C. Brühl

King Saud University, Ar Riyāḑ, Ar Riyāḑ, Saudi Arabia

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Publications (143)271.62 Total impact

  • Geoscientific Model Development 01/2014; 7:2503-2516. · 5.03 Impact Factor
  • Geoscientific Model Development Discussions 01/2014; 7(3):3367-3402.
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    ABSTRACT: Sulphur dioxide (SO2) is one of the key species determining the aerosol content of the stratosphere. Apart from this study, only three measured profiles of SO2 concentrations (by ATMOS) covering the altitude range of the stratosphere have been published, two of which are heavily perturbed by the Pinatubo eruption and one by El Chichon. Here we present a climatology of monthly and 10° zonal mean profiles of SO2 volume mixing ratios in the altitude range 15-45 km as derived from MIPAS/Envisat measurements from July 2002 until April 2012. The vertical resolution varies from 3.5-4 km in the lower stratosphere up to 6-10 km at the upper end of the profiles with estimated total errors of 5-20 pptv for background conditions of SO2. Comparisons are made with few available observations of SO2 up to high altitudes from ATMOS, for volcanically perturbed situations in the lower stratosphere from ACE-FTS and at the lowest altitudes with stratospheric in-situ observations. The dataset proves for the first time several features of the stratospheric SO2 distribution, which up to now, have only been shown by models: (1) the local maximum of SO2 at around 25-30 km altitude from conversion of COS as the pre-curser of the Junge layer and (2) the downwelling of SO2-rich air to altitudes of 25-30 km at high latitudes during winter and its subsequent depletion during spring as cause for the sudden appearance of enhanced concentrations of condensation nuclei. Comparison with model results of SO2 from the SPARC aerosol assessment report indicate several inconsistencies between simulations and our observations. Further, dedicated EMAC model runs reveal that the strong increase of SO2 to values of 80-100 pptv in the upper stratosphere can only be explained by taking into account visible and near-IR photolysis of H2SO4 and, in addition, a meteoritic sink. Lower stratospheric variability of SO2 can mainly be explained by volcanic activity. A modulation of the mid-stratospheric maximum could be observed for several equatorial eruptions during the time period of observations.
    04/2013;
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    ABSTRACT: A multiyear study with the atmospheric chemistry general circulation model EMAC with the aerosol module GMXe at high altitude resolution demonstrates that the sulfur gases COS and SO2, the latter from low-latitude volcanic eruptions, predominantly control the formation of stratospheric aerosol. The model consistently uses the same parameters in the troposphere and stratosphere for 7 aerosol modes applied. Lower boundary conditions for COS and other long-lived trace gases are taken from measurement networks, while estimates of volcanic SO2 emissions are based on satellite observations. We show comparisons with satellite data for aerosol extinction (e.g. SAGE) and SO2 in the middle atmosphere (MIPAS on ENVISAT). This corroborates the interannual variability induced by the Quasi-Biennial Oscillation, which is internally generated by the model. The model also realistically simulates the radiative effects of stratospheric and tropospheric aerosol including the effects on the model dynamics. The medium strength volcanic eruptions of 2005 and 2006 exerted a nonnegligible radiative forcing of up to -0.6 W m-2 in the tropics, while the large Pinatubo eruption caused a maximum though short term tropical forcing of about -10 W m-2. The study also shows that observed upper stratospheric SO2 can be simulated accurately only when a sulphur sink on meteoritic dust is included and the photolysis of gaseous H2SO4 in the near infrared is higher than assumed previously.
    Atmospheric Chemistry and Physics 04/2013; 13(4):11395-11425. · 4.88 Impact Factor
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    ABSTRACT: Multiyear studies with the atmospheric chemistry general circulation model EMAC with the aerosol module GMXe demonstrate that stratospheric aerosol formation is controlled by COS oxidation and SO2 injected by low-latitude volcanic eruptions. The model consistently uses the same parameters in the troposphere and stratosphere for 7 aerosol modes applied. Calculated radiative heating by aerosol feeds back to stratospheric dynamics. Radiative forcing by stratospheric aerosol can be diagnosed separately. The simulations include the medium size tropical eruptions in 2003, 2005 and 2006 but also the major eruption of Pinatubo in 1991. We show that calculated radiative forcing by stratospheric aerosol agrees well with the corresponding satellite derived quantity and that the medium size tropical eruptions should not be neglected in climate simulations. Changes in temperature, dynamics and tracer transport due to interactive aerosol will be also presented. We show also that calculated aerosol and SO2 concentrations are consistent with the observations by SAGE and by MIPAS on ENVISAT.
