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Mapping in situ eddy covariance measurements of terrestrial land–atmosphere fluxes to the globe is a key method for diagnosing the Earth system from a data-driven perspective. We describe the first global products (called X-BASE) from a newly implemented upscaling framework, FLUXCOM-X, representing an advancement from the previous generation of FLUXCOM products in terms of flexibility and technical capabilities. The X-BASE products are comprised of estimates of CO2 net ecosystem exchange (NEE), gross primary productivity (GPP), evapotranspiration (ET), and for the first time a novel, fully data-driven global transpiration product (ETT), at high spatial (0.05°) and temporal (hourly) resolution. X-BASE estimates the global NEE at −5.75 ± 0.33 Pg C yr−1 for the period 2001–2020, showing a much higher consistency with independent atmospheric carbon cycle constraints compared to the previous versions of FLUXCOM. The improvement of global NEE was likely only possible thanks to the international effort to increase the precision and consistency of eddy covariance collection and processing pipelines, as well as to the extension of the measurements to more site years resulting in a wider coverage of bioclimatic conditions. However, X-BASE global net ecosystem exchange shows a very low interannual variability, which is common to state-of-the-art data-driven flux products and remains a scientific challenge. With 125 ± 2.1 Pg C yr−1 for the same period, X-BASE GPP is slightly higher than previous FLUXCOM estimates, mostly in temperate and boreal areas. X-BASE evapotranspiration amounts to 74.7×103 ± 0.9×103 km3 globally for the years 2001–2020 but exceeds precipitation in many dry areas, likely indicating overestimation in these regions. On average 57 % of evapotranspiration is estimated to be transpiration, in good agreement with isotope-based approaches, but higher than estimates from many land surface models. Despite considerable improvements to the previous upscaling products, many further opportunities for development exist. Pathways of exploration include methodological choices in the selection and processing of eddy covariance and satellite observations, their ingestion into the framework, and the configuration of machine learning methods. For this, the new FLUXCOM-X framework was specifically designed to have the necessary flexibility to experiment, diagnose, and converge to more accurate global flux estimates.

The atmospheric composition forecasting system used to produce the Copernicus Atmosphere Monitoring Service (CAMS) forecasts of global aerosol and trace gas distributions, the Integrated Forecasting System (IFS-COMPO), undergoes periodic upgrades. In this study we describe the development of the future operational cycle 49R1 and focus on the implementation of the thermodynamical model EQSAM4Clim version 12, which represents gas–aerosol partitioning processes for the nitric acid–nitrate and ammonia–ammonium couples and computes diagnostic aerosol, cloud, and precipitation pH values at the global scale. This information on aerosol acidity influences the simulated tropospheric chemistry processes associated with aqueous-phase chemistry and wet deposition. The other updates of cycle 49R1 concern wet deposition, sea-salt aerosol emissions, dust optics, and size distribution used for the calculation of sulfate aerosol optics. The implementation of EQSAM4Clim significantly improves the partitioning of reactive nitrogen compounds, decreasing surface concentrations of both nitrate and ammonium in the particulate phase, which reduces PM2.5 biases for Europe, the US, and China, especially during summertime. For aerosol optical depth there is generally a decrease in the simulated wintertime biases and for some regions an increase in the summertime bias. Improvements in the simulated Ångström exponent are noted for almost all regions, resulting in generally good agreement with observations. The diagnostic aerosol and precipitation pH calculated by EQSAM4Clim have been compared to ground observations and published simulation results. For precipitation pH, the annual mean values show relatively good agreement with the regional observational datasets, while for aerosol pH the simulated values over continents are quite close to those simulated by ISORROPIA II. The use of aerosol acidity has a relatively smaller impact on the aqueous-phase production of sulfate compared to the changes in gas-to-particle partitioning induced by the use of EQSAM4Clim.

The Equilibrium Simplified Aerosol Model for Climate version 12 (EQSAM4Clim-v12) has recently been revised to provide an accurate and efficient method for calculating the acidity of atmospheric particles. EQSAM4Clim is based on an analytical concept that is not only sufficiently fast for chemical weather prediction applications but also free of numerical noise, which also makes it attractive for air quality forecasting. EQSAM4Clim allows the calculation of aerosol composition based on the gas–liquid–solid and the reduced gas–liquid partitioning with the associated water uptake for both cases and can therefore provide important information about the acidity of the aerosols. Here we provide a comprehensive description of the recent changes made to the aerosol acidity parameterization (referred to as a version 12) which builds on the original EQSAM4Clim. We evaluate the pH improvements using a detailed box model and compare them against previous model calculations and both ground-based and aircraft observations from the USA and China, covering different seasons and scenarios. We show that, in most cases, the simulated pH is within reasonable agreement with the reference results of the Extended Aerosol Inorganics Model (E-AIM) and of satisfactory accuracy.

Long-term tall-tower eddy-covariance (EC) measurements have been recently established in three European pilot cities as part of the ICOS-Cities project. We conducted a comparison of EC software to ensure a reliable generation of interoperable flux estimates, which is the prerequisite for avoiding methodological biases and improving the comparability of the results. We analyzed datasets covering 5 months collected from EC tall-tower installations located in urbanized areas of Munich, Zurich, and Paris. Fluxes of sensible heat, latent heat, and CO2 were calculated using three software packages (i.e., TK3, EddyPro, and eddy4R) to assess the uncertainty of flux estimations attributed to differences in implemented postprocessing schemes. A very good agreement on the mean values and standard deviations was found across all three sites, which can probably be attributed to a uniform instrumentation, data acquisition, and preprocessing. The overall comparison of final flux time series products showed a good but not yet perfect agreement among the three software packages. TK3 and EddyPro both calculated fluxes with low-frequency spectral correction, resulting in better agreement than between TK3 and the eddy4R workflow with disabled low-frequency spectral treatment. These observed flux discrepancies indicate the crucial role of treating low-frequency spectral loss in flux estimation for tall-tower EC systems.

