A recent build-up of atmospheric CO2 over Europe. Part 1: observed signals and possible explanations

We analysed interannual and decadal changes in the atmospheric CO₂ concentration gradient (ΔCO₂) between Europe and the Atlantic Ocean over the period 1995–2007. Fourteen measurement stations are used, with Mace-Head being used to define background conditions. The variability of ΔCO₂ reflects fossil fuel emissions and natural sinks activity over Europe, as well as atmospheric transport variability. The mean ΔCO₂ increased by 1–2 ppm at Eastern European stations (∼30% growth), between 1990–1995 and 2000–2005. This built up of CO₂ over the continent is predominantly a winter signal. If the observed increase of ΔCO₂ is explained by changes in ecosystem fluxes, a loss of about 0.46 Pg C per year would be required during 2000–2005. Even if severe droughts have impacted Western Europe in 2003 and 2005, a sustained CO₂ loss of that magnitude is unlikely to be true. We sought alternative explanations for the observed CO₂ build-up into transport changes and into regional redistribution of fossil fuel CO₂ emissions. Boundary layer heights becoming shallower can only explain 32% of the variance of the signal. Regional changes of emissions may explain up to 27% of the build-up. More insights are given in the Aulagnier et al. companion paper.     

Simulating effects of land use changes on carbon fluxes: past contributions to atmospheric CO2 increases and future commitments due to losses of terrestrial sink capacity

The impact of land use on the global carbon cycle and climate is assessed. The Bern carbon cycle-climate model was used with land use maps from HYDE3.0 for 1700 to 2000 A.D. and from post-SRES scenarios for this century. Cropland and pasture expansion each cause about half of the simulated net carbon emissions of 188 Gt C over the industrial period and 1.1 Gt C yr⁻¹ in the 1990s, implying a residual terrestrial sink of 113 Gt C and of 1.8 Gt C yr⁻¹, respectively. Direct CO₂ emissions due to land conversion as simulated in book-keeping models dominate carbon fluxes due to land use in the past. They are, however, mitigated by 25% through the feedback of increased atmospheric CO₂ stimulating uptake. CO₂ stimulated sinks are largely lost when natural lands are converted. Past land use change has eliminated potential future carbon sinks equivalent to emissions of 80–150 Gt C over this century. They represent a commitment of past land use change, which accounts for 70% of the future land use flux in the scenarios considered. Pre-industrial land use emissions are estimated to 45 Gt C at most, implying a maximum change in Holocene atmospheric CO₂ of 3 ppm. This is not compatible with the hypothesis that early anthropogenic CO₂ emissions prevented a new glacial period.     

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.     

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.     

Evaluation of the atmospheric transport model NIRE-CTM-96 by using measured radon-222 concentrations

An atmospheric transport model, NIRE-CTM-96, was evaluated by using measured radon-222 concentrations. The model has 2.5×2.5 degree horizontal resolution and 15 vertical levels. Assimilated global meteorological data for 1990–1996 from the European Centre for Medium Range Weather Forecasts were used to drive the model. We used an emanation rate of radon-222 of 1 atom cm⁻² s⁻¹ over mostly ice-free land. Simulated concentrations were compared with measured concentrations for 22 sites worldwide including 10 stations in China. Simulated annual mean concentrations for Freiburg, Germany, and Socorro, New Mexico, and for four stations in northern China were consistent with the measured concentrations. Simulated daily concentrations for Ogasawara-Hahajima, Japan, correlated well with the measured concentrations. Simulated upper tropospheric concentrations for Moffet Field, California, demonstrated the cross-Pacific transport from central Eurasia and India-Indochina area. Simulated concentrations for two stations in southern China were almost half of the measured concentrations. Mixing layer depth in the model was consistent with other estimates which indicates higher emanation rate there. Simulated concentrations for the South Indian Ocean and the Antarctic during summer were significantly lower than the measured concentrations; this difference was accounted for when emanation from the ocean at a rate of 0.01 atom cm⁻² s⁻¹ was included in the model. The model failed to simulate amplitudes of high-concentration events at Mauna Loa. These high-concentration events were possibly a result of filament-like horizontal structure or laminated vertical structure. The vertical as well as horizontal resolution of the model were supposed to be insufficient to reproduce these fine structures.     

Aircraft observation of carbon dioxide at 8–13 km altitude over the western Pacific from 1993 to 1999

Abstract The spatial and temporal variations of atmospheric CO₂ at 8–13 km from April 1993 to April 1999 were observed by measuring CO₂ mixing ratios in samples collected biweekly from a commercial airliner between Australia and Japan. The CO₂ growth rate showed a considerable interannual variation, with a maximum of about 3 ppm yr⁻¹ during late 1997. This variation is related to the El Niño/Southern Oscillation (ENSO) events. A year-to-year change related to the ENSO events was also found in the latitudinal distribution pattern of the CO₂ annual mean between 30°N and 30°S. The averaged CO₂ seasonal cycle in the Northern Hemisphere gradually decayed toward the equator, and a relatively complicated variation with a double seasonal maximum appeared in the Southern Hemisphere. A significant yearly change of the seasonal cycle pattern was observed in the Southern Hemisphere. The impact of a tropical biomass-burning injection on the upper tropospheric CO₂ was estimated on the basis of the CO data from the same airliner observation.     