    04/2013;
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    ABSTRACT: The photolysis of HONO is important for the atmospheric HOx (OH + HO2) radical budget and ozone formation, especially in polluted air. Nevertheless, owing to the incomplete knowledge of HONO sources, realistic HONO mechanisms have not yet been implemented in global models. We investigated measurement data sets from 15 field measurement campaigns conducted in different countries worldwide. It appears that the HONO/NOx ratio is a good proxy predictor for HONO mixing ratios under different atmospheric conditions. From the robust relationship between HONO and NOx, a representative mean HONO/NOx ratio of 0.02 has been derived. Using a global chemistry-climate model and employing this HONO/NOx ratio, realistic HONO levels are simulated, being about one order of magnitude higher than the reference calculations that only consider the reaction OH + NO → HONO. The resulting enhancement of HONO significantly impacts HOx levels and photo-oxidation products (e.g, O3, PAN), mainly in polluted regions. Furthermore, the relative enhancements in OH and secondary products are higher in winter than in summer, thus enhancing the oxidation capacity in polluted regions, especially in winter when other photolytic OH sources are of minor importance. Our results underscore the need to improve the understanding of HONO chemistry and its representation in atmospheric models.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 10/2012; 12(20):9977-10000. · 5.51 Impact Factor
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    ABSTRACT: The photolysis of HONO is important for the atmospheric HOx (OH+HO2) radical budget and ozone formation, especially in polluted air. Nevertheless, owing to the incomplete knowledge of HONO sources, realistic HONO mechanisms have not yet been implemented in global models. We investigated measurement data sets from 15 field measurement campaigns conducted in different countries worldwide. It appears that the HONO/NOx ratio is a good proxy predictor for HONO mixing ratios under different atmospheric conditions. From the robust relationship between HONO and NOx, a representative mean HONO/NOx ratio of 0.02 has been derived. Using a global chemistry-climate model and employing this HONO/NOx ratio, realistic HONO levels are simulated, being about one order of magnitude higher than the reference calculations, which only consider the reaction OH+NO-> HONO. The resulting enhancement of HONO significantly impacts HOx levels and photo-oxidation products (e.g, O3, PAN), mainly in polluted regions. Furthermore, the relative enhancements in OH and secondary products were higher in winter than in summer, thus enhancing the oxidation capacity in polluted regions, especially in winter, when the other photolytic OH sources are of minor importance. Our results underscore the need to improve the understanding of HONO chemistry and its representation in atmospheric models.
    Atmospheric Chemistry and Physics 05/2012; 12(5):12885-12934. · 4.88 Impact Factor
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    ABSTRACT: In the Project on Solar Effects on Chemistry and Climate Including Ocean Interactions (ProSECCO) fundamental questions of the impact of solar variability on Earth's Climate have been investigated with improved climate system models and observations. On the decadal time scale, the atmospheric signatures of the 11-year Schwabe cycle and the underlying mechanisms have been studied using a comprehensive troposphere-stratosphere-chemistry model. This study included the impact of variations in UV radiation (with 27d rotational cycle) and particle precipitation on stratospheric chemistry and ozone, as well as on the solar signal in the troposphere and on climate. A clear solar signal can be detected not only in the stratosphere, but also in the troposphere. On the centennial to millenium time scale, effects of solar variability on climate of different pre-industrial periods, focusing on the Maunder Minimum and the mid-Holocene, have been addressed using a coupled troposphere-stratosphere-ocean model. A link between the stratospheric polar vortex strength and the solar variability can be detected on the decadal and centennial timescales. A tropospheric signal as response to the solar forcing, for example in the North Atlantic Oscillation, becomes visible once the stratosphere is treated in a realistic way.