Fluxes of nitrogen oxides (NOx=NO+NO2) and carbon dioxide (CO2) were measured using eddy covariance at the British Telecommunications (BT) Tower in central London during the coronavirus pandemic. Comparing fluxes to those measured in 2017 prior to the pandemic restrictions and the introduction of the Ultra-Low Emissions Zone (ULEZ) highlighted a 73 % reduction in NOx emissions between the two periods but only a 20 % reduction in CO2 emissions and a 32 % reduction in traffic load. Use of a footprint model and the London Atmospheric Emissions Inventory (LAEI) identified transport and heat and power generation to be the two dominant sources of NOx and CO2 but with significantly different relative contributions for each species. Application of external constraints on NOx and CO2 emissions allowed the reductions in the different sources to be untangled, identifying that transport NOx emissions had reduced by >73 % since 2017. This was attributed in part to the success of air quality policy in central London but crucially due to the substantial reduction in congestion that resulted from pandemic-reduced mobility. Spatial mapping of the fluxes suggests that central London was dominated by point source heat and power generation emissions during the period of reduced mobility. This will have important implications on future air quality policy for NO2 which, until now, has been primarily focused on the emissions from diesel exhausts.

During March–June 2017 emissions of nitrogen oxides were measured via eddy covariance at the British Telecom Tower in central London, UK. Through the use of a footprint model the expected emissions were simulated from the spatially resolved National Atmospheric Emissions Inventory for 2017 and compared with the measured emissions. These simulated emissions were shown to underestimate measured emissions during the daytime by a factor of 1.48, but they agreed well overnight. Furthermore, underestimations were spatially mapped, and the areas around the measurement site responsible for differences in measured and simulated emissions were inferred. It was observed that areas of higher traffic, such as major roads near national rail stations, showed the greatest underestimation by the simulated emissions. These discrepancies are partially attributed to a combination of the inventory not fully capturing traffic conditions in central London and both the spatial and temporal resolution of the inventory not fully describing the high heterogeneity of the urban centre. Understanding of this underestimation may be further improved with longer measurement time series to better understand temporal variation and improved temporal scaling factors to better simulate sub-annual emissions.

The observing system design of multidisciplinary field measurements involves a variety of considerations on logistics, safety, and science objectives. Typically, this is done based on investigator intuition and designs of prior field measurements. However, there is potential for considerable increases in efficiency, safety, and scientific success by integrating numerical simulations in the design process. Here, we present a novel numerical simulation–environmental response function (NS–ERF) approach to observing system simulation experiments that aids surface–atmosphere synthesis at the interface of mesoscale and microscale meteorology. In a case study we demonstrate application of the NS–ERF approach to optimize the Chequamegon Heterogeneous Ecosystem Energy-balance Study Enabled by a High-density Extensive Array of Detectors 2019 (CHEESEHEAD19). During CHEESEHEAD19 pre-field simulation experiments, we considered the placement of 20 eddy covariance flux towers, operations for 72 h of low-altitude flux aircraft measurements, and integration of various remote sensing data products. A 2 h high-resolution large eddy simulation created a cloud-free virtual atmosphere for surface and meteorological conditions characteristic of the field campaign domain and period. To explore two specific design hypotheses we super-sampled this virtual atmosphere as observed by 13 different yet simultaneous observing system designs consisting of virtual ground, airborne, and satellite observations. We then analyzed these virtual observations through ERFs to yield an optimal aircraft flight strategy for augmenting a stratified random flux tower network in combination with satellite retrievals. We demonstrate how the novel NS–ERF approach doubled CHEESEHEAD19's potential to explore energy balance closure and spatial patterning science objectives while substantially simplifying logistics. Owing to its modular extensibility, NS–ERF lends itself to optimizing observing system designs also for natural climate solutions, emission inventory validation, urban air quality, industry leak detection, and multi-species applications, among other use cases.

Flux measurements of nitrogen oxides (NOx) were made over London using airborne eddy covariance from a low-flying aircraft. Seven low-altitude flights were conducted over Greater London, performing multiple overpasses across the city during eight days in July 2014. NOx fluxes across the Greater London region (GLR) exhibited high heterogeneity and strong diurnal variability, with central areas responsible for the highest emission rates (20–30 mg m−2 h−1). Other high-emission areas included the M25 orbital motorway. The complexity of London's emission characteristics makes it challenging to pinpoint single emissions sources definitively using airborne measurements. Multiple sources, including road transport and residential, commercial and industrial combustion sources, are all likely to contribute to measured fluxes. Measured flux estimates were compared to scaled National Atmospheric Emissions Inventory (NAEI) estimates, accounting for monthly, daily and hourly variability. Significant differences were found between the flux-driven emissions and the NAEI estimates across Greater London, with measured values up to 2 times higher in Central London than those predicted by the inventory. To overcome the limitations of using the national inventory to contextualise measured fluxes, we used physics-guided flux data fusion to train environmental response functions (ERFs) between measured flux and environmental drivers (meteorological and surface). The aim was to generate time-of-day emission surfaces using calculated ERF relationships for the entire GLR; 98 % spatial coverage was achieved across the GLR at 400 m2 spatial resolution. All flight leg projections showed substantial heterogeneity across the domain, with high emissions emanating from Central London and major road infrastructure. The diurnal emission structure of the GLR was also investigated, through ERF, with the morning rush hour distinguished from lower emissions during the early afternoon. Overall, the integration of airborne fluxes with an ERF-driven strategy enabled the first independent generation of surface NOx emissions, at high resolution using an eddy-covariance approach, for an entire city region.

Mixing ratios of volatile organic compounds (VOCs) were recorded in two field campaigns in central Beijing as part of the Air Pollution and Human Health in a Chinese Megacity (APHH) project. These data were used to calculate, for the first time in Beijing, the surface–atmosphere fluxes of VOCs using eddy covariance, giving a top-down estimation of VOC emissions from a central area of the city. The results were then used to evaluate the accuracy of the Multi-resolution Emission Inventory for China (MEIC). The APHH winter and summer campaigns took place in November and December 2016 and May and June 2017, respectively. The largest VOC fluxes observed were of small oxygenated compounds such as methanol, ethanol + formic acid and acetaldehyde, with average emission rates of 8.31 ± 8.5, 3.97 ± 3.9 and 1.83 ± 2.0 nmol m−2 s−1, respectively, in the summer. A large flux of isoprene was observed in the summer, with an average emission rate of 5.31 ± 7.7 nmol m−2 s−1. While oxygenated VOCs made up 60 % of the molar VOC flux measured, when fluxes were scaled by ozone formation potential and peroxyacyl nitrate (PAN) formation potential the high reactivity of isoprene and monoterpenes meant that these species represented 30 % and 28 % of the flux contribution to ozone and PAN formation potential, respectively. Comparison of measured fluxes with the emission inventory showed that the inventory failed to capture the magnitude of VOC emissions at the local scale.

