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.     

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).     

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.     

An idealized model of the one-dimensional carbon dioxide rectifier effect

The net flux of carbon dioxide (CO₂) from the land surface into the atmospheric boundary layer has a diurnal cycle. Drawdown of CO₂ occurs during daytime photosynthesis, and return of CO₂ to the atmosphere occurs during night. Even when the net diurnal-average surface flux vanishes, the diurnal-average profile of atmospheric CO₂ mixing ratio is usually not vertically uniform. This is because of the diurnal rectifier effect, by which atmospheric vertical transport and the surface flux conspire to produce a surplus of CO₂ near the ground and a deficit aloft.
This paper constructs an idealized, 1-D, eddy-diffusivity model of the rectifier effect and provides an analytic series solution. When non-dimensionalized, the intensity of the rectifier effect is related solely to a single 'rectifier parameter'. Given this model's governing equation and boundary conditions, we prove that the existence of the rectifier effect is related to the correlation of CO₂ gradient and transport, and also to the day–night symmetry of transport.
The rectifier-induced near-surface CO₂ surplus ought to be included in inverse calculations that use near-surface CO₂ mixing ratio to infer land–surface sources and sinks of carbon. Such inverse modeling is facilitated by our model's simplicity. To illustrate, we use a 1-D inverse calculation to infer the amplitude of diurnal CO₂ surface flux.     

Chemical composition of the background aerosol at two sites in southwestern and northwestern China: potential influences of regional transport

Concentrations of organic carbon (OC), elemental carbon (EC), selected trace elements and water-soluble (WS) ions were determined for samples collected from August 2004 to February 2005 to assess the aerosol background at two remote sites in China. The OC and EC concentrations in PM₁₀ from near the Tibetan Plateau at Zhuzhang (ZUZ) were comparable with other background sites, averaging 3.1 and 0.34 μg m⁻³, respectively, with no pronounced seasonality. At Akdala (AKD) on northern margin of the Zhungaer Basin, the average concentrations were similar (mean OC = 2.9 μg m⁻³ and EC = 0.35 μg m⁻³), but the concentrations were higher in winter. The aerosol mass at both sites was dominated by OC and SO₄²⁻, but a stronger contribution from soil dust was observed at AKD. At ZUZ, NO₃⁻ showed a unique weather-related fluctuation in PM₁₀ with a periodicity of ∼1 week. Anthropogenic sources in the Sichuan Basin and southeastern Yunnan Province evidently influence ZUZ in summer and autumn while pollutants from Russia and the China–Mongolia border affect AKD nearly all year. The identification of these upwind sources demonstrates that transboundary transport needs to be taken into account when assessing air quality in remote parts of China.     

Spring initiation and autumn cessation of boreal coniferous forest CO2 exchange assessed by meteorological and biological variables

We studied the commencement and finishing of the growing season using different air temperature indices, the surface albedo, the chlorophyll fluorescence (Fv/Fm) and the carbon dioxide (CO₂) tropospheric concentration, together with eddy covariance measurements of CO₂ flux. We used CO₂ flux data from four boreal coniferous forest sites covering a wide latitudinal range, and CO₂ concentration measurements from Sammaltunturi in Pallas. The CO₂ gas exchange was taken as the primary determinant for the growing season to which other methods were compared.
Indices based on the cumulative temperature sum and the variation in daily mean temperature were successfully used for approximating the start and cessation of the growing season. The beginning of snow melt was a successful predictor of the onset of the growing season. The chlorophyll fluorescence parameter Fv/Fm and the CO₂ concentration were good indicators of both the commencement and cessation of the growing season. By a derivative estimation method for the CO₂ concentration, we were also able to capture the larger-scale spring recovery. The trends of the CO₂ concentration and temperature indices at Pallas/Sammaltunturi were studied over an 11-yr time period, and a significant tendency towards an earlier spring was observed. This tendency was not observed at the other sites.     

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.     

Diurnal variation of CO2 concentration, Δ14C and δ13C in an urban forest: estimate of the anthropogenic and biogenic CO2 contributions

Diurnal variation in the atmospheric CO₂ concentration and the carbon isotopic composition (Δ¹⁴C and δ¹³C) was measured in a forest in an urban area on 9 February 1999. The carbon isotope approach used in the present study differentiated between the quantitative contributions from anthropogenic and biogenic CO₂ sources in the urban atmosphere. The anthropogenic (fossil fuel) and biogenic (soil respiration) contributions was estimated, and they ranged from 1 to 16% and from 2 to 8% of the total atmospheric CO₂. The diurnal variation of the anthropogenic CO₂ was the major cause of the total atmospheric CO₂ variation, while the biogenic CO₂ remained relatively constant throughout the day. Estimating the contribution of soil respired CO₂ provided the mean residence time of soil respired CO₂ within the forest atmosphere.     

Short-wave aerosol radiative efficiency over the global oceans derived from satellite data

Using 5 yr (December 2000–November 2005) of satellite data from the clouds and the earths radiant energy system (CERES) and moderate resolution imaging spectroradiometer (MODIS), we examine the instantaneous short-wave radiative efficiency ( E_τ ) of aerosols during the morning Terra satellite overpass time over the global oceans (60°N–60°S). We calculate E_τ using two commonly used methods. The first method uses the MODIS aerosol optical thickness (AOT) at 0.55 μm with radiative transfer calculations, whereas the second method utilizes the same AOT values along with a new generation of aerosol angular distribution models to convert the CERES-measured broad-band radiances to fluxes. Over the 5 yr, the global mean instantaneous E_τ between the methods is remarkably consistent and within 5 W m⁻²τ⁻¹ with a mean value of –70 W m⁻²τ⁻¹. The largest differences between the methods occur in high-latitude regions, primarily in the Southern Hemisphere, where AOT is low. In dust dominated regions, there is an excellent agreement between the methods with differences of <3 W m⁻²τ⁻¹. These differences are largely due to assumptions in aerosol models and definition of clear sky backgrounds. Independent assessments of aerosol radiative effects from different satellite sensors and methods are extremely valuable and should be used to verify numerical modelling simulations.     

