The emission of organic compounds from biogenic processes acts as an important source of trace gases in remote regions away from urban conurbations, and is likely to become more important in future ...decades due to the further mitigation of anthropogenic emissions that affect air quality and climate forcing. In this study we examine the contribution of biogenic volatile organic compounds (BVOCs) towards global tropospheric composition using the global 3-D chemistry transport model TM5 and the recently developed modified CB05 chemical mechanism. By comparing regional BVOC emission estimates we show that biogenic processes act as dominant sources for many regions and exhibit a large variability in the annually and seasonally integrated emission fluxes. By performing sensitivity studies we find that the contribution of BVOC species containing between 1 to 3 carbon atoms has an impact on the resident mixing ratios of tropospheric O3 and CO, accounting for ~2.5% and ~10.8% of the simulated global distribution, respectively. This is approximately a third of the cumulative effect introduced by isoprene and the monoterpenes. By examining an ensemble of 3-D global chemistry transport simulations which adopt different global BVOC emission inventories we determine the associated uncertainty introduced towards simulating the composition of the troposphere for the year 2000. By comparing the model ensemble values against a composite of atmospheric measurements we show that the effects on tropospheric O3 are limited to the lower troposphere (with an uncertainty between −2% to 10%), whereas that for tropospheric CO extends up to the upper troposphere (with an uncertainty of between 10 to 45%). Comparing the mixing ratios for low molecular weight alkenes in TM5 against surface measurements taken in Europe implies that the cumulative emission estimates are too low, regardless of the chosen BVOC inventory. This variability in the global distribution of CO due to BVOC emissions introduces an associated uncertainty in the tropospheric CO burden of 11.4%, which impacts strongly on the oxidative capacity of the troposphere, introducing an uncertainty in the atmospheric lifetime of the greenhouse gas CH4 of ~3.3%. This study thus identifies the necessity of placing further constraints on non-CH4 global biogenic emission estimates in large-scale global atmospheric chemistry models.
We present variations of methyl chloride (CH3Cl) and nitrous oxide (N2O) in the lowermost stratosphere (LMS) obtained from air samples collected by the In‐service Aircraft for a Global Observing ...System‐Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (IAGOS‐CARIBIC) passenger aircraft observatory for the period 2008–2012. To correct for the temporal increase of atmospheric N2O, the CARIBIC N2O data are expressed as deviations from the long‐term trend at the northern hemispheric baseline station Mauna Loa, Hawaii (ΔN2O). ΔN2O undergoes a pronounced seasonal variation in the LMS with a minimum in spring. The amplitude increases going deeper in the LMS (up to potential temperature of 40 K above the thermal tropopause), as a result of the seasonally varying subsidence of air from the stratospheric overworld. Seasonal variation of CH3Cl above the tropopause is similar in phase to that of ΔN2O. Significant correlations are found between CH3Cl and ΔN2O in the LMS from winter to early summer, both being affected by mixing between stratospheric air and upper tropospheric air. This correlation, however, disappears in late summer to autumn. The slope of the CH3Cl‐ΔN2O correlation observed in the LMS allows us to determine the stratospheric lifetime of CH3Cl to be 35 ± 7 years. Finally, we examine the partitioning of stratospheric air and tropical/extratropical tropospheric air in the LMS based on a mass balance approach using ΔN2O and CH3Cl. This analysis clearly indicates efficient inflow of tropical tropospheric air into the LMS in summer and demonstrates the usefulness of CH3Cl as a tracer of tropical tropospheric air.
