The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling study

We have performed simulations using a 3-D global chemistry-transport model to investigate the influence that biogenic emissions from the African continent exert on the composition of the troposphere in the tropical region. For this purpose we have applied two recently developed biogenic emission inventories provided for use in large-scale global models (Granier et al., 2005; LathiSre et al., 2006) whose seasonality and temporal distribution for biogenic emissions of isoprene, other volatile organic compounds and NO is markedly different. The use of the 12 year average values for biogenic emissions provided by LathiSre et al. (2006) results in an increase in the amount of nitrogen sequestrated into longer lived reservoir compounds which contributes to the reduction in the tropospheric ozone burden in the tropics. The associated re-partitioning of nitrogen between PAN, HNO3 and organic nitrates also results in a similar to 5% increase in the loss of nitrogen by wet deposition. At a global scale there is a reduction in the oxidizing capacity of the model atmosphere which increases the atmospheric lifetimes of CH4 and CO by similar to 1.5% and similar to 4%, respectively. Comparisons against a range of different measurements indicate that applying the 12 year average of LathiSre et al. (2006) improves the performance of TM4_AMMA for 2006 in the tropics. By the use of sensitivity studies we show that the release of NO from soils in Africa accounts for between similar to 2-45% of tropospheric ozone in the African troposphere, similar to 10% in the upper troposphere and between similar to 5-20% of the tropical tropospheric ozone column over the tropical Atlantic Ocean. The subsequent reduction in OH over the source regions allows enhanced transport of CO out of the region. For biogenic volatile organic C1 to C3 species released from Africa, the effects on tropical tropospheric ozone are rather limited, although this source contributes to the global burden of VOC by between similar to 2-4% and has a large influence on the organic composition of the troposphere over the tropical Atlantic Ocean

Simulation of tropospheric chemistry and aerosols with the climate model EC-Earth

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

Origin of aerosol particles in the mid-latitude and subtropical upper troposphere and lowermost stratosphere from cluster analysis of CARIBIC data

The origin of aerosol particles in the upper troposphere and lowermost stratosphere over the Eurasian continent was investigated by applying cluster analysis methods to in situ measured data. Number concentrations of submicrometer aerosol particles and trace gas mixing ratios derived by the CARIBIC (Civil Aircraft for Regular Investigation of the Atmosphere Based on an Instrument Container) measurement system on flights between Germany and South-East Asia were used for this analysis. Four cluster analysis methods were applied to a test data set and their capability of separating the data points into scientifically reasonable clusters was assessed. The best method was applied to seasonal data subsets for summer and winter resulting in five cluster or air mass types: stratosphere, tropopause, free troposphere, high clouds, and boundary layer influenced. Other source clusters, like aircraft emissions could not be resolved in the present data set with the used methods. While the cluster separation works satisfactory well for the summer data, in winter interpretation is more difficult, which is attributed to either different vertical transport pathways or different chemical lifetimes in both seasons. The geographical distribution of the clusters together with histograms for nucleation and Aitken mode particles within each cluster are presented. Aitken mode particle number concentrations show a clear vertical gradient with the lowest values in the lowermost stratosphere (750–2820 particles/cm3 STP, minimum of the two 25% – and maximum of the two 75%-percentiles of both seasons) and the highest values for the boundary-layer-influenced air (4290–22 760 particles/cm3 STP). Nucleation mode particles are also highest in the boundary-layer-influenced air (1260–29 500 particles/cm3 STP), but are lowest in the free troposphere (0–450 particles/cm3 STP). The given submicrometer particle number concentrations represent the first large-scale seasonal data sets for the upper troposphere and lowermost stratosphere over the Eurasian continent

Investigating African trace gas sources, vertical transport, and oxidation using IAGOS-CARIBIC measurements between Germany and South Africa between 2009 and 2011

Between March 2009 and March 2011 a commercial airliner equipped with a custom built measurement container (IAGOS-CARIBIC observatory) conducted 13 flights between South Africa and Germany at 10–12 km altitude, traversing the African continent north-south. In-situ measurements of trace gases (CO, CH4, H2O) and aerosol particles indicated that strong surface sources (like biomass burning) and rapid vertical transport combine to generate maximum concentrations in the latitudinal range between 10°N and 10°S coincident with the inter-tropical convergence zone (ITCZ). Pressurized air samples collected during these flights were subsequently analyzed for a suite of trace gases including C2-C8 non-methane hydrocarbons (NMHC) and halocarbons. These shorter-lived trace gases, originating from both natural and anthropogenic sources, also showed near equatorial maxima highlighting the effectiveness of convective transport in this region. Two source apportionment methods were used to investigate the specific sources of NMHC: positive matrix factorization (PMF), which is used for the first time for NMHC analysis in the upper troposphere (UT), and enhancement ratios to CO. Using the PMF method three characteristic airmass types were identified based on the different trace gas concentrations they obtained: biomass burning, fossil fuel emissions, and “background” air. The first two sources were defined with reference to previously reported surface source characterizations, while the term “background” was given to air masses in which the concentration ratios approached that of the lifetime ratios. Comparison of enhancement ratios between NMHC and CO for the subset of air samples that had experienced recent contact with the planetary boundary layer (PBL) to literature values showed that the burning of savanna and tropical forest is likely the main source of NMHC in the African upper troposphere (10–12 km). Photochemical aging patterns for the samples with PBL contact revealed that the air had different degradation histories depending on the hemisphere in which they were emitted. In the southern hemisphere (SH) air masses experienced more dilution by clean background air whereas in the northern hemisphere (NH) air masses are less diluted or mixed with background air still containing longer lived NMHC. Using NMHC photochemical clocks ozone production was seen in the BB outflow above Africa in the NH

