Wet‐only sequential deposition in a rural area in north‐eastern Spain

The present work summarises the results of a 2‐year study of wet‐only sequential deposition in 2 rural areas (Alcan¯iz and Morella) located at different distances from a large coal‐fired power station. Precipitation chemistry was characterised by relatively high , Ca²⁺ and average concentrations. Sequential study of single precipitation events showed that concentrations of most of the ions studied decreased exponentially throughout single precipitation events, with a sharper decrease in concentrations at the beginning of the event. Usually, 40 to 80% of the wet‐only deposition of major ions occurred in the first 2 mm. pH measurements, ranging from 5.6 to 8.1, showed a decrease in the pH values throughout a precipitation event. Deposition levels of Ca²⁺ and accounted for the neutralisation of major acidic species in the precipitation events except in 5 rain episodes sampled at Morella. The sequential study of the evolution of the ratio during a single precipitation allowed us to identify potential acidic rainfall fractions after an initial volume of precipitation, after most of the Ca²⁺ in atmospheric particles had been scavenged. A higher neutralisation capacity was deduced for Alcan¯iz owing to the higher atmospheric levels of natural carbonates and .     

Determination of microbial versus root‐produced CO2 in an agricultural ecosystem by means of δ13CO2 measurements in soil air

The amounts of microbial and root‐respired CO₂ in a maize/winter wheat agricultural system in south western Germany were investigated by measurements of the CO₂ mixing ratio and the ¹³C/¹²C ratio in soil air. CO₂ fluxes at the soil surface for the period of investigation (1993–1995) were also determined. Root respired CO₂ shows a strong correlation with the plant mass above ground surface of the respective vegetation (R²≥0.88); the maximum CO₂ release from roots was in August for the maize (2.0±0.5 mmol m⁻² h⁻¹) and in June for winter wheat (1.5±0.5 mmol m⁻² h⁻¹). Maximum CO₂ production by roots correlate well with the maximum amount of plant root matter. Integrating the CO₂ production over the whole growing season and normalizing to the dry root matter yields, the CO₂ production per gram dry organic root matter (DORM) of maize was found to be 0.14±0.03 gC (g DORM)⁻¹. At the sites investigated, root‐produced CO₂ contributed (16±4)% for maize, and (24±4)% for winter wheat, respectively, to the total annual CO₂ production in the soil (450±50 gC m⁻² for maize, 210±30 gC m⁻² for winter wheat).     

Model analysis of the influence of gas diffusivity in soil on CO and H2 uptake

CO and H₂ uptake by soil was studied as a diffusion process. A diffusion model was used to determine how the surface fluxes (net deposition velocities) were controlled by in‐situ microbial uptake rates and soil gas diffusivity calculated from the 3‐phase system (solid, liquid, gas) in the soil. Analytical solutions of the diffusion model assuming vertical uniformity of soil properties showed that physical properties such as air‐filled porosity and soil gas diffusivity were more important in the uptake process than in the emission process. To incorporate the distribution of in‐situ microbial uptake, we used a 2‐layer model incorporating "a microbiologically inactive layer and an active layer" as suggested from experimental results. By numerical simulation using the 2‐layer model, we estimated the effect of several factors on deposition velocities. The variations in soil gas diffusivity due to physical properties, i.e., soil moisture and air‐filled porosity, as well as to the depth of the inactive layer and in‐situ microbial uptake, were found to be important in controlling deposition velocities. This result shows that the diffusion process in soil is critically important for CO and H₂ uptake by soil, at least in soils with higher in‐situ uptake rates and/or with large variation in soil moisture. Similar uptake rates and the difference in deposition velocity between CO and H₂ may be attributable to differences in CO and H₂ molecular diffusivity. The inactive layer is resistant to diffusion and creates uptake limits in CO and H₂ by soil. The coupling of high temperature and a thick inactive layer, common in arid soils, markedly lowers net CO deposition velocity. The temperature for maximum uptake of CO changes with depth of the inactive layer.     