    04/2012;
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    ABSTRACT: Simultaneous limb observations of HCOOH, CO, PAN, C2H6, O3, NOx and other species by MIPAS in the upper troposphere and lower stratosphere are compared with results of the chemical circulation model EMAC. To allow for point by point comparisons with the satellite data, the tropospheric meteorology of the CCM is nudged by observations of ECMWF. The method is used for evaluation and further development of the new isoprene oxidation scheme MIM3 and also for checking and distinguishing biogenic and anthropogenic emissions used in the model. We show that the model is able to reproduce the main features of the observations, including the seasonal cycle, and that proper modelling of isoprene chemistry (and to less extent terpene chemistry) is critical for understanding the observed chemical composition of the upper troposphere.
    04/2012;
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    ABSTRACT: A multiyear study with the modular atmospheric chemistry circulation model EMAC with the aerosol module GMXe and high vertical resolution demonstrates that the most abundant sulfur gas in the atmosphere COS is to a large degree responsible for the formation of the stratospheric background aerosol. The model consistently uses the same parameters in the troposphere and stratosphere for the 7 aerosol modes applied. Lower boundary conditions for COS and other longlived gases are taken from observations. We show comparisons with satellite data for aerosol extinction (e.g. SAGE) as well as for SO2 in the middle atmosphere (e.g. ATMOS) and COS. This includes the variation induced by the Quasi-Biennial Oscillation which is internally generated by the model. We also show that organic aerosol contributes significantly to aerosol in the lowermost tropical stratosphere. The radiative impacts of COS and of the COS-induced aerosol will be discussed. Globally, the effects of the anthropogenic contribution of COS on radiative forcing almost cancel. We show that the model is also able to simulate aerosol from SO2 injected by big volcanic eruptions including its radiative effects and implications for geoengineering applications.
    AGU Fall Meeting Abstracts. 12/2011;
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    ABSTRACT: Globally, carbonyl sulphide (COS) is the most abundant sulphur gas in the atmosphere. Our chemistry-climate model of the lower and middle atmosphere with aerosol module realistically simulates the background stratospheric sulphur cycle, as observed by satellites in volcanically quiescent periods. The model results indicate that upward transport of COS from the troposphere largely controls the sulphur budget and the aerosol loading of the background stratosphere. This differs from most previous studies which indicated that short-lived sulphur gases are also important. The model realistically simulates the modulation of the particulate and gaseous sulphur abundance in the stratosphere by the quasi-biennial oscillation (QBO). In the lowermost stratosphere organic carbon aerosol contributes significantly to extinction. Further, we compute that the radiative forcing efficiency by 1 kg of COS is 724 times that of 1 kg CO2, which translates into an overall radiative forcing by anthropogenic COS of 0.003 W m-2. The global warming potentials of COS over time horizons of 20 and 100 yr are GWP(20 yr) = 97 and GWP(100 yr) = 27, respectively (by mass). Furthermore, stratospheric aerosol particles produced by the photolysis of COS contribute to a negative radiative forcing, which amounts to -0.007 W m-2 at the top of the atmosphere for the anthropogenic fraction, more than two times the warming forcing of COS. Considering that the lifetime of COS is twice that of stratospheric aerosols the warming and cooling tendencies approximately cancel. If the forcing of the troposphere near the tropopause is considered, the cooling dominates.
    Atmospheric Chemistry and Physics 06/2011; 11:20823-20854. · 4.88 Impact Factor
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    ABSTRACT: Abstract. The submodel PSC of the ECHAM5/MESSy Atmospheric Chemistry model (EMAC) has been developed to simulate the main types of polar stratospheric clouds (PSC). The parameterisation of the supercooled ternary solutions (STS, type 1b PSC) in the submodel is based on Carslaw et al. (1995b), the thermodynamic approach to simulate ice particles (type 2 PSC) on Marti and Mauersberger (1993). For the formation of nitric acid trihydrate (NAT) particles (type 1a PSC) two different parameterisations exist. The first is based on an instantaneous thermodynamic approach from Hanson and Mauersberger (1988), the second is new implemented and considers the growth of the NAT particles with the aid of a surface growth factor based on Carslaw et al. (2002). It is possible to choose one of this NAT parameterisation in the submodel. This publication explains the background of the submodel PSC and the use of the submodel with the goal of simulating realistic PSC in EMAC.
