have good agreement with MOPITT CO data. O3 and NOx values were initially too great in the model plumes. However, by including additional vertical mixing of O3 above the fires, and using a lower NO2/CO emission ratio (0.008) for boreal fires, O3 concentrations are reduced closer to aircraft measurements, with NO2 closer to SCIAMACHY data. Too little PAN is produced within the simulated plumes, and our VOC scheme’s simplicity may be another reason for O3 and NOx modeldata discrepancies. In the p-TOMCAT simulations the fire emissions lead to increased tropospheric O3 over North America, the north Atlantic and western Europe from photochemical production and transport. The increased O3 over the Northern Hemisphere in the simulations reaches a peak in July 2004 in the range 2.0 to 6.2 Tg over a baseline of about 150 Tg.

Emissions of CH3Br, organochlorines, and organoiodines from temperate macroalgae

The production rates of a range of low molecular weight halogenated organics have been determined in cultures of five temperate species of macroalgae collected from the north coast of Norfolk, England. Compounds studied included CH3Br, the chlorinated organics CH3Cl, CH2Cl2 and CHCl3, and the iodinated organics CH3I, C2H5I, and CH2ClI. Measurements of a wider range of halocarbon concentrations in an isolated rockpool and in air over the seaweed bed were also conducted to evaluate the local impact of the seaweeds on halocarbon concentrations in the natural environment. Estimates for the global emissions of some of the key halogenated compounds from macroalgae have been derived. In general macrophytes appear not to be globally significant producers of the particular halocarbons studied. In coastal regions, however, the impact on local atmospheric composition and chemistry could be greater.

Impact of mesoscale vegetation heterogeneities on the dynamical and thermodynamic properties of the planetary boundary layer

This study uses aircraft observations over the Republic of Benin from the African Monsoon Multidisciplinary Analyses (AMMA) campaign to investigate the impact of vegetation heterogeneities on the dynamics within the planetary boundary layer, such as convection, transport, and mixing. Isoprene, a biogenic volatile organic compound emitted primarily by woody vegetation, was used as a tracer for transport to link the land surface to the boundary layer properties. Associated to planetary boundary layer (PBL) temperature gradients at vegetation boundaries, a persistent mesoscale organization of the winds which controlled patterns in the formation of cumulus congestus clouds was observed. A strong relationship among PBL temperatures, meridional wind velocity, isoprene concentrations, and fraction of forest or shrub cover was found, corroborating the land surface forcing of the observed dynamics. The observations show that the convergence zones tended to occur on the southern edge of warm surface and atmospheric anomalies. The northerly synoptic wind appears to have increased the coherency of the southerly part of the mesoscale flow and displaced the convergence zones southward. The relationships between the PBL potential temperatures and the meridional wind and isoprene concentrations were spatially coherent down to wavelengths of 10 and 8 km, respectively. A seasonal climatology of visible satellite data shows enhanced cloud cover in the afternoon over cropland, suggesting that the results presented are not limited to this case study but are of climatological significance in the region.