Vertical profiles and storage fluxes of CO2, heat and water in a tropical rainforest at Pasoh, Peninsular Malaysia

Ambient CO₂ concentration, air temperature and relative humidity were measured intermittently for a 3-year period from the floor to the canopy top of a tropical rainforest in Pasoh, Peninsular Malaysia. Mean diurnal CO₂ storage flux ( S _c; μmol m⁻² s⁻¹) and sensible and latent heat storage fluxes ( Q _a and Q _w; W m⁻²) ranged from −12.7 to 3.2 μmol m⁻² s⁻¹, −15 to 27 W m⁻² and −10 to 20 W m⁻², respectively. Small differences in diurnal changes were observed in S _c and Q _a between the driest and wettest periods. Compared with the ranges of mean diurnal CO₂ eddy flux (−14.7 to 4.9 μmol m⁻² s⁻¹), sensible eddy flux (−12 to 169 W m⁻²) and latent eddy flux (0 to 250 W m⁻²), the contribution of CO₂ storage flux was especially large. Comparison with summertime data from a temperate Japanese cypress forest suggested a higher contribution of S _c in the tropical rainforest, probably mainly due to the difference in nighttime friction velocity at the sites. On the other hand, differences in Q _a and Q _w were smaller than the difference in S _c, probably because of the smaller nighttime sinks/sources of heat and water vapour.     

Analysis of regional budgets of sulfur species modeled for the COSAM exercise

The COSAM intercomparison exercise (comparison of large‐scale sulfur models) was organized to compare and evaluate the performance of global sulfur cycle models. Eleven models participated, and from these models the simulated surface concentrations, vertical profiles and budget terms were submitted. This study focuses on simulated budget terms for the sources and sinks of SO₂ and sulfate in three polluted regions in the Northern Hemisphere, i.e., eastern North America, Europe, and Southeast Asia. Qualitatively, features of the sulfur cycle are modeled quite consistently between models, such as the relative importance of dry deposition as a removal mechanism for SO₂, the importance of aqueous phase oxidation over gas phase oxidation for SO₂, and the importance of wet over dry deposition for removal of sulfate aerosol. Quantitatively, however, models may show large differences, especially for cloud‐related processes, i.e., aqueous phase oxidation of SO₂ and sulfate wet deposition. In some cases a specific behavior can be related to the treatment of oxidants for aqueous phase SO₂ oxidation, or the vertical resolution applied in models. Generally, however, the differences between models appear to be related to simulated cloud (micro‐)physics and distributions, whereas differences in vertical transport efficiencies related to convection play an additional rôle. The estimated sulfur column burdens, lifetimes and export budgets vary between models by about a factor of 2 or 3. It can be expected that uncertainties in related effects which are derived from global sulfur model calculations, such as direct and indirect climate forcing estimates by sulfate aerosol, are at least of similar magnitude.     

Seasonal variation of the molecular hydrogen uptake by soils inferred from continuous atmospheric observations in Heidelberg, southwest Germany

The dominant sink of atmospheric molecular hydrogen (H₂) is its enzymatic destruction in soils. Quantitative estimates of the global sink strength, as derived from bottom-up process studies, are, however, still associated to large uncertainties. Here we present an alternative way to estimate atmosphere-to-soil flux densities, respectively deposition velocities of H₂, based on atmospheric H₂ and ²²²Rn observations in the boundary layer. Two and a half years of continuous measurements from a polluted site in the Rhine-Neckar area have been evaluated and night-time flux densities were calculated for situations of strong nocturnal boundary layer inversions using the Radon-Tracer Method. The influences from local anthropogenic combustion sources could be detected and successfully separated by parallel measurements of carbon monoxide. Inferred daily uptake fluxes in the Heidelberg catchment area range from 0.5 to 3 × 10⁻⁸ g H₂ m⁻² s⁻¹ with a mean value of (1.28 ± 0.31) × 10⁻⁸ g H₂ m⁻² s⁻¹. Uptake rates are about 25% larger during summer than during winter, when soil moisture is high, and diffusive transport of H₂ into the soil is inhibited. The mean deposition velocity is 3.0 ± 0.7 × 10⁻² cm s⁻¹_, which is very well in line with direct measurements on similar soil types in Europe and elsewhere.     