    Geoscientific Model Development 03/2011; 4:169-182. · 5.03 Impact Factor
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    ABSTRACT: We describe the setup and first results of an inverse modelling system for atmospheric N2O, based on a four-dimensional variational (4DVAR) technique and the atmospheric transport zoom model TM5. We focus in this study on the European domain, utilizing a comprehensive set of quasi-continuous measurements over Europe, complemented by N2O measurements from the Earth System Research Laboratory of the National Oceanic and Atmospheric Administration (NOAA/ESRL) cooperative global air sampling network. Despite ongoing measurement comparisons among networks parallel measurements at a limited number of stations show that significant offsets exist among the different laboratories. Since the spatial gradients of N2O mixing ratios are of the same order of magnitude as these biases, the direct use of these biased datasets would lead to significant errors in the derived emissions. Therefore, in order to also use measurements with unknown offsets, a new bias correction scheme has been implemented within the TM5-4DVAR inverse modelling system, thus allowing the simultaneous assimilation of observations from different networks. The N2O bias corrections determined in the TM5-4DVAR system agree within ~0.1 ppb (dry-air mole fraction) with the bias derived from the measurements at monitoring stations where parallel NOAA discrete air samples are available. The N2O emissions derived for the northwest European and east European countries for 2006 show good agreement with the bottom-up emission inventories reported to the United Nations Framework Convention on Climate Change (UNFCCC). Moreover, the inverse model can significantly narrow the uncertainty range reported in N2O emission inventories for these countries, while the lack of measurements does not allow to reduce the uncertainties of emission estimates in southern Europe. Several sensitivity experiments were performed to test the robustness of the results. It is shown that also inversions without detailed a priori spatio-temporal emission distributions are capable to reproduce major regional emission patterns within the footprint of the existing atmospheric network, demonstrating the strong constraints of the atmospheric observations on the derived emissions.
    Atmospheric Chemistry and Physics 01/2011; 11:2381-2398. · 5.51 Impact Factor
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    ABSTRACT: 1] The stratospheric climate and variability from simulations of sixteen chemistry‐ climate models is evaluated. On average the polar night jet is well reproduced though its variability is less well reproduced with a large spread between models. Polar temperature biases are less than 5 K except in the Southern Hemisphere (SH) lower stratosphere in spring. The accumulated area of low temperatures responsible for polar stratospheric cloud formation is accurately reproduced for the Antarctic but underestimated for the Arctic. The shape and position of the polar vortex is well simulated, as is the tropical upwelling in the lower stratosphere. There is a wide model spread in the frequency of major sudden stratospheric warnings (SSWs), late biases in the breakup of the SH vortex, and a weak annual cycle in the zonal wind in the tropical upper stratosphere. Quantitatively, "metrics" indicate a wide spread in model performance for most diagnostics with systematic biases in many, and poorer performance in the SH than in the Northern Hemisphere (NH). Correlations were found in the SH between errors in the final warming, polar temperatures, the leading mode of variability, and jet strength, and in the NH between errors in polar temperatures, frequency of major SSWs, and jet strength. Models with a stronger QBO have stronger tropical upwelling and a colder NH vortex. Both the qualitative and quantitative analysis indicate a number of common and long‐standing model problems, particularly related to the simulation of the SH and stratospheric variability.
