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1.
Dimethylsulphide (DMS) is an important sulphur‐containing trace gas produced by enzymatic cleavage of its precursor compound, dimethylsulphoniopropionate (DMSP), which is released by marine phytoplankton in the upper ocean. After ventilation to the atmosphere, DMS is oxidised to form sulphate aerosols which in the unpolluted marine atmosphere are a major source of cloud condensation nuclei (CCN). Because the micro‐physical properties of clouds relevant to climate change are sensitive to CCN concentration in air, it has been postulated that marine sulphur emissions may play a rôle in climate regulation. The Subantarctic Southern Ocean (41–53°S) is relatively free of anthropogenic sulphur emissions, thus sulphate aerosols will be mainly derived from the biogenic source of DMS, making it an ideal region in which to evaluate the DMS‐climate regulation hypothesis. We have extended a previous modelling analysis of the DMS cycle in this region by employing a coupled general circulation model (CGCM) which has been run in transient mode to provide a more realistic climate scenario. The CGCM output provided meteorological data under the IPCC/IS92a radiative forcing scenario. A DMS production model has been forced with the CGCM climate data to simulate the trend in the sea‐to‐air DMS flux for the period 1960 to 2080, corresponding to equivalent CO2 tripling relative to pre‐industrial levels. The results confirm a minor but non‐negligible increase in DMS flux in this region, in the range +1% to +6% predicted over the period simulated. Uncertainty analysis of the DMS model predictions have confirmed the positive sign for the change in DMS flux, that is a negative DMS feedback on warming.  相似文献   

2.
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).  相似文献   

3.
The recent discovery of an anomalous enrichment in 17O isotope in atmospheric sulfate has opened a new way to investigate the oxidation pathways of sulfur in the atmosphere. From laboratory investigations, it has been suggested that the wet oxidation of sulfur in rain droplets was responsible for the excess 17O. In order to confirm this theory, sulfur and oxygen isotope ratios of different primary sulfates produced during fossil fuel combustion have been investigated and are reported. None of these samples exhibits any anomalous oxygen or sulfur isotopic content, as compared to urban sulfate aerosols. These results, in agreement with the laboratory investigations, reinforce the idea of an aqueous origin for the oxygen-17 anomaly found in tropospheric sulfates.  相似文献   

4.
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.  相似文献   

5.
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.  相似文献   

6.
Potential impact of climate change on marine dimethyl sulfide emissions   总被引：1，自引：0，他引：1  
Dimethyl sulfide (DMS) is a biogenic compound produced in sea-surface water and outgased to the atmosphere. Once in the atmosphere, DMS is a significant source of cloud condensation nuclei in the unpolluted marine atmosphere. It has been postulated that climate may be partly modulated by variations in DMS production through a DMS-cloud condensation nuclei-albedo feedback. We present here a modelled estimation of the response of DMS sea-water concentrations and DMS fluxes to climate change, following previous work on marine DMS modeling ( Aumont et al., 2002 ) and on the global warming impact on marine biology ( Bopp et al., 2001 ). An atmosphere–ocean general circulation model (GCM) was coupled to a marine biogeochemical scheme and used without flux correction to simulate climate response to increased greenhouse gases (a 1% increase per year in atmospheric CO2 until it has doubled). The predicted global distribution of DMS at  1 × CO2  compares reasonably well with observations; however, in the high latitudes, very elevated concentrations of DMS due to spring and summer blooms of Phaeocystis can not be reproduced. At  2 × CO2  , the model estimates a small increase of global DMS flux to the atmosphere (+2%) but with large spatial heterogeneities (from −15% to +30% for the zonal mean). Mechanisms affecting DMS fluxes are changes in (1) marine biological productivity, (2) relative abundance of phytoplankton species and (3) wind intensity. The mean DMS flux perturbation we simulate represents a small negative feedback on global warming; however, the large regional changes may significantly impact regional temperature and precipitation patterns.  相似文献   

7.
Latitudinal distribution of radon-222 flux from continents   总被引：1，自引：0，他引：1  
Global atmospheric transport models are frequently tested by using 222Rn as a tracer. Generally this tracer is assumed to be emitted at a uniform rate (1 atom cm−2 s−1) from all ice-free land surfaces. The analysis of published data suggests a strong decrease from 30°N northwards to 0.2 atom cm−2 s−1 at 70°N. This could be a result of increasing water tables and proportions of organic soils as indicated by larger proportions of wetlands in northern latitudes.  相似文献   