Excess 210Po in the coastal atmosphere

Many researchers have reported the widespread occurrence of excess ²¹⁰ Po in the global atmosphere and suggested probable sources such as resuspension of top soils, stratospheric aerosols, sea spray of the surface micro‐layer, volcanic emission, and bio‐volatile ²¹⁰Po species from the productive ocean. We have observed excess ²¹⁰Po on aerosols in the coastal atmosphere of the Chesapeake and Delaware Bays. On‐board measurements in the Chesapeake Bay atmosphere show that the increase of this excess ²¹⁰Po is dependent upon wind speed. Simultaneously measured activity ratios of ⁷Be/²¹⁰Pb and ²¹⁰Pb/²²²Rn argue against either higher altitude air or continental soils as the source of this excess. We hypothesize that the excess ²¹⁰Po originates mainly from surface waters either by the sea‐spray of the surface microlayer, or more likely, by gas exchange. We conclude gas exchange as the mechanism since the polonium excess increases linearly with wind speed over a threshold of 3 m s⁻¹(mean) similar to other gases (i.e., CO₂, SF₆ , and DMS). In addition, higher ²¹⁰Po excess with lower ²²²Rn is observed in on‐shore marine air at Lewes, DE. This suggests sea‐air exchange of volatile Po along with other bio‐volatile species (i.e., DMS, DMSe, and MMHg) in the coastal productive ocean during high wind speeds.     

A pseudo-Lagrangian study of the sulfur budget in the remote Arctic marine boundary layer

The atmospheric sulfur cycle of the remote Arctic marine boundary layer is studied using trajectories and measurements of sulfur compounds from the International Arctic Ocean Expedition 1991, along with a pseudo-Lagrangian approach and an analytical model. The dimethyl sulfide [DMS(g)] turnover time was  h. Only  % of DMS(g) followed reaction paths to sulfur dioxide [SO₂(g)], sub-micrometre aerosol non-seasalt sulfate (nss-SO₄²⁻) or methane sulfonate (MSA). During the first 3 d of transport over the pack ice, fog deposition and drizzle resulted in short turnover times;  h for SO₂(g),  h for MSA and  h for nss-SO₄²⁻. Therefore, DMS(g) will, owing to its origin along or south of the ice edge and longer turnover time, survive the original sub-micrometre sulfur aerosol mass and gradually replace it with new biogenic sulfur aerosol mass. The advection of DMS(g) along with heat and moisture will influence the clouds and fogs over the Arctic pack ice through the formation of cloud condensation nuclei (CCN). If the pack ice cover were to decrease owing to a climate change, the total Arctic Ocean DMS production would change, and potentially there could be an ice–DMS–cloud–albedo climate feedback effect, but it would be accompanied by changes in the fog aerosol sink.     

Size‐segregated chemical, gravimetric and number distribution‐derived mass closure of the aerosol in Sagres, Portugal during ACE‐2

During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R²>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R²= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R²=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.     

Observations of the evolution of the aerosol, cloud and boundary‐layer characteristics during the 1st ACE‐2 Lagrangian experiment

During the 1st Lagrangian experiment of the North Atlantic Regional Aerosol Characterisation Experiment (ACE‐2), a parcel of air was tagged by releasing a smart, constant level balloon into it from the Research Vessel Vodyanitskiy . The Meteorological Research Flight's C‐130 aircraft then followed this parcel over a period of 30 h characterising the marine boundary layer (MBL), the cloud and the physical and chemical aerosol evolution. The air mass had originated over the northern North Atlantic and thus was clean and had low aerosol concentrations. At the beginning of the experiment the MBL was over 1500 m deep and made up of a surface mixed layer (SML) underlying a layer containing cloud beneath a subsidence inversion. Subsidence in the free troposphere caused the depth of the MBL to almost halve during the experiment and, after 26 h, the MBL became well mixed throughout its whole depth. Salt particle mass in the MBL increased as the surface wind speed increased from 8 m s⁻¹ to 16 m s⁻¹ and the accumulation mode (0.1μm to 3.0 μm) aerosol concentrations quadrupled from 50 cm⁻³ to 200 cm⁻³. However, at the same time the total condensation nuclei (>3 nm) decreased from over 1000 cm⁻³ to 750 cm⁻³. The changes in the accumulation mode aerosol concentrations had a significant effect on the observed cloud microphysics. Observational evidence suggests that the important processes in controlling the Aitken mode concentration which, dominated the total CN concentration, included, scavenging of interstitial aerosol by cloud droplets, enhanced coagulation of Aitken mode aerosol and accumulation mode aerosol due to the increased sea salt aerosol surface area, and dilution of the MBL by free tropospheric air.     