Key Points
Variations of CH3Cl and N2O in the LMS observed by CARIBIC are presented
Stratospheric lifetime of CH3Cl is estimated based on the correlation between CH3Cl and N2O
Partitioning of stratospheric and tropical/extratropical tropospheric air in the LMS is examined
Natural methane (CH4) emissions from wet ecosystems are an important part of today's global CH4 budget. Climate affects the exchange of CH4 between ecosystems and the atmosphere by influencing CH4 ...production, oxidation, and transport in the soil. The net CH4 exchange depends on ecosystem hydrology, soil and vegetation characteristics. Here, the LPJ-WHyMe global dynamical vegetation model is used to simulate global net CH4 emissions for different ecosystems: northern peatlands (45°–90° N), naturally inundated wetlands (60° S–45° N), rice agriculture and wet mineral soils. Mineral soils are a potential CH4 sink, but can also be a source with the direction of the net exchange depending on soil moisture content. The geographical and seasonal distributions are evaluated against multi-dimensional atmospheric inversions for 2003–2005, using two independent four-dimensional variational assimilation systems. The atmospheric inversions are constrained by the atmospheric CH4 observations of the SCIAMACHY satellite instrument and global surface networks. Compared to LPJ-WHyMe the inversions result in a~significant reduction in the emissions from northern peatlands and suggest that LPJ-WHyMe maximum annual emissions peak about one month late. The inversions do not put strong constraints on the division of sources between inundated wetlands and wet mineral soils in the tropics. Based on the inversion results we diagnose model parameters in LPJ-WHyMe and simulate the surface exchange of CH4 over the period 1990–2008. Over the whole period we infer an increase of global ecosystem CH4 emissions of +1.11 Tg CH4 yr−1, not considering potential additional changes in wetland extent. The increase in simulated CH4 emissions is attributed to enhanced soil respiration resulting from the observed rise in land temperature and in atmospheric carbon dioxide that were used as input. The long-term decline of the atmospheric CH4 growth rate from 1990 to 2006 cannot be fully explained with the simulated ecosystem emissions. However, these emissions show an increasing trend of +3.62 Tg CH4 yr−1 over 2005–2008 which can partly explain the renewed increase in atmospheric CH4 concentration during recent years.
An extensive set of in situ water vapor (H sub(2)O) data obtained by the IAGOS-CARIBIC passenger aircraft at 10-12km altitude over 8years (2005-2013) is analyzed. A multifaceted description of the ...vertical distribution of H sub(2)O from the upper troposphere (UT) via the extratropical tropopause mixing layer (exTL) into the lowermost stratosphere (LMS) is given. Compared to longer-lived trace gases, H sub(2)O is highly variable in the UT and exTL. It undergoes considerable seasonal variation, with maxima in summer and in phase from the UT up to ~4km above the tropopause. The transport and dehydration pathways of air starting at the Earth's surface and ending at 10-12km altitude are reconstructed based upon (i) potential temperature (thetas), (ii) relative humidity with respect to ice (RHi), and (iii) back trajectories as a function of altitude relative to the tropopause. RHi of an air mass was found to be primarily determined by its temperature change during recent vertical movement, i.e., cooling during ascent/expansion and warming during descent/compression. The data show, with great clarity, that H sub(2)O and RHi at 10-12km altitude are controlled by three dominant transport/dehydration pathways: (i) the Hadley circulation, i.e., convective uplift in the tropics and poleward directed subsidence drying from the tropical tropopause layer with observed RHi down to 2%; (ii) warm conveyor belts and midlatitude convection transporting moist air into the UT with observed RHi usually above 60%; and (iii) the Brewer-Dobson shallow and deep branches with observed RHi down to 1%. Key Points * Largest data set of water vapor in UT/LMS obtained onboard passenger aircraft * High-resolution description of seasonal variation of water vapor in UT/LMS * Processes controlling water vapor and relative humidity in the UT/LMS
We have integrated the atmospheric chemistry and transport model TM5 into the global climate model EC-Earth version 2.4. We present an overview of the TM5 model and the two-way data exchange between ...TM5 and the IFS model from the European Centre for Medium-Range Weather Forecasts (ECMWF), the atmospheric general circulation model of EC-Earth. In this paper we evaluate the simulation of tropospheric chemistry and aerosols in a one-way coupled configuration. We have carried out a decadal simulation for present-day conditions and calculated chemical budgets and climatologies of tracer concentrations and aerosol optical depth. For comparison we have also performed offline simulations driven by meteorological fields from ECMWF's ERA-Interim reanalysis and output from the EC-Earth model itself. Compared to the offline simulations, the online-coupled system produces more efficient vertical mixing in the troposphere, which reflects an improvement of the treatment of cumulus convection. The chemistry in the EC-Earth simulations is affected by the fact that the current version of EC-Earth produces a cold bias with too dry air in large parts of the troposphere. Compared to the ERA-Interim driven simulation, the oxidizing capacity in EC-Earth is lower in the tropics and higher in the extratropics. The atmospheric lifetime of methane in EC-Earth is 9.4 years, which is 7% longer than the lifetime obtained with ERA-Interim but remains well within the range reported in the literature. We further evaluate the model by comparing the simulated climatologies of surface radon-222 and carbon monoxide, tropospheric and surface ozone, and aerosol optical depth against observational data. The work presented in this study is the first step in the development of EC-Earth into an Earth system model with fully interactive atmospheric chemistry and aerosols.