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.     

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.     

Assessment of the soil CO2 gradient method for soil CO2 efflux measurements: comparison of six models in the calculation of the relative gas diffusion coefficient

This paper uses a refined soil gradient method to estimate soil CO₂ efflux. Six different models are used to determine the relative gas diffusion coefficient (ξ). A weighted harmonic averaging is used to estimate the soil CO₂ diffusion coefficient, yielding a better estimate of soil CO₂ efflux. The resulting soil CO₂ efflux results are then compared to the soil CO₂ efflux measured with a soil chamber. Depending on the choice of ξ model used, the estimated soil CO₂ efflux using the gradient method reasonably approximates the efflux obtained using the soil chamber method. In addition, the estimated soil CO₂ efflux obtained by this improved method is well described by an exponential function of soil temperature at a depth of 0.05 m with the temperature sensitivity ( Q ₁₀) of 1.81 and a linear function of soil moisture at a depth of 0.12 m, in general agreement with previous findings. These results suggest that the gradient method is a practical cost-effective means to measure soil CO₂ emissions. Results from the present study suggest that the gradient method can be used successfully to measure soil CO₂ efflux provided that proper attention is paid to the judicious use of the proper diffusion coefficient.     

Aircraft study of aerosol vertical distributions over Beijing and their optical properties

A set of 152 vertical profiles of aerosol number concentration and size distribution with diameter ranging from 0.12 to 3.0 μm observed by the airborne optical spectrometer probe in Beijing, China, between February 2005 and September 2006 is analysed and discussed. The statistic of aerosol number concentration ( N _a) reveals a high aerosol number density in this region with average surface level number concentration ( N ₀) of about 6600 cm⁻³ (0.12–3.0 μm). The average vertical profile of N _a approximately satisfies an exponential decline function with a scale height of 1419 m. The N _a profiles are influenced by the structures of planetary boundary layer (PBL) significantly and two typical types of N _a profile under different conditions of PBL are presented and parametrized in this study. The observations of aerosol size distribution show that, in most cases the aerosol size distributions are not very sensitive to altitude, with effective radii ranging from 0.16 to 0.28 μm. Comparison between aircraft-derived aerosol optical depth (AOD) and Moderate Resolution Imaging Spectroradiometer-derived AOD shows good agreement. The Mie model calculations suggest that the surface level number concentration, the PBL height and the structure of PBL can influence the AOD significantly.     

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.     

Anthropogenic and biogenic winter sources of Arctic CO2—a model study

Long‐range transport of anthropogenic and biogenic CO₂ to a remote site in the Arctic is studied. A limited area, off‐line, Eulerian atmospheric transport model is used, and the results are compared to the observed CO₂ concentration at the "Ny‐Alesund International Arctic Research and Monitoring Facility". Inventories of anthropogenic CO₂ emissions and estimates of biogenic CO₂ emissions are used to investigate the respective impact of these emissions on Arctic CO₂ variations during 4 winter months. A direct comparison of the modelled and observed concentrations reveals remarkably good timing in the modelled variations as compared to the observed variations for most of the time. The correlation of observed versus modelled CO₂ concentration is significant at the 95% confidence level. The biogenic and the anthropogenic CO₂ emissions are shown to have approximately equal influence on Arctic CO₂ variations during winter. Europe is found to be the dominant source of anthropogenic CO₂ at the monitoring station, while Siberia and Northern America have little influence on Arctic CO₂, during the months studied. These results contradict Engardt and Holmén whose results indicate that the lower‐Ob region in western Siberia has a large impact on Arctic CO₂.     

Spectral surface albedo over Morocco and its impact on radiative forcing of Saharan dust

In May–June 2006, airborne and ground-based solar (0.3–2.2 μm) and thermal infrared (4–42 μm) radiation measurements have been performed in Morocco within the Saharan Mineral Dust Experiment (SAMUM). Upwelling and downwelling solar irradiances have been measured using the Spectral Modular Airborne Radiation Measurement System (SMART)-Albedometer. With these data, the areal spectral surface albedo for typical surface types in southeastern Morocco was derived from airborne measurements for the first time. The results are compared to the surface albedo retrieved from collocated satellite measurements, and partly considerable deviations are observed. Using measured surface and atmospheric properties, the spectral and broad-band dust radiative forcing at top-of-atmosphere (TOA) and at the surface has been estimated. The impact of the surface albedo on the solar radiative forcing of Saharan dust is quantified. In the SAMUM case of 19 May 2006, TOA solar radiative forcing varies by 12 W m⁻² per 0.1 surface-albedo change. For the thermal infrared component, values of up to +22 W m⁻² were derived. The net (solar plus thermal infrared) TOA radiative forcing varies between −19 and +24 W m⁻² for a broad-band solar surface albedo of 0.0 and 0.32, respectively. Over the bright surface of southeastern Morocco, the Saharan dust always has a net warming effect.     

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.     

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.     

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.     

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.