Seasonal and global NOx production by lightning estimated from the Optical Transient Detector (OTD)

The Optical Transient Detector (OTD) lightning data for the 12‐month period of 1996 are used to estimate the seasonal and global distributions of lightning‐produced NO _x . The relatively small viewing footprint and the low detection efficiency of the OTD sensor and other difficulties require extrapolations of the OTD data to the actual global flash distributions. Furthermore, available measurements for the ratios of intracloud (IC) to cloud‐to‐ground (CG) flashes have been used to partition lightning counts for IC versus CG flashes from the OTD observations. The resulting lightning distributions are then used to calculate the global and seasonal production of NO _x , assuming a NO production rate of 6.2×10²⁵ molecules for each CG flash and 8.7×10²⁴ molecules for each IC flash. Consequently, we find that CG flashes produce more NO _x than IC flashes despite fewer CG flashes by a factor of 3 or more. NO _x production by lightning varies seasonally in accordance with the global lightning distribution, with the maximum production occurring in the Northern Hemisphere in the local summer. The latitudinal distribution of NO _x production exhibits a strong seasonal variation outside the tropics with the production occurring mainly in the summer hemisphere, whereas in the tropics the production is high throughout the year. The annual contribution to NO _x production by lightning is higher in the Northern Hemisphere than that in the Southern Hemisphere.     

Isotopic composition and origin of polar precipitation in present and glacial climate simulations

The Hamburg atmospheric general circulation model (AGCM) ECHAM‐4 is used to identify the main source regions of precipitation falling on Greenland and Antarctica. Both water isotopes H₂¹⁸O and HDO are explicitly built into the water cycle of the AGCM, and in addition the capability to trace water from different source regions was added to the model. Present and LGM climate simulations show that water from the most important source regions has an isotopic signature similar to the mean isotope values of the total precipitation amount. But water from other source regions (with very different isotopic signatures) contributes an additional, non‐negligible part of the total precipitation amount on both Greenland and Antarctica. Analyses of the temperature‐isotope‐relations for both polar regions reveal a solely bias of the glacial isotope signal on Greenland, which is caused by a strong change in the seasonal deposition of precipitation originating from nearby polar seas and the northern Atlantic. Although the performed simulations under LGM boundary conditions show a decrease of the δ ¹⁸O values in precipitation in agreement with ice core measurements, the AGCM fails to reproduce the observed simultaneous decrease of the deuterium excess signal.     

Precipitable water evaluations from infrared sun‐photometric measurements analyzed using the atmospheric hygrometry technique

Measurements of direct solar irradiance were taken employing 4 different sun‐photometers at near infrared wavelengths, suitable for use in atmospheric hygrometry. This technique utilising a set of spectral ratios, in and out of selected water vapour absorption bands, was applied to the measurements to obtain accurate evaluations of precipitable water. For all the hygrometric ratios given by the 4 sun‐photometers used at the 3 stations of Sagres, Monchique and Mt. Foia, during the CLEARCOLUMN experiment, we determined the calibration curves by correcting them for the Rayleigh scattering effects and, then, plotting the natural logarithms of such corrected ratios versus the square root of the water vapour mass present along the atmospheric slant path. The regression lines drawn for the various scatter diagrams were estimated to give evaluations of precipitable water with an uncertainty of less than 5%, 3% and 10% at the 3 stations, respectively. The calibration curves of the sun‐photometer located at the Sagres station were determined using the precipitable water evaluations obtained from the local radiosounding measurements taken on 5 clear‐sky days. Those of the sun‐photometers used at the Monchique and Mt. Foia stations were instead determined through intercomparison between subsets of measurements simultaneously taken with various instruments at Sagres and Mt. Foia. Using these calibration curves, we examined all the field measurements determining the time‐patterns of precipitable water at the 3 stations. During the period from 16 June to 25 July 1997, precipitable water was found to vary between 1.1 and 3.7 g cm⁻² at the Sagres station (with an accuracy within ±13%), between 1.0 and 2.8 g cm⁻² at Monchique (±11%) and between 0.8 and 3.0 g cm⁻² at the top of Mt. Foia (±26%).     

