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The aerosol-climate modelling system ECHAM5-HAM is introduced. It is based on a flexible microphysical approach and, as the number of externally imposed parameters is minimised, allows the application in a wide range of climate regimes. ECHAM5-HAM predicts the evolution of an ensemble of microphysically interacting internally- and externally-mixed aerosol populations as well as their size-distribution and composition. The size-distribution is represented by a superposition of log-normal modes. In the current setup, the major global aerosol compounds sulfate (SU), black carbon (BC), particulate organic matter (POM), sea salt (SS), and mineral dust (DU) are included. The simulated global annual mean aerosol burdens (lifetimes) for the year 2000 are for SU: 0.80 Tg(S) (3.9 days), for BC: 0.11 Tg (5.4 days), for POM: 0.99 Tg (5.4 days), for SS: 10.5 Tg (0.8 days), and for DU: 8.28 Tg (4.6 days). An extensive evaluation with in-situ and remote sensing measurements underscores that the model results are generally in good agreement with observations of the global aerosol system. The simulated global annual mean aerosol optical depth (AOD) is with 0.14 in excellent agreement with an estimate derived from AERONET measurements (0.14) and a composite derived from MODIS-MISR satellite retrievals (0.16). Regionally, the deviations are not negligible. However, the main patterns of AOD attributable to anthropogenic activity are reproduced.
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The paper by Jensen et al. (2005) provides an excellent use of a microphysical model to examine the logical consequences of high saturation ratios indicated by measurements during a high altitude flight of the NASA WB-57F. I would like to comment on a turn made by the aircraft that makes this particular event harder to interpret.
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This paper presents several analysis techniques relating to large-scale atmospheric waves. Such analysis tools allow the extraction of planetary waves from reanalysis or model datasets, and can contribute to a detailed insight into the forcing, propagation, and vertical structure of planetary waves, and their dynamic impact on the atmosphere. The different tools presented here use time series of space Fourier coefficients in order to extract transient and stationary wave parts by zonal wavenumbers, and to quantify their dynamic effect in the form of sensible heat and momentum fluxes. In this work, they have been applied to model results from the coupled chemistry-climate model ECHAM4.L39(DLR)/CHEM (E39/C) (Hein et al., 2001) and to the ERA-15 reanalysis dataset from ECMWF. We show that E39/C qualitatively matches the variance distribution and vertical structure of transient waves from reanalysis data; quantitative differences can be traced back to the horizontal model resolution and the modelled zonal winds. The modelled polar vortex during Northern Hemisphere winter has previously been shown to be colder and more stable than observed (Hein et al., 2001; Schnadt et al., 2002; a possible explanation is that in the model experiment, a reduced heat flux by long transient waves at high latitudes disturbs and warms the polar vortex less than ERA-15 suggests, thereby leading to an overestimated stationary wavenumber 1 in E39/C. The results show that the tools used are well suited to investigate and estimate the impact of various dynamic processes related to large-scale waves.
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The behavior of the concentration of positive small (or cluster) air ions and naturally charged nanometer aerosol particles (aerosol ions) has been studied on the basis of measurements carried out in a boreal forest at the Hyytiälä SMEAR station, Finland, during the BIOFOR III campaign in spring 1999. Statistical characteristics of the concentrations of cluster ions, two classes of aerosol ions of the sizes of 2.5–8 nm and 8–ca 20 nm and the quantities that determine the balance of small ions in the atmosphere have been given for the nucleation event days and non-event days. The dependence of small ion concentration on the ion loss (sink) due to aerosol particles was investigated applying a model of bipolar diffusion charging of particles by small ions. The small ion concentration and the ion sink were closely correlated (correlation coefficient 87%) when the fog events and the hours of high relative humidity (above 97%), as well as nocturnal calms and weak wind (wind speed<0.6 m s<sup>-1</sup> had been excluded. In the case of nucleation burst events, variations in the concentration of small positive ions were in accordance with the changes caused by the ion sink due to aerosols; no clear indication of positive ion depletion by ion-induced nucleation was found. The estimated average ionization rate of air at the Hyytiälä station in early spring, when the ground was partly covered with snow, was about 4.8 ion pairs cm<sup>-3</sup> s<sup>-1</sup>. The study of the charging state of nanometer aerosol particles (2.5–8 nm) revealed a strong correlation (correlation coefficient 88%) between the concentrations of particles and their charged fraction (positive air ions) during nucleation bursts. The estimated charged fraction of particles, which varied from 3% to 6% considering various nucleation event days, confirms that these particles are almost quasi-steady state charged. Also the particles and air ions in the size range of 8–ca 20 nm showed a good qualitative consistency; the correlation coefficient was 92%.