Influences on stratospheric aerosol during the first four months following the eruption of Kasatochi volcano (Alaska) were studied using observations at 10700 ± 600 m altitude from the CARIBIC ...platform. Collected aerosol samples were analyzed for elemental constituents. Particle number concentrations were recorded in three size intervals together with ozone mixing ratios and slant column densities of SO2. The eruption increased particulate sulfur concentrations by a factor of up to 10 compared to periods before the eruption (1999–2002 and 2005–August 2008). Three to four months later, the concentration was still elevated by a factor of 3 in the lowermost stratosphere at northern midlatitudes. Besides sulfur, the Kasatochi aerosol contained a significant carbonaceous component and ash that declined in time after the eruption. The carbon‐to‐sulfur mass concentration ratio of the volcanic aerosol was 2.6 seven days after the eruption and reached 1.2 after 3–4 months.
Large volcanic eruptions impact significantly on climate and lead to ozone depletion due to injection of particles and gases into the stratosphere where their residence times are long. In this the ...composition of volcanic aerosol is an important but inadequately studied factor. Samples of volcanically influenced aerosol were collected following the Kasatochi (Alaska), Sarychev (Russia) and also during the Eyjafjallajokull (Iceland) eruptions in the period 2008-2010. Sampling was conducted by the CARIBIC platform during regular flights at an altitude of 10-12 km as well as during dedicated flights through the volcanic clouds from the eruption of Eyjafjallajokull in spring 2010. Elemental concentrations of the collected aerosol were obtained by accelerator-based analysis. Aerosol from the Eyjafjallajokull volcanic clouds was identified by high concentrations of sulphur and elements pointing to crustal origin, and confirmed by trajectory analysis. Signatures of volcanic influence were also used to detect volcanic aerosol in stratospheric samples collected following the Sarychev and Kasatochi eruptions. In total it was possible to identify 17 relevant samples collected between 1 and more than 100 days following the eruptions studied. The volcanically influenced aerosol mainly consisted of ash, sulphate and included a carbonaceous component. Samples collected in the volcanic cloud from Eyjafjallajokull were dominated by the ash and sulphate component ( similar to 45% each) while samples collected in the tropopause region and LMS mainly consisted of sulphate (50-77%) and carbon (21-43%). These fractions were increasing/decreasing with the age of the aerosol. Because of the long observation period, it was possible to analyze the evolution of the relationship between the ash and sulphate components of the volcanic aerosol. From this analysis the residence time (1/e) of sulphur dioxide in the studied volcanic cloud was estimated to be 45 plus or minus 22 days.