CARIBIC aircraft measurements of Eyjafjallajökull volcanic clouds in April/May 2010

The Civil Aircraft for the Regular Investigation of the Atmosphere Based on an Instrument Container (CARIBIC) project investigates physical and chemical processes in the Earth's atmosphere using a Lufthansa Airbus long-distance passenger aircraft. After the beginning of the explosive eruption of the Eyjafjallajökull volcano on Iceland on 14 April 2010, the first CARIBIC volcano-specific measurement flight was carried out over the Baltic Sea and Southern Sweden on 20 April. Two more flights followed: one over Ireland and the Irish Sea on 16 May and the other over the Norwegian Sea on 19 May 2010. During these three special mission flights the CARIBIC container proved its merits as a comprehensive flying laboratory. The elemental composition of particles collected over the Baltic Sea during the first flight (20 April) indicated the presence of volcanic ash. Over Northern Ireland and the Irish Sea (16 May), the DOAS system detected SO2 and BrO co-located with volcanic ash particles that increased the aerosol optical depth. Over the Norwegian Sea (19 May), the optical particle counter detected a strong increase of particles larger than 400 nm diameter in a region where ash clouds were predicted by aerosol dispersion models. Aerosol particle samples collected over the Irish Sea and the Norwegian Sea showed large relative enhancements of the elements silicon, iron, titanium and calcium. Non-methane hydrocarbon concentrations in whole air samples collected on 16 and 19 May 2010 showed a pattern of removal of several hydrocarbons that is typical for chlorine chemistry in the volcanic clouds. Comparisons of measured ash concentrations and simulations with the FLEXPART dispersion model demonstrate the difficulty of detailed volcanic ash dispersion modelling due to the large variability of the volcanic cloud sources, extent and patchiness as well as the thin ash layers formed in the volcanic clouds

Comparison between archived and off-line diagnosed convective mass fluxes in the chemistry transport model TM3

The 40-year reanalysis data set ERA-40 from the European Centre for Medium-Range Weather Forecasts includes, unlike ERA-15, archived convective mass fluxes. These convective fluxes are useful for off-line chemistry transport modeling. The impact of using these archived convective mass fluxes (based on a convective parameterization described in Gregory et al. [2000] ) instead of off-line diagnosed mass fluxes (based on a convective parameterization described in Tiedtke [1989] ) was investigated with the chemistry transport model TM3. At first sight the two types of mass fluxes look similar. However, some differences can be noted: the archived updrafts extend higher than the off-line diagnosed ones; they are also less intense below 500 hPa over sea. The archived downdrafts are much weaker than the off-line diagnosed downdrafts. With archived convective mass fluxes, we found slightly higher ²²²Rn concentrations in the boundary layer, lower ²²²Rn values in the free troposphere and significantly higher ²²²Rn values in the upper troposphere and lower stratosphere. The effect on tropospheric chemistry of using archived mass fluxes instead of diagnosed ones is an increase of NO x and O3 in the free troposphere, but a decrease in the upper troposphere. The differences amount to up to 20% for O3 in the zonal and seasonal mean. Our results thus underline the sensitivity of tropospheric ozone chemistry to the description of convective transport. Comparison with ²²²Rn observations shows that the archived convective mass fluxes give better agreement in the tropical upper troposphere. More comparisons to free tropospheric observations of ²²²Rn or another tracer of convective transport will be needed to unambiguously identify either of the convective data sets as optimal for use in chemistry transport models

An analytical model describing the basic structure and development of mature extratropical cyclones

Understanding the basic structure and development of extratropical cyclones is still quite important in modern meteorology. For this purpose a simple analytical model has been developed that is qualitative as well as quantitative and also reveals modern concepts like the frontal fracture and conveyor belts. The model solution can be derived from the quasigeostrophic equations of the two-layer model with a few additional assumption

Assimilation of GOME total ozone satellite observations in a three-dimensional tracer transport model

A data-assimilation scheme to assimilate the Global Ozone Monitoring Experiment (GOME) total-ozone data is described. The corresponding software (called TM3DAM) has been operational since early 2000 and is used to produce daily ozone analyses and five-day ozone forecasts. The model is a tracer-transport model with a parametrized description of stratospheric gas-phase and heterogeneous ozone chemistry. It is driven by operational meteorological fields from the ECMWF numerical weather-prediction model. TM3DAM analyses near-real-time level-2 ozone data from the GOME instrument on the ESA ERS-2 satellite. The focus of this paper is on the data-assimilation aspects and the analysis results. The assimilation approach is based on the Kalman-filter equations and provides detailed and realistic maps of the forecast error. The analysis scheme is nevertheless computationally efficient. The forecast-minus-observation statistics, accumulated over a two-year period, are described in detail. A comparison with TOMS and Brewer observations shows good agreement. Copyright © 2003 Royal Meteorological Societ