A fast-response (10 Hz) chemiluminescence detector for ozone (O3) was used to determine O3 fluxes using the eddy covariance technique at the Penlee Point Atmospheric Observatory (PPAO) on the south coast of the UK during April and May 2018. The median O3 flux was −0.132 mg m−2 h−1 (0.018 ppbv m s−1), corresponding to a deposition velocity of 0.037 cm s−1 (interquartile range 0.017–0.065 cm s−1) – similar to the higher values previously reported for open-ocean flux measurements but not as high as some other coastal results. We demonstrate that a typical single flux observation was above the 2σ limit of detection but had considerable uncertainty. The median 2σ uncertainty of deposition velocity was 0.031 cm s−1 for each 20 min period, which reduces with the square root of the sample size. Eddy covariance footprint analysis of the site indicates that the flux footprint was predominantly over water (> 96 %), varying with atmospheric stability and, to a lesser extent, with the tide. At very low wind speeds when the atmosphere was typically unstable, the observed ozone deposition velocity was elevated, most likely because the footprint contracted to include a greater land contribution in these conditions. At moderate to high wind speeds when atmospheric stability was near-neutral, the ozone deposition velocity increased with wind speed and showed a linear dependence with friction velocity. This observed dependence on friction velocity (and therefore also wind speed) is consistent with the predictions from the one-layer model of Fairall et al. (2007), which parameterises the oceanic deposition of ozone from the fundamental conservation equation, accounting for both ocean turbulence and near-surface chemical destruction, while assuming that chemical O3 destruction by iodide is distributed over depth. In contrast to our observations, the deposition velocity predicted by the recently developed two-layer model of Luhar et al. (2018) (which considers iodide reactivity in both layers but with molecular diffusivity dominating over turbulent diffusivity in the first layer) shows no major dependence of deposition velocity on wind speed and underestimates the measured deposition velocities. These results call for further investigation into the mechanisms and control of oceanic O3 deposition.

Direct measurements of NOx, CO and aromatic volatile organic compound (VOC) (benzene, toluene, C2-benzenes and C3-benzenes) flux were made for a central area of Beijing using the eddy-covariance technique. Measurements were made during two intensive field campaigns in central Beijing as part of the Air Pollution and Human Health (APHH) project, the first in November–December 2016 and the second during May–June 2017, to contrast wintertime and summertime emission rates. There was little difference in the magnitude of NOx flux between the two seasons (mean NOx flux was 4.41 mg m−2 h−1 in the winter compared to 3.55 mg m−2 h−1 in the summer). CO showed greater seasonal variation, with mean CO flux in the winter campaign (34.7 mg m−2 h−1) being over twice that of the summer campaign (15.2 mg m−2 h−1). Larger emissions of aromatic VOCs in summer were attributed to increased evaporation due to higher temperatures. The largest fluxes in NOx and CO generally occurred during the morning and evening rush hour periods, indicating a major traffic source with high midday emissions of CO, indicating an additional influence from cooking fuel. Measured NOx and CO fluxes were then compared to the MEIC 2013 emissions inventory, which was found to significantly overestimate emissions for this region, providing evidence that proxy-based emissions inventories have positive biases in urban centres. This first set of pollutant fluxes measured in Beijing provides an important benchmark of emissions from the city which can help to inform and evaluate current emissions inventories.

We scrutinize the importance of aerosol water for the aerosol optical depth (AOD) calculations using a long-term evaluation of the EQuilibrium Simplified Aerosol Model v4 for climate modeling. EQSAM4clim is based on a single solute coefficient approach that efficiently parameterizes hygroscopic growth, accounting for aerosol water uptake from the deliquescence relative humidity up to supersaturation. EQSAM4clim extends the single solute coefficient approach to treat water uptake of multicomponent mixtures. The gas–aerosol partitioning and the mixed-solution water uptake can be solved analytically, preventing the need for iterations, which is computationally efficient. EQSAM4clim has been implemented in the global chemistry climate model EMAC and compared to ISORROPIA II on climate timescales. Our global modeling results show that (I) our EMAC results of the AOD are comparable to modeling results that have been independently evaluated for the period 2000–2010, (II) the results of various aerosol properties of EQSAM4clim and ISORROPIA II are similar and in agreement with AERONET and EMEP observations for the period 2000–2013, and (III) the underlying assumptions on the aerosol water uptake limitations are important for derived AOD calculations. Sensitivity studies of different levels of chemical aging and associated water uptake show larger effects on AOD calculations for the year 2005 compared to the differences associated with the application of the two gas–liquid–solid partitioning schemes. Overall, our study demonstrates the importance of aerosol water for climate studies.

Low-level flights over tundra wetlands in Alaska and Canada have been conducted during the Airborne Measurements of Methane Emissions (AirMeth) campaigns to measure turbulent methane fluxes in the atmosphere. In this paper we describe the instrumentation and new calibration procedures for the essential pressure parameters required for turbulence sensing by aircraft that exploit suitable regular measurement flight legs without the need for dedicated calibration patterns. We estimate the accuracy of the mean wind and the turbulence measurements. We show that airborne measurements of turbulent fluxes of methane and carbon dioxide using cavity ring-down spectroscopy trace gas analysers together with established turbulence equipment achieve a relative accuracy similar to that of measurements of sensible heat flux if applied during low-level flights over natural area sources. The inertial subrange of the trace gas fluctuations cannot be resolved due to insufficient high-frequency precision of the analyser, but, since this scatter is uncorrelated with the vertical wind velocity, the covariance and thus the flux are reproduced correctly. In the covariance spectra the −7∕3 drop-off in the inertial subrange can be reproduced if sufficient data are available for averaging. For convective conditions and flight legs of several tens of kilometres we estimate the flux detection limit to be about 4 mg m−2 d−1 for w′CH4′, 1.4 g m−2 d−1 for w′CO2′ and 4.2 W m−2 for the sensible heat flux.