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We use ground-based observations of CO mixing ratios and vertical column abundances together with tropospheric NO<sub>2</sub> columns from the GOME satellite instrument as constraints for improving the global annual emission estimates of CO and NO<sub>x</sub> for the year 1997. The agreement between concentrations calculated by the global 3-dimensional CTM IMAGES and the observations is optimized using the adjoint modelling technique, which allows to invert for CO and NO<sub>x</sub> fluxes simultaneously, taking their chemical interactions into account. Our analysis quantifies a total of 39 flux parameters, comprising anthropogenic and biomass burning sources over large continental regions, soil and lightning emissions of NO<sub>x</sub>, biogenic emissions of CO and non-methane hydrocarbons, as well as the deposition velocities of both CO and NO<sub>x</sub>. Comparison between observed, prior and optimized CO mixing ratios at NOAA/CMDL sites shows that the inversion performs well at the northern mid- and high latitudes, and that it is less efficient in the Southern Hemisphere, as expected due to the scarsity of measurements over this part of the globe. The inversion, moreover, brings the model much closer to the measured NO<sub>2</sub> columns over all regions. Sensitivity tests show that anthropogenic sources exhibit weak sensitivity to changes of the a priori errors associated to the bottom-up inventory, whereas biomass burning sources are subject to a strong variability. Our best estimate for the 1997 global top-down CO source amounts to 2760 Tg CO. Anthropogenic emissions increase by 28%, in agreement with previous inverse modelling studies, suggesting that the present bottom-up inventories underestimate the anthropogenic CO emissions in the Northern Hemisphere. The magnitude of the optimized NO<sub>x</sub> global source decreases by 14% with respect to the prior, and amounts to 42.1 Tg N, out of which 22.8 Tg N are due to anthropogenic sources. The NO<sub>x</sub> emissions increase over Tropical regions, whereas they decrease over Europe and Asia. Our inversion results have been evaluated against independent observations from aircraft campaigns. This comparison shows that the optimization of CO emissions constrained by both CO and NO<sub>2</sub> observations leads to a better agreement between modelled and observed values, especially in the Tropics and the Southern Hemisphere, compared to the case where only CO observations are used. A posteriori estimation of errors on the control parameters shows that a significant error reduction is achieved for the majority of the anthropogenic source parameters, whereas biomass burning emissions are still subject to large errors after optimization. Nonetheless, the constraints provided by the GOME measurements allow to reduce the uncertainties on savanna burning emissions of both CO and NO<sub>x</sub>, suggesting thus that the incorporation of these data in the inversion yields more robust results for carbon monoxide.