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.     

The YAK-AEROSIB transcontinental aircraft campaigns: new insights on the transport of CO2, CO and O3 across Siberia

Two airborne campaigns were carried out to measure the tropospheric concentrations and variability of CO₂, CO and O₃ over Siberia. In order to quantify the influence of remote and regional natural and anthropogenic sources, we analysed a total of 52 vertical profiles of these species collected in April and September 2006, every ∼200 km and up to 7 km altitude. CO₂ and CO concentrations were high in April 2006 (respectively 385–390 ppm CO₂ and 160–200 ppb CO) compared to background values. CO concentrations up to 220 ppb were recorded above 3.5 km over eastern Siberia, with enhancements in 500–1000 m thick layers. The presence of CO enriched air masses resulted from a quick frontal uplift of a polluted air mass exposed to northern China anthropogenic emissions and to fire emissions in northern Mongolia. A dominant Asian origin for CO above 4 km (71.0%) contrasted with a dominant European origin below this altitude (70.9%) was deduced both from a transport model analysis, and from the contrasted ΔCO/ΔCO₂ ratio vertical distribution. In September 2006, a significant O₃ depletion (∼–30 ppb) was repeatedly observed in the boundary layer, as diagnosed from virtual potential temperature profiles and CO₂ gradients, compared to the free troposphere aloft, suggestive of a strong O₃ deposition over Siberian forests.     

Tropospheric carbon dioxide concentrations at a northern boreal site in Finland: basic variations and source areas

Diurnal and annual variations of CO₂, O_3, SO₂, black carbon and condensation nuclei and their source areas were studied by utilizing air parcel trajectories and tropospheric concentration measurements at a boreal GAW site in Pallas, Finland. The average growth trend of CO₂ was about 2.5 ppm yr⁻¹ according to a 4-yr measurement period starting in October 1996. The annual cycle of CO₂ showed concentration difference of about 19 ppm between the summer minimum and winter maximum. The diurnal cycle was most pronounced during July and August. The variation between daily minimum and maximum was about 5 ppm. There was a diurnal cycle in aerosol concentrations during spring and summer. Diurnal variation in ozone concentrations was weak. According to trajectory analysis the site was equally affected by continental and marine air masses. During summer the contribution of continental air increased, although the southernmost influences decreased. During daytime in summer the source areas of CO₂ were mainly located in the northern parts of the Central Europe, while during winter the sources were more evenly distributed. Ozone showed similar source areas during summer, while during winter, unlike CO₂, high concentrations were observed in air arriving from the sea. Sulfur dioxide sources were more northern (Kola peninsula and further east) and CO₂ sources west-weighted in comparison to sources of black carbon. Source areas of black carbon were similar to source areas of aerosols during winter. Aerosol source area distributions showed signs of marine sources during spring and summer.     

Interannual variability of water transport by the East Kamchatka and East Sakhalin Currents and their influence on dissolved oxygen concentration in the Sea of Okhotsk and subarctic pacific

The influence of interannual variability of water transport by the East Kamchatka Current, the Oyashio, and the East Sakhalin Current on the dissolved oxygen concentration in the western subarctic Pacific and the Sea of Okhotsk is considered for studying climate change impact on sea water chemical parameters. It is shown that statistically significant relation is observed between the calculated with the Sverdrup equation interannual variations in water transport with the East Kamchatka Current, the Oyashio, and the East Sakhalin Current and changes in mean sea water level at coastal stations in winter. It is found that the main reason of interannual variability of the dissolved oxygen concentration at isopycnic surfaces in the intermediate water layer (100–800 m) of the Sea of Okhotsk and in the western subarctic Pacific is caused by variations in water transport by the East Kamchatka Current, the Oyashio, and the East Sakhalin Current.     

Atmospheric concentrations and deposition of oxidised sulfur and nitrogen species at Petaling Jaya, Malaysia, 1993–1998

Wet‐only rainwater composition, acid‐precursor gas mixing ratios and aerosol loading were determined from weekly‐averaged samples at Petaling Jaya, Malaysia, over the five year period from March 1993 to March 1998. Annual deposition fluxes of acidic sulfur and nitrogen species estimated from these data show this site to be heavily impacted by acidic deposition, with total oxidised sulfur plus nitrogen deposition in the range 277–480 meq m⁻² yr⁻¹. Average contributions were 56% as sulfur species, 44% as nitrogen species, with wet deposition in this region of high rainfall accounting for 67% of total deposition. Thus total acid deposition fluxes were equivalent to levels that provided motivation for emissions reduction programs in both Europe and North America. The possibility of adverse environmental effects in Malaysia caused by acid deposition therefore merits serious consideration and assessment.     