The objective of this study was to upscale airborne flux measurements of sensible heat and latent heat and to develop high-resolution flux maps. In order to support the evaluation of coupled atmospheric–land-surface models we investigated spatial patterns of energy fluxes in relation to land-surface properties.We used airborne eddy-covariance measurements acquired by the Polar 5 research aircraft in June–July 2012 to analyze surface fluxes. Footprint-weighted surface properties were then related to 21 529 sensible heat flux observations and 25 608 latent heat flux observations using both remote sensing and modeled data. A boosted regression tree technique was used to estimate environmental response functions between spatially and temporally resolved flux observations and corresponding biophysical and meteorological drivers. In order to improve the spatial coverage and spatial representativeness of energy fluxes we used relationships extracted across heterogeneous Arctic landscapes to infer high-resolution surface energy flux maps, thus directly upscaling the observational data. These maps of projected sensible heat and latent heat fluxes were used to assess energy partitioning in northern ecosystems and to determine the dominant energy exchange processes in permafrost areas. This allowed us to estimate energy fluxes for specific types of land cover, taking into account meteorological conditions. Airborne and modeled fluxes were then compared with measurements from an eddy-covariance tower near Atqasuk.Our results are an important contribution for the advanced, scale-dependent quantification of surface energy fluxes and they provide new insights into the processes affecting these fluxes for the main vegetation types in high-latitude permafrost areas.

To improve the aeolian dust budget calculations with the global ECHAM/MESSy atmospheric chemistry–climate model (EMAC), which combines the Modular Earth Submodel System (MESSy) with the ECMWF/Hamburg (ECHAM) climate model developed at the Max Planck Institute for Meteorology in Hamburg based on a weather prediction model of the European Centre for Medium-Range Weather Forecasts (ECMWF), we have implemented new input data and updates of the emission scheme.The data set comprises land cover classification, vegetation, clay fraction and topography. It is based on up-to-date observations, which are crucial to account for the rapid changes of deserts and semi-arid regions in recent decades. The new Moderate Resolution Imaging Spectroradiometer (MODIS)-based land cover and vegetation data are time dependent, and the effect of long-term trends and variability of the relevant parameters is therefore considered by the emission scheme. All input data have a spatial resolution of at least 0.1° compared to 1° in the previous version, equipping the model for high-resolution simulations.We validate the updates by comparing the aerosol optical depth (AOD) at 550 nm wavelength from a 1-year simulation at T106 (about 1.1°) resolution with Aerosol Robotic Network (AERONET) and MODIS observations, the 10 µm dust AOD (DAOD) with Infrared Atmospheric Sounding Interferometer (IASI) retrievals, and dust concentration and deposition results with observations from the Aerosol Comparisons between Observations and Models (AeroCom) dust benchmark data set. The update significantly improves agreement with the observations and is therefore recommended to be used in future simulations.

Extreme hydrometeorological conditions typically impact ecophysiological processes on land. Satellite-based observations of the terrestrial biosphere provide an important reference for detecting and describing the spatiotemporal development of such events. However, in-depth investigations of ecological processes during extreme events require additional in situ observations. The question is whether the density of existing ecological in situ networks is sufficient for analysing the impact of extreme events, and what are expected event detection rates of ecological in situ networks of a given size. To assess these issues, we build a baseline of extreme reductions in the fraction of absorbed photosynthetically active radiation (FAPAR), identified by a new event detection method tailored to identify extremes of regional relevance. We then investigate the event detection success rates of hypothetical networks of varying sizes. Our results show that large extremes can be reliably detected with relatively small networks, but also reveal a linear decay of detection probabilities towards smaller extreme events in log–log space. For instance, networks with ≈ 100 randomly placed sites in Europe yield a ≥ 90 % chance of detecting the eight largest (typically very large) extreme events; but only a ≥ 50 % chance of capturing the 39 largest events. These findings are consistent with probability-theoretic considerations, but the slopes of the decay rates deviate due to temporal autocorrelation and the exact implementation of the extreme event detection algorithm. Using the examples of AmeriFlux and NEON, we then investigate to what degree ecological in situ networks can capture extreme events of a given size. Consistent with our theoretical considerations, we find that today's systematically designed networks (i.e. NEON) reliably detect the largest extremes, but that the extreme event detection rates are not higher than would be achieved by randomly designed networks. Spatio-temporal expansions of ecological in situ monitoring networks should carefully consider the size distribution characteristics of extreme events if the aim is also to monitor the impacts of such events in the terrestrial biosphere.

Large differences in instrumentation, site setup, data format, and operating system stymie the adoption of a universal computational environment for processing and analyzing eddy-covariance (EC) data. This results in limited software applicability and extensibility in addition to often substantial inconsistencies in flux estimates. Addressing these concerns, this paper presents the systematic development of portable, reproducible, and extensible EC software achieved by adopting a development and systems operation (DevOps) approach. This software development model is used for the creation of the eddy4R family of EC code packages in the open-source R language for statistical computing. These packages are community developed, iterated via the Git distributed version control system, and wrapped into a portable and reproducible Docker filesystem that is independent of the underlying host operating system. The HDF5 hierarchical data format then provides a streamlined mechanism for highly compressed and fully self-documented data ingest and output. The usefulness of the DevOps approach was evaluated for three test applications. First, the resultant EC processing software was used to analyze standard flux tower data from the first EC instruments installed at a National Ecological Observatory (NEON) field site. Second, through an aircraft test application, we demonstrate the modular extensibility of eddy4R to analyze EC data from other platforms. Third, an intercomparison with commercial-grade software showed excellent agreement (R2 = 1.0 for CO2 flux). In conjunction with this study, a Docker image containing the first two eddy4R packages and an executable example workflow, as well as first NEON EC data products are released publicly. We conclude by describing the work remaining to arrive at the automated generation of science-grade EC fluxes and benefits to the science community at large. This software development model is applicable beyond EC and more generally builds the capacity to deploy complex algorithms developed by scientists in an efficient and scalable manner. In addition, modularity permits meeting project milestones while retaining extensibility with time.

