J. A. Pyle

Two‐dimensional assessment of the impact of aircraft sulphur emissions on the stratospheric sulphate aerosol layer

We have developed a two-dimensional sulphate aerosol model, which includes most of the important microphysical processes governing the formation and evolution of stratospheric sulphate particles. Simulations of the background aerosol layer shows that important aerosol properties (surface area density, optically active particle concentration, mass mixing ratio) are strongly latitude dependent. This model is used to investigate if the sulphur aircraft emissions may have caused the 60% increase in large aerosol particles observed over the 1979–1990 time period. Results suggest that although aircraft may represent a substantial source of sulphate below 20 km, the rise in air traffic is insufficient to account for the apparent trend in stratospheric aerosol particles.

Validation and intercomparison of wet and dry deposition schemes using 210Pb in a global three-dimensional off-line chemical transport model

We have used 210 Pb, a tracer originating from the radioactive decay of 222 Rn emitted from soils, to validate different wet and dry deposition schemes in our global three-dimensional off-line chemical transport model, TOMCAT. We have tested two different parameterizations for the dry deposition, one with the turbulent exchange in the boundary layer and one without. When dry deposition is linked to the boundary layer scheme, the model shows the ability to resolve shallow mixing depths in winter with enhanced lifetimes and concentrations of surface aerosol. Three conceptually different wet deposition schemes have been implemented and tested in TOMCAT. In the first, where wet removal is assumed to be proportional to the local gradient of the specific humidity, the model has a global mean bias for the surface concentrations of -40%. Using this scheme, the observed surface concentrations are seriously underpredicted, and most of the aerosol burden is scavenged within the boundary layer. In the second scheme, where scavenging is parameterized proportional to the model-derived total precipitation rate (large scale and convective), the model exhibits a +26% bias. The concentrations are overpredicted, especially in continental areas as this scheme fails to capture the coupling between vertical transport and rainout. In the third scheme, wet removal is coupled with the vertical transport inside convective clouds. The model then shows the best performance with only a -4% bias for the concentrations. Furthermore, other regional discrepancies between model and observations point to a variability in 222 Rn emissions, which was not taken into account with our simple 222 Rn emission scenario, and also to anomalies in our model-derived precipitation rate. The aerosol residence times are realistic only when the wet removal schemes use the precipitation rate rather than the specific humidity. The dry subtropical and polar regions can be captured with lifetimes at 500 hPa of more than 50 days whereas in regions of high precipitation the lifetimes are less than 5 days.

The variability of ClONO2 and HNO3 in the Arctic polar vortex : comparison of Transall Michelson interferometer for passive atmospheric sounding measurements and three-dimensional model results

A three-dimensional radiative-dynamical-chemical model has been used to investigate measurements of column ClONO2 and HNO3 made by the airborne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument. MIPAS made measurements from the Transall aircraft in the northern hemisphere lower stratosphere from December 1992 to March 1993. The three-dimensional model has a detailed stratospheric chemistry scheme including heterogeneous reactions on polar stratospheric clouds and sulfate aerosols. The circulation in the model is specified from the European Centre for Medium Range Weather Forecasts analyses. The MIPAS measurements reveal large variability in column ClONO2 at the edge of the polar vortex. For the measurements of January 27 and 31, 1993, the model experiments show that variability in ClONO2 observed over this period can be explained by polar stratospheric cloud processing and recovery. Measurements of ClONO2 on February 2, 1993, showed large variations depending on the orientation of the aircraft relative to the edge of the vortex. Results from the model show that this is qualitatively consistent with the aircraft flying near to the collar region with its associated strong horizontal gradients of ClONO2. The models ability to simulate these strong gradients is limited by its relatively coarse resolution. In early March the vortex became very distorted. During this period MIPAS measured very large values of ClONO2 at high latitudes within the vortex but lower, although still large, values in the more southerly regions of the vortex. At this stage of the winter ClONO2 is the major chlorine species in the model at high latitudes. The model shows how the distortion of the vortex in March led to relatively high columns of ClONO2 in vortex air over southern Europe. The model also reproduces the observed gradient in ClONO2 within the vortex, and experiments show that these gradients are due, at least in part, to the availability of sunlight. This variability of ClONO2, and therefore active chlorine (ClOχ), implies that these tracers do not correlate well with potential vorticity. This places limitations on extrapolating localized measurements of anything but the longest lived chemical tracers to the whole of the polar vortex using potential vorticity, or indeed a long-lived tracer, as part of a coordinate system.

Measurements of δ13C in CH4 and using particle dispersion modeling to characterize sources of arctic methane within an air mass

Abstract A stratified air mass enriched in methane (CH4) was sampled at ~600u2009m to ~2000u2009m altitude, between the north coast of Norway and Svalbard as part of the Methane in the Arctic: Measurements and Modelling campaign on board the UKs BAe‐146‐301 Atmospheric Research Aircraft. The approach used here, which combines interpretation of multiple tracers with transport modeling, enables better understanding of the emission sources that contribute to the background mixing ratios of CH4 in the Arctic. Importantly, it allows constraints to be placed on the location and isotopic bulk signature of the emission source(s). Measurements of δ13C in CH4 in whole air samples taken while traversing the air mass identified that the source(s) had a strongly depleted bulk δ13C CH4 isotopic signature of −70 (±2.1)‰. Combined Numerical Atmospheric‐dispersion Modeling Environment and inventory analysis indicates that the air mass was recently in the planetary boundary layer over northwest Russia and the Barents Sea, with the likely dominant source of methane being from wetlands in that region.