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An Analysis of Covariance (ANCOVA) was used to derive the influence of the meteorological variability on the daily maximum ozone concentrations at 12 low-elevation sites north of the Alps in Switzerland during the four seasons in the 1992–2002 period. The afternoon temperature and the morning global radiation were the variables that accounted for most of the meteorological variability in summer and spring, while other variables that can be related to vertical mixing and dilution of primary pollutants (afternoon global radiation, wind speed, stability or day of the week) were more significant in winter. In addition, the number of days after a frontal passage was important to account for ozone build-up in summer and ozone destruction in winter. The statistical model proved to be a robust tool for reducing the impact of the meteorological variability on the ozone concentrations. The explained variance of the model, averaged over all stations, ranged from 60.2% in winter to 71.9% in autumn. The year-to-year variability of the seasonal medians of daily ozone maxima was reduced by 85% in winter, 60% in summer, and 50% in autumn and spring after the meteorological adjustment. For most stations, no significantly negative trends (at the 95% confidence level) of the summer medians of daily O<sub>3</sub> or O<sub>x</sub> (O<sub>3</sub>+NO<sub>2</sub>) maxima were found despite the significant reduction in the precursor emissions in Central Europe. However, significant downward trends in the summer 90th percentiles of daily O<sub>x</sub> maxima were observed at 6 sites in the region around Zürich (on average −0.73 ppb yr<sup>-1</sup> for those sites). The lower effect of the titration by NO as a consequence of the reduced emissions could partially explain the significantly positive O<sub>3</sub> trends in the cold seasons (on average 0.69 ppb yr<sup>-1</sup> in winter and 0.58 ppb yr<sup>-1</sup> in autumn). The increase of O<sub>x</sub> found for most stations in autumn (on average 0.23 ppb yr<sup>-1</sup>) and winter (on average 0.39 ppb yr<sup>-1</sup>) could be due to increasing European background ozone levels, in agreement with other studies. The statistical model was also able to explain the very high ozone concentrations in summer 2003, the warmest summer in Switzerland for at least ~150 years. On average, the measured daily ozone maximum was 15 ppb (nearly 29%) higher than in the reference period summer 1992–2002, corresponding to an excess of 5 standard deviations of the summer means of daily ozone maxima in that period.
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A thermodynamic modelling framework to predict the equilibrium behaviour of mixed inorganic salt aerosols is developed, and then coupled with a technique for finding a solution to the Kohler equation in order to create a diameter dependent hygroscopic aerosol model (Aerosol Diameter Dependent Equilibrium Model – ADDEM). The model described here provides a robust and accurate inorganic basis using a mole fraction based activity coefficient model and adjusted energies of formation for treating solid precipitation. The model framework can accommodate organic components, though this added complexity is considered in a companion paper, this paper describes the development of the modelling architecture to be used and predictions of an inorganic model alone. The modelling framework has been developed to flexibly use a combination of mixing rules and other potentially more accurate techniques where available to calculate the water content. Comparisons with other state-of-the-art general equilibrium models and experimental data are presented and show excellent agreement. The Kelvin effect can be considered in this scheme using a variety of surface tension models. Comparison of predicted diameter dependent phenomena, such as the increased relative humidity for onset of deliquescence with decreasing diameter, with another diameter dependent model is very good despite the different approach used. The model is subject to various sensitivities. For the inorganic systems studied here, the model is sensitive to choice of surface tension scheme used, which decreases for larger aerosol. Large sensitivities are found for the value of dry density used. It is thus likely that the history of the aerosol studied in a hygroscopic tandem differential mobility analyser (HTDMA), specifically the nature of the drying process that will influence the final crystalline form, will create systematic uncertainties upon comparisons with theoretical predictions. However, the magnitudes of all of the above sensitivities are potentially less than those introduced when using a semi ideal growth factor analogue for certain conditions.
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This paper describes the inclusion of organic particulate material within the Aerosol Diameter Dependent Equilibrium Model (ADDEM) framework described in the companion paper applied to inorganic aerosol components. The performance of ADDEM is analysed in terms of its capability to reproduce the behaviour of various organic and mixed inorganic/organic systems using recently published bulk data. Within the modelling architecture already described two separate thermodynamic models are coupled in an additive approach and combined with a method for solving the Kohler equation in order to develop a tool for predicting the water content associated with an aerosol of known inorganic/organic composition and dry size. For development of the organic module, the widely used group contribution method UNIFAC is employed to explicitly deal with the non-ideality in solution. The UNIFAC predictions for components of atmospheric importance were improved considerably by using revised interaction parameters derived from electro-dynamic balance studies. Using such parameters, the model was found to adequately describe mixed systems including 5–6 dicarboxylic acids, down to low relative humidity conditions. By comparison with electrodynamic balance data, it was also found that the model was capable of capturing the behaviour of aqueous aerosols containing Suwannee River Fulvic acid, a structure previously used to represent the functionality of complex oxidised macromolecules often found in atmospheric aerosols. The additive approach for modelling mixed inorganic/organic systems worked well for a variety of mixtures. As expected, deviations between model predictions and measurements increase with increasing concentration. Available surface tension models, used in evaluating the Kelvin term, were found to reproduce measured data with varying success. Deviations from experimental data increased with increased organic compound complexity. For components only slightly soluble in water, significant deviations from measured surface tension depression behaviour were predicted with both model formalisms tested. A Sensitivity analysis showed that such variation is likely to lead to predicted growth factors within the measurement uncertainty for growth factor taken in the sub-saturated regime. Greater sensitivity was found for the value of dry density used in the assumed form of the dried out aerosol. Comparison with a coupled thermodynamic approach showed that assumed values for interactions parameters may lead to erroneous results where a simple additive approach may provide more accurate results. However, where available, the use of coupled thermodynamics can better reproduce measured behaviour. Further work (and laboratory data) is required to assess whether this difference lies within the experimental uncertainty of observed hygroscopic behaviour for a variety of systems.