Feedback mechanisms and sensitivities of ocean carbon uptake under global warming

Global warming simulations are performed with a coupled climate model of reduced complexity to investigate global warming–marine carbon cycle feedbacks. The model is forced by emissions of CO₂ and other greenhouse agents from scenarios recently developed by the Intergovernmental Panel on Climate Change and by CO₂ stabilization profiles. The uptake of atmospheric CO₂ by the ocean is reduced between 7 to 10% by year 2100 compared to simulations without global warming. The reduction is of similar size in the Southern Ocean and in low‐latitude regions (32.5°S‐32.5°N) until 2100, whereas low‐latitude regions dominate on longer time scales. In the North Atlantic the CO₂ uptake is enhanced, unless the Atlantic thermohaline circulation completely collapses. At high latitudes, biologically mediated changes enhance ocean CO₂ uptake, whereas in low‐latitude regions the situation is reversed. Different implementations of the marine biosphere yield a range of 5 to 16% for the total reduction in oceanic CO₂ uptake until year 2100. Modeled oceanic O₂ inventories are significantly reduced in global warming simulations. This suggests that the terrestrial carbon sink deduced from atmospheric O₂/N₂ observations is potentially overestimated if the oceanic loss of O₂ to the atmosphere is not considered.     

Sulfur budget above the Eastern Mediterranean: relative contribution of anthropogenic and biogenic sources

To access the relative contribution of anthropogenic and biogenic sulfur sources to the sulfur budget in the Eastern Mediterranean, an area characterized by very high nss-     levels, measurements of both wet and dry deposition of sulfur were performed at a remote area on the island of Crete (Finokalia) during a 3-yr period (1996–1999). The estimation of dry deposition is based on both gaseous sulfur dioxide (SO₂) and particulate phase non-sea-salt sulfate (nss-     ) and methane sulfonate (MSA) measurements. During the dry period, deposition of SO₂ from long-range transport is the main component of anthropogenic sulfur deposition in the area. The results of the wet and dry deposition obtained at Finokalia have been compared with DMS emission from seawater obtained during two yearly surveys (1997–1998) in the Cretan Sea. Our results indicate that the contribution from biogenic sources to the sulfur budget in the Eastern Mediterranean, although negligible during winter, can account for up to 26% during summer.     

Development of particle size and composition distributions with a novel aerosol dynamics model

An aerosol dynamics model, AEROFOR2, is developed in the context of the BIOFOR project focussing on boreal forest aerosol. It is the second version of a Lagrangian type box model AEROFOR for investigating the formation and growth of particles under clear sky atmospheric conditions. Particles can consist of soluble and insoluble material and the particle population can be externally or internally mixed. AEROFOR2 includes gas phase chemistry and aerosol dynamics, and calculates the number and composition distributions of particles as functions of time. Observed growth rates of the nucleation mode particles after a typical nucleation event are 2–3 nm/h. The model simulations predict that 3·10⁷ molecules cm⁻³ of insoluble organic vapour and less than 6·10⁶ molecules cm⁻³ of soluble vapour condensing onto particles are enough to make them grow in good agreement with the observed growth rates. Then the source rate of the organic vapour must be an order of 10⁵ molecules cm⁻³ s⁻¹, and its saturation vapour density should be below 10⁶ molecules cm⁻³. If the aerosol was initially an internal mixture of soluble (70%) and insoluble (30%) constituents it transformed to an externally mixed aerosol during the simulation. By applying the externally‐mixed aerosol based on measured soluble volume fractions, it was concluded that the modelled soluble fraction of the nucleation mode was too low in comparison with the measurements, and thus, a part of the condensable organic vapour must be water soluble.     

Aerosol modulation of atmospheric and surface solar heating over the tropical Indian Ocean

The major finding of this study is that aerosols over the tropical Indian Ocean enhance clear sky atmospheric solar heating significantly and decrease the surface solar heating by even a larger amount. The results presented here are based on aerosol chemical, microphysical, and optical and radiometric data collected at the island of Kaashidhoo (4.97°N, 73.47°E) during February and March of 1998, as part of the first field phase of the Indian Ocean experiment (INDOEX). The aerosol optical properties were integrated with a multiple scattering Monte Carlo radiative transfer model which was validated at the surface with broadband flux measurements and at the top of the atmosphere (TOA) with the clouds and earth's radiant energy system (CERES) radiation budget measurements. We consider both externally and internally mixed aerosol models with very little difference between the two models in the estimated forcing. For the February–March period, the aerosols increase the monthly mean clear sky atmospheric solar heating by about 12 W/m²(about 15% of the total atmospheric solar heating) and decrease the sea surface clear sky solar heating by about 16 W/m² with a daily range from 5 to 23 W/m². The net aerosol forcing at the top of the atmosphere is about −4 W/m² with a daily range from −2 to −6 W/m². Although the soot contributes only about 10% to the aerosol optical thickness, it contributes more than 50% to the aerosol induced atmospheric solar heating. The fundamental conclusion of this study is that anthropogenic aerosols over the tropical Indian Ocean are altering the clear sky radiation budget of the atmosphere and surface in a major manner.     