Variations of atmospheric nitrous oxide concentration in the northern and western Pacific

Atmospheric N₂O concentration was observed in the Pacific for the period 1991–2006, using commercial container ships sailing between Japan and North America and between Japan and Australia or New Zealand. The N₂O concentration showed a secular increase and interannual variations at all sampling locations, but a seasonal cycle was detectable only at northern high latitudes. The annual mean N₂O concentration showed little longitudinal variations (within ± 0.3 ppb) in the northern Pacific, but showed a clear north-south gradient of about 0.8 ppb, with higher values in the Northern Hemisphere. The annual mean N₂O was also characterized by especially high values at 30°N due to strong local N₂O emissions and by a steep latitudinal decrease from the equator to 20°S due to the suppression of interhemispheric exchange of air by the South Pacific Convergence Zone. The N₂O growth rate showed an interannual variation with a period of about 3 yr (high-values in 1999 and 2000), with a delayed eastward and poleward phase propagation in the northern and western Pacific, respectively. The interannual variations of the N₂O growth rate and soil water showed a good correlation, suggesting that the N₂O emission from soils have an important causative role in the atmospheric N₂O variation.     

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).     

Modes of variability of Southern Hemisphere atmospheric circulation estimated by AGCMs

The seasonal mean variability of the atmospheric circulation is affected by processes with time scales from less than seasonal to interannual or longer. Using monthly mean data from an ensemble of Atmospheric General Circulation Model (AGCM) realisations, the interannual variability of the seasonal mean is separated into intraseasonal, and slowly varying components. For the first time, using a recently developed method, the slowly varying component in multiple AGCM ensembles is further separated into internal and externally forced components. This is done for Southern Hemisphere 500?hPa geopotential height from five AGCMs in the CLIVAR International Climate of the Twentieth Century project for the summer and winter seasons. In both seasons, the intraseasonal and slow modes of variability are qualitatively well reproduced by the models when compared with reanalysis data, with a relative metric finding little overall difference between the models. The Southern Annular Mode (SAM) is by far the dominant mode of slowly varying internal atmospheric variability. Two slow-external modes of variability are related to El Ni?o-Southern Oscillation (ENSO) variability, and a third is the atmospheric response to trends in external forcing. An ENSO-SAM relationship is found in the model slow modes of variability, similar to that found by earlier studies using reanalysis data. There is a greater spread in the representation of model slow-external modes in winter than summer, particularly in the atmospheric response to external forcing trends. This may be attributable to weaker external forcing constraints on SH atmospheric circulation in winter.     

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.     

Reconciliation of excess 14C-constrained global CO2 piston velocity estimates

Oceanic excess radiocarbon data is widely used as a constraint for air–sea gas exchange. However, recent estimates of the global mean piston velocity  〈 k 〉  from Naegler et al., Krakauer et al., Sweeney et al. and Müller et al. differ substantially despite the fact that they all are based on excess radiocarbon data from the GLODAP data base. Here I show that these estimates of  〈 k 〉  can be reconciled if first, the changing oceanic radiocarbon inventory due to net uptake of CO₂ is taken into account; second, if realistic reconstructions of sea surface  Δ¹⁴C  are used and third, if  〈 k 〉  is consistently reported with or without normalization to a Schmidt number of 660. These corrections applied, unnormalized estimates of  〈 k 〉  from these studies range between 15.1 and 18.2 cm h⁻¹. However, none of these estimates can be regarded as the only correct value for  〈 k 〉  . I thus propose to use the 'average' of the corrected values of  〈 k 〉  presented here (16.5 ± 3.2 cm h⁻¹) as the best available estimate of the global mean unnormalized piston velocity  〈 k 〉  , resulting in a gross ocean-to-atmosphere CO₂ flux of 76 ± 15 PgC yr⁻¹ for the mid-1990s.     

Vertical profiles of biospheric and fossil fuel-derived CO2 and fossil fuel CO2 : CO ratios from airborne measurements of Δ14C, CO2 and CO above Colorado, USA

Measurements of  Δ¹⁴C  in atmospheric CO₂ are an effective method of separating CO₂ additions from fossil fuel and biospheric sources or sinks of CO₂. We illustrate this technique with vertical profiles of CO₂ and  Δ¹⁴C  analysed in whole air flask samples collected above Colorado, USA in May and July 2004. Comparison of lower tropospheric composition to cleaner air at higher altitudes (>5 km) revealed considerable additions from respiration in the morning in both urban and rural locations. Afternoon concentrations were mainly governed by fossil fuel emissions and boundary layer depth, also showing net biospheric CO₂ uptake in some cases. We estimate local industrial CO₂:CO emission ratios using in situ measurements of CO concentration. Ratios are found to vary by 100% and average 57 mole CO₂:1 mole CO, higher than expected from emissions inventories. Uncertainty in CO₂ from different sources was ±1.1 to ±4.1 ppm for addition or uptake of −4.6 to 55.8 ppm, limited by  Δ¹⁴C  measurement precision and uncertainty in background  Δ¹⁴C  and CO₂ levels.     

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%).     

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.