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We investigate the formation and evolution of an ice-supersaturated region (ISSR) that was detected by means of an operational radiosonde sounding launched from the meteorological station of Lindenberg on 21 March 2000, 00:00 UTC. The supersaturated layer was situated below the local tropopause, between 320 and 408 hPa altitude. Our investigation uses satellite imagery from METEOSAT and the Advanced Very High Resolution Radiometer (AVHRR) and analyses of the European Centre for Medium-Range Weather Forecasts (ECMWF). Mesoscale simulations reveal that the ISSR was formed by a temporary vertical uplift of upper tropospheric air parcels by 20 to 40 hPa in 1 to 2 h. This resulted in a significant local increase of the specific humidity by the moisture transport from below. The ascent was triggered by the superposition of two internal gravity waves, a mountain wave induced by flow past the Erzgebirge and Riesengebirge south of Lindenberg, and an inertial gravity wave excited by the anti-cyclonically curved jet stream over the Baltic Sea. The wave-induced ISSR was rather thick with a depth of about 2 km. The wave-induced upward motion causing the supersaturation also triggered the formation of a cirrus cloud. METEOSAT imagery shows that the cirrus cloud got optically thick within two hours. During this period another longer lasting thin but extended cirrus existed just beneath the tropopause. The wave-induced ISSR disappeared after about half a day in accordance with the decaying wave activity.
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A transient model simulation of the 40-year time period 1960 to 1999 with the coupled climate-chemistry model (CCM) ECHAM4.L39(DLR)/CHEM shows a stratospheric water vapor increase over the last two decades of 0.7 ppmv and, additionally, a short-term increase after major volcanic eruptions. Furthermore, a long-term decrease in global total ozone as well as a short-term ozone decline in the tropics after volcanic eruptions are modeled. In order to understand the resulting effects of the water vapor changes on lower stratospheric ozone chemistry, different perturbation simulations were performed with the CCM ECHAM4.L39(DLR)/CHEM feeding the water vapor perturbations only to the chemistry part. Two different long-term perturbations of lower stratospheric water vapor, +1 ppmv and +5 ppmv, and a short-term perturbation of +2 ppmv with an e-folding time of two months were applied. An additional stratospheric water vapor amount of 1 ppmv results in a 5–10% OH increase in the tropical lower stratosphere between 100 and 30 hPa. As a direct consequence of the OH increase the ozone destruction by the HO<sub>x</sub> cycle becomes 6.4% more effective. Coupling processes between the HO<sub>x</sub>-family and the NO<sub>x</sub>/ClO<sub>x</sub>-family also affect the ozone destruction by other catalytic reaction cycles. The NO<sub>x</sub> cycle becomes 1.6% less effective, whereas the effectiveness of the ClO<sub>x</sub> cycle is again slightly enhanced. A long-term water vapor increase does not only affect gas-phase chemistry, but also heterogeneous ozone chemistry in polar regions. The model results indicate an enhanced heterogeneous ozone depletion during antarctic spring due to a longer PSC existence period. In contrast, PSC formation in the northern hemisphere polar vortex and therefore heterogeneous ozone depletion during arctic spring are not affected by the water vapor increase, because of the less PSC activity. Finally, this study shows that 10% of the global total ozone decline in the transient model run can be explained by the modeled water vapor increase, but the simulated tropical ozone decrease after volcanic eruptions is caused dynamically rather than chemically.
