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We show that mineral dust optical depth and altitude can be retrieved from the Aqua - Advanced Infrared Radiation Sounder (AIRS) measurements. Sensitivity studies performed with a high spectral resolution radiative transfer code show that dust effect on brightness temperatures may reach about 10 Kelvins for some channels. Using a Look-Up-Table approach, we retrieve not only the 10 µm optical depth but also the altitude of Saharan dust layer, above the Atlantic Ocean, from April to September 2003. A key point of our method is its ability to retrieve dust altitude from satellite observations. The time and space distribution of the optical depth is in good agreement with the Moderate resolution Imaging Spectroradiometer (MODIS) products. Comparing MODIS and AIRS aerosol optical depths, we find that the ratio between infrared and visible optical depths decreases during transport from 0.35 to 0.22, revealing a loss in coarse particles caused by gravitational settling. The evolution of dust altitude from spring to summer is in agreement with current knowledge on transport seasonality.
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Future increases in the concentration of greenhouse gases and water vapour may cool the stratosphere further and increase the amount of polar stratospheric clouds (PSCs). Future Arctic PSC areas have been extrapolated from the highly significant trends 1958-2001. Using a tight correlation between PSC area and the total vortex ozone depletion and taking the decreasing amounts of ozone depleting substances into account we make empirical estimates of future ozone. The result is that Arctic ozone losses increase until 2010-2015 and decrease only slightly afterwards. However, for such a long extrapolation into the future caution is necessary. Tentatively taking the modelled decrease in the ozone trend in the future into account results in almost constant ozone depletions until 2020 and slight decreases afterwards. This approach is a complementary method of prediction to that based on the complex coupled chemistry-climate models (CCMs).
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The vertical transport of tracers by a cumulus ensemble at the TOGA-COARE site is modelled during a 7 day episode using 2-D and 3-D cloud-resolving setups of the Weather Research and Forecast (WRF) model. Lateral boundary conditions (LBC) for tracers, water vapour, and wind are specified and the horizontal advection of trace gases across the lateral domain boundaries is considered. Furthermore, the vertical advection of trace gases by the large-scale motion (short: vertical large-scale advection of tracers, VLSAT) is considered. It is shown that including VLSAT partially compensates the calculated net downward transport from the middle and upper troposphere (UT) due to the mass balancing mesoscale subsidence induced by deep convection. Depending on whether the VLSAT term is added or not, modelled domain averaged vertical tracer profiles can differ significantly. Differences between a 2-D and a 3-D model run were mainly attributed to an increase in horizontal advection across the lateral domain boundaries due to the meridional wind component not considered in the 2-D setup.
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The use of PV equivalent latitude for assimilating stratospheric tracer observations is discussed - with particular regard to the errors in the equivalent latitude coordinate, and to the assimilation of sparse data. Some example measurements are assimilated: they sample the stratosphere sporadically and inhomogeneously. The aim was to obtain precise information about the isentropic tracer distribution and evolution as a function of equivalent latitude. Precision is important, if transport across barriers like the vortex edge are to be detected directly. The main challenges addressed are the errors in modelled equivalent latitude, and the non-ideal observational sampling. The methods presented allow first some assessment of equivalent latitude errors and a picture of how good or poor the observational coverage is. This information determines choices in the approach for estimating as precisely as possible the true equivalent latitude distribution of the tracer, in periods of good and poor observational coverage. This is in practice an optimisation process, since better understanding of the equivalent latitude distribution of the tracer feeds back into a clearer picture of the errors in the modelled equivalent latitude coordinate. Error estimates constrain the reliability of using equivalent latitude to make statements like "this observation samples air poleward of the vortex edge" or that of more general model-measurement comparisons. The approach is demonstrated for ground-based lidar soundings of the Mount Pinatubo aerosol cloud, focusing on the 1991-92 arctic vortex edge between 475-520K. Equivalent latitude is estimated at the observation times and locations from Eulerian model tracers initialised with PV and forced by UK Meteorological Office analyses. With the model formulation chosen, it is shown that tracer transport of a few days resulted in an error distribution that was much closer to Gaussian form, although the mean error was not significantly affected. The analysis of the observations revealed a small amount of irreversible transport of aerosol across the vortex edge during late January 1992, coincident with a strongly disturbed vortex.