8.
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.  相似文献   

9.
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.  相似文献   

10.
Boron isotope variations in the atmosphere   总被引：2，自引：0，他引：2  
We report here the first measurements of boron isotope ratios in the maritime atmosphere together with those of precipitation. The δ11B values of atmospheric condensates in the western North Pacific and Japanese coast and snow in Tokyo range from −12.8 to +5.1‰ and from −0.4 to +0.4‰, respectively, which are significantly lower than those of rainwater (+18.9 to +34.7‰) collected mostly over the North Pacific. Since the 11B/10B ratios of the atmosphere are lower than those of volcanic emissions (δ11B=+2.3 to +21.4‰), we must seek sources for atmospheric boron other than volcanism. We postulate that the sea may be an important supplier for atmospheric boron under some dynamic conditions and that boron isotope fractionation during evaporation from seawater and removal from the atmosphere may account for the large variations of 11B/10B ratios observed in the atmosphere and precipitation.  相似文献   

11.
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.  相似文献   

12.
Reduction of biosphere life span as a consequence of geodynamics   总被引：1，自引：0，他引：1  
The long‐term co‐evolution of the geosphere–biospere complex from the Proterozoic up to 1.5 billion years into the planet's future is investigated using a conceptual earth system model including the basic geodynamic processes. The model focusses on the global carbon cycle as mediated by life and driven by increasing solar luminosity and plate tectonics. The main CO2 sink, the weathering of silicates, is calculated as a function of biologic activity, global run‐off and continental growth. The main CO2 source, tectonic processes dominated by sea‐floor spreading, is determined using a novel semi‐empirical scheme. Thus, a geodynamic extension of previous geostatic approaches can be achieved. As a major result of extensive numerical investigations, the "terrestrial life corridor", i.e., the biogeophysical domain supporting a photosynthesis‐based ecosphere in the planetary past and in the future, can be identified. Our findings imply, in particular, that the remaining life‐span of the biosphere is considerably shorter (by a few hundred million years) than the value computed with geostatic models by other groups. The "habitable‐zone concept" is also revisited, revealing the band of orbital distances from the sun warranting earth‐like conditions. It turns out that this habitable zone collapses completely in some 1.4 billion years from now as a consequence of geodynamics.  相似文献   

13.
ATTILA: atmospheric tracer transport in a Lagrangian model   总被引：2，自引：0，他引：2  
The model ATTILA has been developed to treat the global-scale transport of passive trace species in the atmosphere within the framework of a general circulation model (GCM). ATTILA runs online within the GCM ECHAM4 and advects the centroids of 80.000 to 190.000 constant mass air parcels. Each trace constituent is thereby represented by a mass mixing ratio in each parcel. ATTILA contains state-of-the-art parameterizations of convection, turbulent boundary layer mixing and inter-parcel transport, and provides an algorithm to map the tracer concentrations from the trajectories to the ECHAM model grid. The transport characteristics of ATTILA are evaluated against observations and the standard semi-Lagrangian transport scheme of ECHAM by two experiments. (1) We simulate the distribution of the short-lived tracer radon (222Rn) in order to examine fast vertical transport over continents, and long-range transport from the continents to remote areas. (2) We simulate the distribution of radiocarbon (14C) from nuclear weapon tests in order to examine upper tropospheric and stratospheric transport characteristics. Contrary to the semi-Lagrangian scheme, ATTILA shows a greatly reduced meridional transport in the upper troposphere and lower stratosphere, and a reduced downward flux from the stratosphere to the troposphere, especially in mid-latitudes. Since ATTILA is a numerically non-diffusive scheme, it is able to maintain steep gradients, which compare better to the observations than the rather smooth gradients produced by the semi-Lagrangian scheme.  相似文献   

14.
Samples of a core (52 m) of ablating Antarctic ice were analysed for 14CO and 14CO2 by accelerator mass spectrometry. The data were compared with a 14C in situ production model that includes muon capture in addition to oxygen spallation by neutrons. The analysis reveals significant in situ 14C at depths below 10 m, which we attribute to 14C production by cosmic ray muons. The age of the ice was determined as 9.3±0.4 14C ka BP.  相似文献   

15.
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.  相似文献   

16.
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.  相似文献   

17.
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.  相似文献   

18.
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.  相似文献   

19.
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.  相似文献   

20.
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.  相似文献   

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