We present a comprehensive description and benchmark evaluation of the tropospheric chemistry version of the global chemistry transport model TM5 (Tracer Model 5, version TM5-chem-v3.0). A full ...description is given concerning the photochemical mechanism, the interaction with aerosol, the treatment of the stratosphere, the wet and dry deposition parameterizations, and the applied emissions. We evaluate the model against a suite of ground-based, satellite, and aircraft measurements of components critical for understanding global photochemistry for the year 2006. The model exhibits a realistic oxidative capacity at a global scale. The methane lifetime is ~8.9 years with an associated lifetime of methyl chloroform of 5.86 years, which is similar to that derived using an optimized hydroxyl radical field. The seasonal cycle in observed carbon monoxide (CO) is well simulated at different regions across the globe. In the Northern Hemisphere CO concentrations are underestimated by about 20 ppbv in spring and 10 ppbv in summer, which is related to missing chemistry and underestimated emissions from higher hydrocarbons, as well as to uncertainties in the seasonal variation of CO emissions. The model also captures the spatial and seasonal variation in formaldehyde tropospheric columns as observed by SCIAMACHY. Positive model biases over the Amazon and eastern United States point to uncertainties in the isoprene emissions as well as its chemical breakdown. Simulated tropospheric nitrogen dioxide columns correspond well to observations from the Ozone Monitoring Instrument in terms of its seasonal and spatial variability (with a global spatial correlation coefficient of 0.89), but TM5 fields are lower by 25–40%. This is consistent with earlier studies pointing to a high bias of 0–30% in the OMI retrievals, but uncertainties in the emission inventories have probably also contributed to the discrepancy. TM5 tropospheric nitrogen dioxide profiles are in good agreement (within ~0.1 ppbv) with in situ aircraft observations from the INTEX-B campaign over (the Gulf of) Mexico. The model reproduces the spatial and seasonal variation in background surface ozone concentrations and tropospheric ozone profiles from the World Ozone and Ultraviolet Radiation Data Centre to within 10 ppbv, but at several tropical stations the model tends to underestimate ozone in the free troposphere. The presented model results benchmark the TM5 tropospheric chemistry version, which is currently in use in several international cooperation activities, and upon which future model improvements will take place.
African biomass burning emission inventories for gaseous and particulate species have been constructed at a resolution of 1 km by 1km with daily coverage for the 2000-2007 period. These inventories ...are higher than the GFED2 inventories, which are currently widely in use. Evaluation specifically focusing on combustion aerosol has been carried out with the ORISAM-TM4 global chemistry transport model which includes a detailed aerosol module. This paper compares modeled results with measurements of surface BC concentrations and scattering coefficients from the AMMA Enhanced Observations period, aerosol optical depths and single scattering albedo from AERONET sunphotometers, LIDAR vertical distributions of extinction coefficients as well as satellite data. Aerosol seasonal and interannual evolutions over the 2004-2007 period observed at regional scale and more specifically at the Djougou (Benin) and Banizoumbou (Niger) AMMA/IDAF sites are well reproduced by our global model, indicating that our biomass burning emission inventory appears reasonable.
The ash cloud of the Eyjafjallajökull (also referred to as: Eyjafjalla (e.g. Schumann et al., 2011), Eyjafjöll or Eyjafjoll (e.g. Ansmann et al., 2010)) volcano on Iceland caused closure of large ...parts of European airspace in April and May 2010. For the validation and improvement of the European volcanic ash forecast models several research flights were performed. Also the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) flying laboratory, which routinely measures at cruise altitude (approximate11 km) performed three dedicated measurements flights through sections of the ash plume. Although the focus of these flights was on the detection and quantification of the volcanic ash, we report here on sulphur dioxide (SO2 ) and bromine monoxide (BrO) measurements with the CARIBIC DOAS (Differential Optical Absorption Spectroscopy) instrument during the second of these special flights on 16 May 2010. As the BrO and the SO2 observations coincide, we assume the BrO to have been formed inside the volcanic plume. Average SO2 and BrO mixing ratios of approximate40 ppb and approximate5 ppt respectively are retrieved inside the plume. The BrO to SO2 ratio retrieved from the CARIBIC observation is approximate1.3×10-4 . Both SO2 and BrO observations agree well with simultaneous satellite (GOME-2) observations. SO2 column densities retrieved from satellite observations are often used as an indicator for volcanic ash. As the CARIBIC O4 column densities changed rapidly during the plume observation, we conclude that the aerosol and the SO2 plume are collocated. For SO2 some additional information on the local distribution can be derived from a comparison of forward and back scan GOME-2 data. More details on the local plume size and position are retrieved by combining CARIBIC and GOME-2 data.
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