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Here we present a concise and efficient algorithm to mimic the growth and sedimentation of Nitric Acid Trihydate (NAT) particles in the polar vortex in a state-of-the-art 3D chemistry transport model. The particle growth and sedimentation are calculated using the microphysical formulation of Carslaw et al. (2002). Once formed, NAT particles are transported in the model as tracers in the form of size-segregated quantities or size bins. Two different approaches were adopted for this purpose: one assuming a fixed particle number density ("FixedDens") and the other assuming a discrete set of particle diameter values ("FixedRad"). Simulations were performed for three separate 10-day periods during the 1999-2000 Arctic winter and compared to the results of an existing Lagrangian model study, which uses similar microphysics in a computationally more expensive method for the simulation of NAT particle growth. The resulting particle sizes for both our approaches compare favourably at 430K with those obtained from this previous model study, and also in-situ observations related to the size of large NAT particles. The particle growth is faster for "FixedDens" resulting in a difference in (de)nitrification by a factor of ~2 for all three simulation periods. Comparisons were made with a standard equilibrium approach and the differences in the redistribution of HNO<sub>3</sub> were found to be substantial. For both approaches the performance of the algorithm is rather insensitive to both the number of size bins and the shape of the size distribution, and show a weak dependence on the prescribed total particle number density during the coldest period. This results in an increase of 7% for the "FixedRad" approach and 17% for the "FixedDens" approach when increasing the total particle number density by a factor of 2.5.
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The aging of soot is one of the key uncertainties in the estimation of both the direct and indirect climate effect. While freshly emitted soot is initially hydrophobic and externally mixed, it can be transferred into an internal mixture by coagulation, condensation or photochemical processes. These aging processes affect the hygroscopic qualities and hence the growth behaviour, the optical properties and eventually the lifetime of the soot particles. However, due to computational limits the aging of soot in global climate models is often only parameterised by an estimated turnover rate resulting in a lifetime of soot of several days. Hence, the aging process of soot is one of the key uncertainties governing the burden and effect of black carbon. In this study, we discuss the time scale on which diesel soot is transferred from an external to an internal mixture based on the results of our simulations with a comprehensive mesoscale model. For daytime conditions during summer condensation of sulphuric acid is dominant and the aging process occurs on a time scale of τ =8h close to the sources and τ =2h above the source region. During winter comparable time scales are found but ammonium nitrate becomes more important. During night time condensation is not effective. Then coagulation is the most important aging process and our results show time scales between 10h and 40h.
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There are at least three reasons why hydrogen cyanide is likely to be significant for atmospheric chemistry. The first is well known, HCN is a product and marker of biomass burning. However, if a detailed ion chemistry of lightning is considered then it is almost certain than in addition to lightning producing NO<sub>x</sub>, it also produces HO<sub>x</sub> and HCN. Unlike NO<sub>x</sub> and HO<sub>x</sub>, HCN is long-lived and could therefore be a useful marker of lightning activity. Observational evidence is considered to support this view. Thirdly, the chemical decomposition of HCN leads to the production of small amounts of CN and NCO. NCO can be photolyzed in the visible portion of the spectrum yielding N atoms. The production of N atoms is significant as it leads to the titration of nitrogen from the atmosphere via N+N→N<sub>2</sub>. Normally the only modelled source of N atoms is NO photolysis which happens largely in the UV Schumann-Runge bands. However, NCO photolysis occurs in the visible and so could be involved in titration of atmospheric nitrogen in the lower stratosphere and troposphere. HCN emission inventories are worthy of attention. The CN and NCO radicals have been termed pseudohalogens since the 1920s. They are strongly bound, univalent, radicals with an extensive and varied chemistry. The products of the atmospheric oxidation of HCN are NO, CO and O<sub>3</sub>. N+CH<sub>4</sub> and N+CH<sub>3</sub>OH are found to be important sources of HCN. Including the pseudohalogen chemistry gives a small increase in ozone and total reactive nitrogen (NO<sub>y</sub>).