Solar dimming and brightening over Thessaloniki, Greece, and Beijing, China

This work presents evidence that ultraviolet (UV)-A solar irradiances show increasing trends at Thessaloniki, Greece, where air quality has been improving because of air pollution abatement strategies. In contrast, over Beijing, China, where air quality measures were taken later, solar brightening was delayed. It is shown that until the early 1990s, UV-A irradiances over Thessaloniki show a downward trend of –0.5% yr⁻¹, which reverses sign and becomes positive in the last decade (+0.8% yr⁻¹). This brightening is related to a decreasing trend in local aerosol amounts. Both the negative rate of change (dimming) and the positive rate of change (brightening) are amplified in the UV-A solar irradiances, compared with the total solar irradiance, by a factor of 2.6. Satellite derived short-wave radiation over Beijing showed negative changes of –0.4% (1984–1991) and –0.1% yr⁻¹ during 1994–2006. The negative trend in solar radiation continued even during 2000–2006. Satellite-derived aerosol optical depth (AOD) increased by +1.0% yr⁻¹ during 2000–2006, in agreement with in situ measurements of increasing AOD. Therefore, a statistically significant change from dimming to brightening in Beijing could not be seen in the last decade, but it is expected to occur in the near future.     

Estimating the Asian radon flux density and its latitudinal gradient in winter using ground-based radon observations at Sado Island

Terrestrial radon-222 flux density for the Asian continent, integrated over distances of 4500 km, is estimated in two 20° latitudinal bands centred on 48.8°N and 63.2°N. The evaluation is based on three years of wintertime radon measurements at Sado Island, Japan, together with meteorological and trajectory information. A selection of 18% of observations are suitable for evaluation of an analytical expression for the continental surface flux. Various meteorological assumptions are discussed; it is found that there is a substantial effect of increased complexity of the formulation on the flux estimates obtained. The distribution of spatially integrated radon flux over the Asian landmass is reported for the first time. Expressed as geometric means and 1σ-ranges, estimated fluxes are 14.1 mBq m⁻² s⁻¹ (1σ-range: 18 mBq m⁻² s⁻¹) and 8.4 mBq m⁻² s⁻¹ (1σ-range: 10 mBq m⁻² s⁻¹) for the lower and higher latitude bands. These results constitute an annual minimum in flux densities for these regions, and are higher than previously reported. The existence of a latitudinal gradient in the continental radon source function is confirmed; the present estimate for Asia (−0.39 mBq m⁻² s⁻¹ per degree of latitude) is in agreement with the northern hemisphere terrestrial radon flux gradient proposed previously.     

Future changes of the atmospheric composition and the impact of climate change

The development of the future atmospheric chemical composition is investigated with respect to NO _y and O₃ by means of the off‐line coupled dynamic‐chemical general circulation model ECHAM3/CHEM. Two time slice experiments have been performed for the years 1992 and 2015, which include changes in sea surface temperatures, greenhouse gas concentrations, emissions of CFCs, NO _x and other species, i.e., the 2015 simulation accounts for changes in chemically relevant emissions and for a climate change and its impact on air chemistry. The 2015 simulation clearly shows a global increase in ozone except for large areas of the lower stratosphere, where no significant changes or even decreases in the ozone concentration are found. For a better understanding of the importance of (A) emissions like NO _x and CFCs, (B) future changes of air temperature and water vapour concentration, and (C) other dynamical parameters, like precipitation and changes in the circulation, diabatic circulation, stratosphere‐troposphere‐exchange, the simulation of the future atmosphere has been performed stepwise. This method requires a climate‐chemistry model without interactive coupling of chemical species. Model results show that the direct effect of emissions (A) plays a major rôle for the composition of the future atmosphere, but they also clearly show that climate change (B and C) has a significant impact and strongly reduces the NO _y and ozone concentration in the lower stratosphere.