We present a sensitivity study on transatlantic dust transport, a process which has many implications for the atmosphere, the ocean and the climate. We investigate the impact of key processes that control the dust outflow, i.e., the emission flux, convection schemes and the chemical aging of mineral dust, by using the EMAC model following Abdelkader et al. (2015). To characterize the dust outflow over the Atlantic Ocean, we distinguish two geographic zones: (i) dust interactions within the Intertropical Convergence Zone (ITCZ), or the dust–ITCZ interaction zone (DIZ), and (ii) the adjacent dust transport over the Atlantic Ocean (DTA) zone. In the latter zone, the dust loading shows a steep and linear gradient westward over the Atlantic Ocean since particle sedimentation is the dominant removal process, whereas in the DIZ zone aerosol–cloud interactions, wet deposition and scavenging processes determine the extent of the dust outflow. Generally, the EMAC simulated dust compares well with CALIPSO observations; however, our reference model configuration tends to overestimate the dust extinction at a lower elevation and underestimates it at a higher elevation. The aerosol optical depth (AOD) over the Caribbean responds to the dust emission flux only when the emitted dust mass is significantly increased over the source region in Africa by a factor of 10. These findings point to the dominant role of dust removal (especially wet deposition) in transatlantic dust transport. Experiments with different convection schemes have indeed revealed that the transatlantic dust transport is more sensitive to the convection scheme than to the dust emission flux parameterization. To study the impact of dust chemical aging, we focus on a major dust outflow in July 2009. We use the calcium cation as a proxy for the overall chemical reactive dust fraction and consider the uptake of major inorganic acids (i.e., H2SO4, HNO3 and HCl) and their anions, i.e., sulfate (SO42−), bisulfate (HSO4−), nitrate (NO3−) and chloride (Cl−), on the surface of mineral particles. The subsequent neutralization reactions with the calcium cation form various salt compounds that cause the uptake of water vapor from the atmosphere, i.e., through the chemical aging of dust particles leading to an increase of 0.15 in the AOD under subsaturated conditions (July 2009 monthly mean). As a result of the radiative feedback on surface winds, dust emissions increased regionally. On the other hand, the aged dust particles, compared to the non-aged particles, are more efficiently removed by both wet and dry deposition due to the increased hygroscopicity and particle size (mainly due to water uptake). The enhanced removal of aged particles decreases the dust burden and lifetime, which indirectly reduces the dust AOD by 0.05 (monthly mean). Both processes can be significant (major dust outflow, July 2009), but the net effect depends on the region and level of dust chemical aging.

We introduce a framework to efficiently parameterise the aerosol water uptake for mixtures of semi-volatile and non-volatile compounds, based on the coefficient, νi. This solute-specific coefficient was introduced in Metzger et al. (2012) to accurately parameterise the single solution hygroscopic growth, considering the Kelvin effect – accounting for the water uptake of concentrated nanometer-sized particles up to dilute solutions, i.e. from the compounds relative humidity of deliquescence (RHD) up to supersaturation (Köhler theory). Here we extend the νi parameterisation from single to mixed solutions. We evaluate our framework at various levels of complexity, by considering the full gas–liquid–solid partitioning for a comprehensive comparison with reference calculations using the E-AIM, EQUISOLV II and ISORROPIA II models as well as textbook examples. We apply our parameterisation in the EQuilibrium Simplified Aerosol Model V4 (EQSAM4clim) for climate simulations, implemented in a box model and in the global chemistry–climate model EMAC. Our results show (i) that the νi approach enables one to analytically solve the entire gas–liquid–solid partitioning and the mixed solution water uptake with sufficient accuracy, (ii) that ammonium sulfate mixtures can be solved with a simple method, e.g. pure ammonium nitrate and mixed ammonium nitrate and (iii) that the aerosol optical depth (AOD) simulations are in close agreement with remote sensing observations for the year 2005. Long-term evaluation of the EMAC results based on EQSAM4clim and ISORROPIA II will be presented separately.

We use the combined Dark Target/Deep Blue aerosol optical depth (AOD) satellite product of the moderate-resolution imaging spectroradiometer (MODIS) collection 6 to study trends over the Middle East between 2000 and 2015. Our analysis corroborates a previously identified positive AOD trend over large parts of the Middle East during the period 2001 to 2012. We relate the annual AOD to precipitation, soil moisture and surface winds to identify regions where these attributes are directly related to the AOD over Saudi Arabia, Iraq and Iran. Regarding precipitation and soil moisture, a relatively small area in and surrounding Iraq turns out to be of prime importance for the AOD over these countries. Regarding surface wind speed, the African Red Sea coastal area is relevant for the Saudi Arabian AOD. Using multiple linear regression we show that AOD trends and interannual variability can be attributed to soil moisture, precipitation and surface winds, being the main factors controlling the dust cycle. Our results confirm the dust driven AOD trends and variability, supported by a decreasing MODIS-derived Ångström exponent and a decreasing AERONET-derived fine mode fraction that accompany the AOD increase over Saudi Arabia. The positive AOD trend relates to a negative soil moisture trend. As a lower soil moisture translates into enhanced dust emissions, it is not needed to assume growing anthropogenic aerosol and aerosol precursor emissions to explain the observations. Instead, our results suggest that increasing temperature and decreasing relative humidity in the last decade have promoted soil drying, leading to increased dust emissions and AOD; consequently an AOD increase is expected due to climate change.