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This paper compares column measurements of NO<sub>2</sub> made by the GOME instrument on ERS-2 to model results from the TOMCAT global CTM. The overall correlation between the model and observations is good (0.79 for the whole world, and 0.89 for North America) but the modelled columns are larger than GOME over polluted areas (gradient of 1.4 for North America and 1.9 for Europe). NO<sub>2</sub> columns in the region of outflow from North America into the Atlantic are higher in winter in the model compared to the GOME results, whereas the modelled columns are smaller off the coast of Africa where there appear to be biomass burning plumes in the satellite data. Several hypotheses are presented to explain these discrepancies. Weaknesses in the model treatment of vertical mixing and chemistry appear to be the most likely explanations.
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The Global Ozone Monitoring Experiment (GOME) allows the retrieval of tropospheric vertical column densities (VCDs) of NO<sub>2</sub> on a global scale. Regions with enhanced industrial activity can clearly be detected, but the standard spatial resolution of the GOME ground pixels (320x40km<sup>2</sup>) is insufficient to resolve regional trace gas distributions or individual cities. <P style="line-height: 20px;"> Every 10 days within the nominal GOME operation, measurements are executed in the so called narrow swath mode with a much better spatial resolution (80x40km<sup>2</sup>). We use this data (1997-2001) to construct a detailed picture of the mean global tropospheric NO<sub>2</sub> distribution. Since - due to the narrow swath - the global coverage of the high resolution observations is rather poor, it has proved to be essential to deseasonalize the single narrow swath mode observations to retrieve adequate mean maps. This is done by using the GOME backscan information. <P style="line-height: 20px;"> The retrieved high resolution map illustrates the shortcomings of the standard size GOME pixels and reveals an unprecedented wealth of details in the global distribution of tropospheric NO<sub>2</sub>. Localised spots of enhanced NO<sub>2</sub> VCD can be directly associated to cities, heavy industry centers and even large power plants. Thus our result helps to check emission inventories. <P style="line-height: 20px;"> The small spatial extent of NO<sub>2</sub> "hot spots" allows us to estimate an upper limit of the mean lifetime of boundary layer NO<sub>x</sub> of 17h on a global scale. <P style="line-height: 20px;"> The long time series of GOME data allows a quantitative comparison of the narrow swath mode data to the nominal resolution. Thus we can analyse the dependency of NO<sub>2</sub> VCDs on pixel size. This is important for comparing GOME data to results of new satellite instruments like SCIAMACHY (launched March 2002 on ENVISAT), OMI (launched July 2004 on AURA) or GOME II (to be launched 2005) with an improved spatial resolution.
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In this study the ion production rates in a boreal forest were studied based on two different methods: 1) cluster ion and particle concentration measurements, 2) external radiation and radon concentration measurements. Both methods produced reasonable estimates for ion production rates. The average ion production rate calculated from aerosol particle size distribution and air ion mobility distribution measurements was 2.6 ion pairs cm<sup>-3</sup>s<sup>-1</sup>, and based on external radiation and radon measurements, 4.5 ion pairs cm<sup>-3</sup>s<sup>-1</sup>. The first method based on ion and particle measurements gave lower values for the ion production rates especially during the day. A possible reason for this is that particle measurements started only from 3nm, so the sink of small ions during the nucleation events was underestimated. It may also be possible that the hygroscopic growth factors of aerosol particles were underestimated. Another reason for the discrepancy is the nucleation mechanism itself. If the ions are somehow present in the nucleation process, there could have been an additional ion sink during the nucleation days.