    Journal of Geophysical Research Atmospheres 01/2011; 116. · 3.44 Impact Factor
  • A. Kubin, U. Langematz, C. Brühl
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    ABSTRACT: The CCM simulates the main features of the ozone response to 27 day cycleThe ozone sensitivity is reduced when 13.5 day period is dominantCycle mean response has common vertical structure for strong and weak cycles
    Journal of Geophysical Research Atmospheres 01/2011; 116. · 3.44 Impact Factor
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    ABSTRACT: The response of stratospheric climate and circulation to increasing amounts of greenhouse gases (GHGs) and ozone recovery in the twenty-first century is analyzed in simulations of 11 chemistry–climate models using near-identical forcings and experimental setup. In addition to an overall global cooling of the stratosphere in the simulations (0.59 ± 0.07 K decade−1 at 10 hPa), ozone recovery causes a warming of the Southern Hemisphere polar lower stratosphere in summer with enhanced cooling above. The rate of warming correlates with the rate of ozone recovery projected by the models and, on average, changes from 0.8 to 0.48 K decade−1 at 100 hPa as the rate of recovery declines from the first to the second half of the century. In the winter northern polar lower stratosphere the increased radiative cooling from the growing abundance of GHGs is, in most models, balanced by adiabatic warming from stronger polar downwelling. In the Antarctic lower stratosphere the models simulate an increase in low temperature extremes required for polar stratospheric cloud (PSC) formation, but the positive trend is decreasing over the twenty-first century in all models. In the Arctic, none of the models simulates a statistically significant increase in Arctic PSCs throughout the twenty-first century. The subtropical jets accelerate in response to climate change and the ozone recovery produces a westward acceleration of the lower-stratospheric wind over the Antarctic during summer, though this response is sensitive to the rate of recovery projected by the models. There is a strengthening of the Brewer–Dobson circulation throughout the depth of the stratosphere, which reduces the mean age of air nearly everywhere at a rate of about 0.05 yr decade−1 in those models with this diagnostic. On average, the annual mean tropical upwelling in the lower stratosphere (70 hPa) increases by almost 2% decade−1, with 59% of this trend forced by the parameterized orographic gravity wave drag in the models. This is a consequence of the eastward acceleration of the subtropical jets, which increases the upward flux of (parameterized) momentum reaching the lower stratosphere in these latitudes.
    Journal of Climate 10/2010; 23(2010):5349-5374. · 4.36 Impact Factor
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    ABSTRACT: First results of research performed within the new DFG Research Unit Stratospheric Change and its Role for Climate Prediction (SHARP) will be presented. SHARP investigates past and future changes in stratospheric dynamics and composition to improve the understanding of global climate change and the accuracy of climate change predictions. SHARP combines the efforts of eight German research institutes and expertise in state-of-the-art climate modelling and observations. Within the scope of the scientific sub-project SHARP-OCF (Ozone-Climate-Feedback) the future evolution of stratospheric ozone will be investigated. After a steady decrease in total column ozone from the late 1970s until the middle 1990s, some increases in ozone have been observed in the upper stratosphere (e.g. Steinbrecht et al., 2006). This turnaround is possibly linked to the starting decline of ozone depleting substances (ODSs) in the stratosphere. However, the return of ozone to pre-1980 levels may not occur at the same time as the return of ODSs to pre-1980 levels (WMO, 2007). Changes in atmospheric composition and dynamics since 1980, in particular the increase of greenhouse gases (GHGs), additionally affect the time of the return of ozone to 1980 values. Here, we will present a detailed analysis of the future evolution of ozone in a simulation with the EMAC Chemistry-Climate Model (CCM). The model has been integrated from 1960 to 2100 following the SCN2d scenario recommendations of the SPARC CCMVal initiative for the temporal evolution of GHGs, ODSs and sea surface temperatures as well as sea ice. For estimating the impact of increasing GHG concentrations on the timing of stratospheric ozone recovery, the SCN2d-results will be compared with a second `non-climate change' (NCC) simulation, in which greenhouse gases have been kept fixed at their 1960 concentrations.
    05/2010;
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    ABSTRACT: The evolution of Antarctic climate during the past four decades was characterized by enhanced tropospheric westerlies and a negative trend in near-surface temperature over the Antarctic plateau during the austral summer, while the Antarctic Peninsula showed a warming (Thompson and Solomon, 2002). Model simulations suggested that these trends are most certainly attributable to the Antarctic ozone depletion since the early 1980s (Gillett and Thompson, 2003). However, the more recent publication of Steig et al. (2009) finds a warming of the whole Antarctic continent since 1957 in data from satellites and automatic weather stations. Motivated by this discussion we have analysed changes in stratospheric ozone, temperature and dynamics, and the corresponding signal in Antarctic climate in a transient simulation of the period 1960 to 2000, performed with the stratosphere-troposphere Chemistry-Climate Model (CCM) EMAC. The model has been integrated following the SCN2d scenario recommendations of the SPARC CCMVal initiative for the temporal evolution of greenhouse gases, ozone depleting substances and sea surface temperatures/sea ice. The model reproduces the main observed features of the Antarctic stratosphere since the 1960s, e.g. the establishment of the ozone hole in the 1980s, a negative stratospheric temperature trend, and a longer lived and deeper polar vortex and its more intense breakdown. The enhancement of the tropospheric jet is well reproduced as well. With respect to the near surface trends the model seems to support the recently published results of a weak positive temperature trend all over Antarctica. Analyses of heat and humidity fluxes will be used to support the interpretation of the model results.