Several initiatives are currently emerging to observe the exchange of energy and matter between the earth's surface and atmosphere standardized over larger space and time domains. For example, the National Ecological Observatory Network (NEON) and the Integrated Carbon Observing System (ICOS) are set to provide the ability of unbiased ecological inference across ecoclimatic zones and decades by deploying highly scalable and robust instruments and data processing. In the construction of these observatories, enclosed infrared gas analyzers are widely employed for eddy covariance applications. While these sensors represent a substantial improvement compared to their open- and closed-path predecessors, remaining high-frequency attenuation varies with site properties and gas sampling systems, and requires correction. Here, we show that components of the gas sampling system can substantially contribute to such high-frequency attenuation, but their effects can be significantly reduced by careful system design. From laboratory tests we determine the frequency at which signal attenuation reaches 50 % for individual parts of the gas sampling system. For different models of rain caps and particulate filters, this frequency falls into ranges of 2.5–16.5 Hz for CO2, 2.4–14.3 Hz for H2O, and 8.3–21.8 Hz for CO2, 1.4–19.9 Hz for H2O, respectively. A short and thin stainless steel intake tube was found to not limit frequency response, with 50 % attenuation occurring at frequencies well above 10 Hz for both H2O and CO2. From field tests we found that heating the intake tube and particulate filter continuously with 4 W was effective, and reduced the occurrence of problematic relative humidity levels (RH > 60 %) by 50 % in the infrared gas analyzer cell. No further improvement of H2O frequency response was found for heating in excess of 4 W. These laboratory and field tests were reconciled using resistor–capacitor theory, and NEON's final gas sampling system was developed on this basis. The design consists of the stainless steel intake tube, a pleated mesh particulate filter and a low-volume rain cap in combination with 4 W of heating and insulation. In comparison to the original design, this reduced the high-frequency attenuation for H2O by ≈ 3∕4, and the remaining cospectral correction did not exceed 3 %, even at high relative humidity (95 %). The standardized design can be used across a wide range of ecoclimates and site layouts, and maximizes practicability due to minimal flow resistance and maintenance needs. Furthermore, due to minimal high-frequency spectral loss, it supports the routine application of adaptive correction procedures, and enables largely automated data processing across sites.

Interactions of desert dust and air pollution over the eastern Mediterranean (EM) have been studied, focusing on two distinct dust transport events on 22 and 28 September 2011. The atmospheric chemistry–climate model EMAC has been used at about 50 km grid spacing, applying an online dust emission scheme and calcium as a proxy for dust reactivity. EMAC includes a detailed tropospheric chemistry mechanism, aerosol microphysics and thermodynamics schemes to describe dust "aging". The model is evaluated using ground-based observations for aerosol concentrations and aerosol optical depth (AOD) as well as satellite observations. Simulation results and back trajectory analysis show that the development of synoptic disturbances over the EM can enhance dust transport from the Sahara and Arabian deserts in frontal systems that also carry air pollution to the EM. The frontal systems are associated with precipitation that controls the dust removal. Our results show the importance of chemical aging of dust, which increases particle size, dust deposition and scavenging efficiency during transport, overall reducing the lifetime relative to non-aged dust particles. The relatively long travel periods of Saharan dust result in more sustained aging compared to Arabian dust. Sensitivity simulations indicate 3 times more dust deposition of aged relative to pristine dust, which significantly decreases the dust lifetime and loading.

We introduce MADE3 (Modal Aerosol Dynamics model for Europe, adapted for global applications, 3rd generation; version: MADE3v2.0b), an aerosol dynamics submodel for application within the MESSy framework (Modular Earth Submodel System). MADE3 builds on the predecessor aerosol submodels MADE and MADE-in. Its main new features are the explicit representation of coarse mode particle interactions both with other particles and with condensable gases, and the inclusion of hydrochloric acid (HCl) / chloride (Cl) partitioning between the gas and condensed phases. The aerosol size distribution is represented in the new submodel as a superposition of nine lognormal modes: one for fully soluble particles, one for insoluble particles, and one for mixed particles in each of three size ranges (Aitken, accumulation, and coarse mode size ranges). In order to assess the performance of MADE3 we compare it to its predecessor MADE and to the much more detailed particle-resolved aerosol model PartMC-MOSAIC in a box model simulation of an idealised marine boundary layer test case. MADE3 and MADE results are very similar, except in the coarse mode, where the aerosol is dominated by sea spray particles. Cl is reduced in MADE3 with respect to MADE due to the HCl / Cl partitioning that leads to Cl removal from the sea spray aerosol in our test case. Additionally, the aerosol nitrate concentration is higher in MADE3 due to the condensation of nitric acid on coarse mode particles. MADE3 and PartMC-MOSAIC show substantial differences in the fine particle size distributions (sizes ≲ 2 μm) that could be relevant when simulating climate effects on a global scale. Nevertheless, the agreement between MADE3 and PartMC-MOSAIC is very good when it comes to coarse particle size distributions (sizes ≳ 2 μm), and also in terms of aerosol composition. Considering these results and the well-established ability of MADE in reproducing observed aerosol loadings and composition, MADE3 seems suitable for application within a global model.

The goal of this study is to characterize the sensible (H) and latent (LE) heat exchange for different land covers in the heterogeneous steppe landscape of the Xilin River catchment, Inner Mongolia, China. Eddy-covariance flux measurements at 50–100 m above ground were conducted in July 2009 using a weight-shift microlight aircraft. Wavelet decomposition of the turbulence data enables a spatial discretization of 90 m of the flux measurements. For a total of 8446 flux observations during 12 flights, MODIS land surface temperature (LST) and enhanced vegetation index (EVI) in each flux footprint are determined. Boosted regression trees are then used to infer an environmental response function (ERF) between all flux observations (H, LE) and biophysical (LST, EVI) and meteorological drivers. Numerical tests show that ERF predictions covering the entire Xilin River catchment (&approx;3670 km2) are accurate to ≤18% (1 σ). The predictions are then summarized for each land cover type, providing individual estimates of source strength (36 W m−2 < H < 364 W m−2, 46 W m−2 < LE < 425 W m−2) and spatial variability (11 W m−2 < σH < 169 W m−2, 14 W m−2 < σLE < 152 W m−2) to a precision of ≤5%. Lastly, ERF predictions of land cover specific Bowen ratios are compared between subsequent flights at different locations in the Xilin River catchment. Agreement of the land cover specific Bowen ratios to within 12 &pm; 9% emphasizes the robustness of the presented approach. This study indicates the potential of ERFs for (i) extending airborne flux measurements to the catchment scale, (ii) assessing the spatial representativeness of long-term tower flux measurements, and (iii) designing, constraining and evaluating flux algorithms for remote sensing and numerical modelling applications.

The objective of this study is to assess the feasibility and quality of eddy-covariance flux measurements from a weight-shift microlight aircraft (WSMA). Firstly, we investigate the precision of the wind measurement (σu,v ≤ 0.09 m s−1, σw = 0.04 m s−1), the lynchpin of flux calculations from aircraft. From here, the smallest resolvable changes in friction velocity (0.02 m s−1), and sensible- (5 W m−2) and latent (3 W m−2) heat flux are estimated. Secondly, a seven-day flight campaign was performed near Lindenberg (Germany). Here we compare measurements of wind, temperature, humidity and respective fluxes between a tall tower and the WSMA. The maximum likelihood functional relationship (MLFR) between tower and WSMA measurements considers the random error in the data, and shows very good agreement of the scalar averages. The MLFRs for standard deviations (SDs, 2–34%) and fluxes (17–21%) indicate higher estimates of the airborne measurements compared to the tower. Considering the 99.5% confidence intervals, the observed differences are not significant, with exception of the temperature SD. The comparison with a large-aperture scintillometer reveals lower sensible heat flux estimates at both tower (−40 to −25%) and WSMA (−25–0%). We relate the observed differences to (i) inconsistencies in the temperature and wind measurement at the tower and (ii) the measurement platforms' differing abilities to capture contributions from non-propagating eddies. These findings encourage the use of WSMA as a low cost and highly versatile flux measurement platform.

Water activity is a key factor in aerosol thermodynamics and hygroscopic growth. We introduce a new representation of water activity (aw), which is empirically related to the solute molality (μs) through a single solute specific constant, νi. Our approach is widely applicable, considers the Kelvin effect and covers ideal solutions at high relative humidity (RH), including cloud condensation nuclei (CCN) activation. It also encompasses concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD). The constant νi can thus be used to parameterize the aerosol hygroscopic growth over a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. In contrast to other aw-representations, our νi factor corrects the solute molality both linearly and in exponent form x · ax. We present four representations of our basic aw-parameterization at different levels of complexity for different aw-ranges, e.g. up to 0.95, 0.98 or 1. νi is constant over the selected aw-range, and in its most comprehensive form, the parameterization describes the entire aw range (0–1). In this work we focus on single solute solutions. νi can be pre-determined with a root-finding method from our water activity representation using an aw−μs data pair, e.g. at solute saturation using RHD and solubility measurements. Our aw and supersaturation (Köhler-theory) results compare well with the thermodynamic reference model E-AIM for the key compounds NaCl and (NH4)2SO4 relevant for CCN modeling and calibration studies. Envisaged applications include regional and global atmospheric chemistry and climate modeling.

This study investigates whether the 3-D wind vector can be measured reliably from a highly transportable and low-cost weight-shift microlight aircraft. We draw up a transferable procedure to accommodate flow distortion originating from the aircraft body and -wing. This procedure consists of the analysis of aircraft dynamics and seven successive calibration steps. For our aircraft the horizontal wind components receive their greatest single amendment (14 %, relative to the initial uncertainty) from the correction of flow distortion magnitude in the dynamic pressure computation. Conversely the vertical wind component is most of all improved (31 %) by subsequent steps considering the 3-D flow distortion distribution in the flow angle computations. Therein the influences of the aircraft's trim (53 %), as well as changes in the aircraft lift (16 %) are considered by using the measured lift coefficient as explanatory variable. Three independent lines of analysis are used to evaluate the quality of the wind measurement: (a) A wind tunnel study in combination with the propagation of sensor uncertainties defines the systems input uncertainty to ≈0.6 m s−1 at the extremes of a 95 % confidence interval. (b) During severe vertical flight manoeuvres the deviation range of the vertical wind component does not exceed 0.3 m s−1. (c) The comparison with ground based wind measurements yields an overall operational uncertainty (root mean square error) of ≈0.4 m s−1 for the horizontal and ≈0.3 m s−1 for the vertical wind components. No conclusive dependence of the uncertainty on the wind magnitude (−1) or true airspeed (ranging from 23–30 m s−1) is found. Hence our analysis provides the necessary basis to study the wind measurement precision and spectral quality, which is prerequisite for reliable Eddy-Covariance flux measurements.

This study investigates whether the 3-D wind vector can be measured reliably from a highly transportable and low-cost weight-shift microlight aircraft. Therefore we draw up a transferable procedure to accommodate flow distortion originating from the aircraft body and -wing. This procedure consists of the analysis of aircraft dynamics and seven successive calibration steps. For our aircraft the horizontal wind components receive their greatest single amendment (14 %, relative to the initial uncertainty) from the correction of flow distortion magnitude in the dynamic pressure computation. Conversely the vertical wind component is most of all improved (31 %) by subsequent steps considering the 3-D flow distortion distribution in the flow angle computations. Therein the influences of the aircraft's trim (53 %), as well as changes in the aircraft lift (16 %) are considered by using the measured lift coefficient as explanatory variable. Three independent lines of analysis are used to evaluate the quality of the wind measurement: (a) A wind tunnel study in combination with the propagation of sensor uncertainties defines the systems input uncertainty to ≈0.6 m s−1 at the extremes of a 95 % confidence interval. (b) During severe vertical flight manoeuvres the deviation range of the vertical wind component does not exceed 0.3 m s−1. (c) The comparison with ground based wind measurements yields an overall operational uncertainty (root mean square error) of ≈0.4 m s−1 for the horizontal and ≈0.3 m s−1 for the vertical wind components. No conclusive dependence of the uncertainty on the wind magnitude (−1) or true airspeed (ranging from 23–30 m s−1) is found. Hence our analysis provides the necessary basis to study the wind measurement precision and spectral quality, which is prerequisite for reliable Eddy-Covariance flux measurements.