    05/2010;
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    ABSTRACT: First results of research performed within the new DFG Research Unit Stratospheric Change and its Role for Climate Prediction (SHARP) will be presented. SHARP investigates past and future changes in stratospheric dynamics and composition to improve the understanding of global climate change and the accuracy of climate change predictions. SHARP combines the efforts of eight German research institutes and expertise in state-of-the-art climate modelling and observations. Within the scope of the scientific sub-project SHARP-BDC (Brewer-Dobson-Circulation) the past and future evolution of the BDC in an atmosphere with changing composition will be analysed. Radiosonde data show an annual mean cooling of the tropical lower stratosphere over the past few decades (Thompson and Solomon, 2005). Several independent model simulations indicate an acceleration of the BDC due to higher greenhouse gas (GHG) concentrations with direct impact on the exchange of air masses between the troposphere and stratosphere (e.g., Butchart et al, 2006). In contrast, from balloon-born measurements no significant acceleration in the BDC could be identified (Engel et al, 2008). This disagreement between observations and model analyses motivates further studies. For the future, expected changes in planetary wave generation and propagation in an atmosphere with increasing GHG concentrations are a major source of uncertainty for predicting future levels of stratospheric composition. To analyse and interpret the past and future evolution of the BDC, results from a transient multi-decadal simulation with the Chemistry-Climate Model (CCM) EMAC will be presented. The model has been integrated from 1960 to 2100 following the SCN2d scenario recommendations of the SPARC CCMVal initiative for the temporal evolution of GHGs, ozone depleting substances and sea surface temperatures as well as sea ice. The role of increasing GHG concentrations for the BDC will be assessed by comparing the SCN2d-results with a `non-climate change' (NCC) simulation, in which greenhouse gases have been kept fixed at their 1960 concentrations.
    05/2010;
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    ABSTRACT: Moist convection in global modelling contributes significantly to the transport of energy, momentum, water and trace gases and aerosols within the troposphere. Since convective clouds are on a scale too small to be resolved in a global model their effects have to be parameterised. However, the whole process of moist convection and especially its parameterisations are associated with uncertainties. In contrast to previous studies on the impact of convection on trace gases, which had commonly neglected the convective transport for some or all compounds, we investigate this issue by examining simulations with five different convection schemes. This permits an uncertainty analysis due to the process formulation, without the inconsistencies inherent in entirely neglecting deep convection or convective tracer transport for one or more tracers. Both the simulated mass fluxes and tracer distributions are analysed. Investigating the distributions of compounds with different characteristics, e.g., lifetime, chemical reactivity, solubility and source distributions, some differences can be attributed directly to the transport of these compounds, whereas others are more related to indirect effects, such as the transport of precursors, chemical reactivity in certain regions, and sink processes. The model simulation data are compared with the average regional profiles of several measurement campaigns, and in detail with two campaigns in fall and winter 2005 in Suriname and Australia, respectively. The shorter-lived a compound is, the larger the differences and consequently the uncertainty due to the convection parameterisation are, as long as it is not completely controlled by local production that is independent of convection and its impacts (e.g. water vapour changes). Whereas for long-lived compounds like CO or O3 the mean differences between the simulations are less than 25%), differences for short-lived compounds reach up to ±100% with different convection schemes. A rating of an overall "best" performing scheme is difficult, since the optimal performance depends on the region and compound.
    ATMOSPHERIC CHEMISTRY AND PHYSICS 02/2010; 10:1931-1951. · 5.51 Impact Factor

Publication Stats

2k Citations
271.62 Total Impact Points

Institutions

  • 2011
    • King Saud University
      Ar Riyāḑ, Ar Riyāḑ, Saudi Arabia
  • 1989–2011
    • Max Planck Institute for Chemistry
      • Department of Atmospheric Chemistry
      Mayence, Rheinland-Pfalz, Germany
  • 2005
    • Max-Planck-Institut für Ökonomik
      Jena, Thuringia, Germany
  • 1997
    • Johannes Gutenberg-Universität Mainz
      Mayence, Rheinland-Pfalz, Germany