Eddy-covariance and Sodar/RASS experimental measurement data of the COPS (Convective and Orographically-induced Precipitation Study) field campaign 2007 are used to investigate the generation of near-ground free convection conditions (FCCs) in the Kinzig valley, Black Forest, Southwest Germany. The measured high-quality turbulent flux data revealed that FCCs are initiated near the ground in situations where moderate to high buoyancy fluxes and a simultaneously occurring drop of the wind speed were present. The minimum in wind speed – observable by the Sodar measurements through the whole vertical extension of the valley atmosphere – is the consequence of a thermally-induced valley wind system, which changes its wind direction from down to up-valley winds in the morning hours. Buoyancy then dominates over shear within the production of turbulence kinetic energy near the ground. These situations are detected by the stability parameter (ratio of the measurement height to the Obukhov length) when the level of free convection, which starts above the Obukhov length, drops below that of the sonic anemometer. An analysis of the scales of turbulent motions during FCCs using wavelet transform shows the occurrence of large-scale turbulence structures. Regarding the entire COPS measurement period, FCCs in the morning hours occur on about 50% of all days. Enhanced surface fluxes of latent and sensible heat are found on these days.

Modeling atmospheric aerosol and cloud microphysics is rather complex, even if chemical and thermodynamical equilibrium is assumed. We show, however, that the thermodynamics can be considerably simplified by reformulating equilibrium to consistently include water, and transform laboratory-based concepts to atmospheric conditions. We generalize the thermodynamic principles that explain hydration and osmosis – merely based on solute solubilities – to explicitly account for the water mass consumed by hydration. As a result, in chemical and thermodynamical equilibrium the relative humidity (RH) suffices to determine the saturation molality, including solute and solvent activities (and activity coefficients), since the water content is fixed by RH for a given aerosol concentration and type. As a consequence, gas/liquid/solid aerosol equilibrium partitioning can be solved analytically and non-iteratively. Our new concept enables an efficient and accurate calculation of the aerosol water mass and directly links the aerosol hygroscopic growth to fog, haze and cloud formation. We apply our new concept in the 3rd Equilibrium Simplified Aerosol Model (EQSAM3) for use in regional and global chemistry-transport and climate models. Its input is limited to the species' solubilities from which a newly introduced stoichiometric coefficient for water is derived. Analogously, we introduce effective stoichiometric coefficients for the solutes to account for complete or incomplete dissociation. We show that these coefficients can be assumed constant over the entire activity range and calculated for various inorganic, organic and non-electrolyte compounds, including alcohols, sugars and dissolved gases. EQSAM3 calculates the aerosol composition and gas/liquid/solid partitioning of mixed inorganic/organic multicomponent solutions and the associated water uptake for almost 100 major compounds. It explicitly accounts for particle hygroscopic growth by computing aerosol properties such as single solute molalities, molal based activities, including activity coefficients for volatile compounds, efflorescence and deliquescence relative humidities of single solute and mixed solutions. Various applications and a model inter-comparison indicate that a) the application is not limited to dilute binary solutions, b) sensitive aerosol properties such as hygroscopic growth and the pH of binary and mixed inorganic/organic salt solutions up to saturation can be computed accurately, and c) aerosol water is central in modeling atmospheric chemistry, visibility, weather and climate.

A thermodynamical model for treatment of gas/aerosol partitioning of semi volatile inorganic aerosols has been implemented in a global chemistry and aerosol transport model (Oslo CTM2). The sulphur cycle and sea salt particles have been implemented earlier in the Oslo CTM2 and the focus of this study is on nitrate partitioning to the aerosol phase and if particulate nitrate is expected to form in fine or coarse mode aerosols. Modelling of the formation of fine mode nitrate particles is complicated since it depends on other aerosol components and aerosol precursors as well as meteorological condition. The surface concentrations from the model are compared to observed surface concentrations at around 20 sites around Europe for nitrate and ammonium. The agreement for nitrate is good but the modelled values are somewhat underestimated compared to observations at high concentrations, whereas for ammonium the agreement is very good. However, we underscore that such a comparison is not of large importance for the aerosol optical depth of particulate nitrate since the vertical profile of aerosol components and their precursors are so important. Fine mode nitrate formation depends on vertical profiles of both ammonia/ammonium and sulphate. The model results show that fine mode particulate nitrate play a non-negligible role in the total aerosol composition in certain industrialized regions and therefore have a significant local radiative forcing. On a global scale the aerosol optical depth of fine mode nitrate is relatively small due to limited availability of ammonia and loss to larger sea salt particles. Inclusion of sea salt in the calculations reduces the aerosol optical depth and burden of fine mode nitrate by 25% on a global scale but with large regional variations.

The partitioning of reactive nitrogen compounds between the gas and the aerosol phase, as observed during the MINOS (Mediterranean INtensive Oxidant Study) campaign in Crete, Greece, in July and August 2001, has been studied with three thermodynamic gas-aerosol equilibrium models (EQMs) of different chemical complexity: ISORROPIA, which is limited to the ammonium-sulfate-nitrate-sodium-chloride-water-system; SCAPE2, which also includes mineral elements (calcium, magnesium and potassium); and EQSAM2, which additionally accounts for organic acids. The different EQMs are constrained by measured gas (g) and aerosol (a) concentrations: Total ammonia (NH3(g) and NH4(a)+), total nitrate (HNO3(g) and NO3(a)-), total sulfate (H2SO4(g) and SO4(a)2-), total chloride (HCl(g) and Cl-(a)), sodium (Na+(a)), calcium (Ca2+(a)), magnesium (Mg2+(a)), potassium (K+(a)) and organic acids (a). Although the three EQMs differ considerably in particular aspects, their application at the same level of complexity yields comparable results for the equilibrium composition and phase partitioning of ammonia and nitric acid, i.e. within the range of measurement uncertainties (~10%). Their application at different levels of complexity, however, gives rise to substantial differences for the gas-aerosol partitioning of reactive nitrogen compounds. Our results show that only if (soluble) mineral components and (lumped) organic acids are accounted for, the observed gas-aerosol partitioning of ammonia and nitric acid can be accurately reproduced for air pollution episodes characterized by a complex chemical mixture, typical for the Mediterranean lower atmosphere.

To elucidate human induced changes of aerosol load and composition in the atmosphere, a coupled aerosol and gas-phase chemistry transport model of the troposphere and lower stratosphere has been used. The present 3-D modeling study focuses on aerosol chemical composition change since preindustrial times considering the secondary organic aerosol formation together with all other main aerosol components including nitrate. In particular, we evaluate non-sea-salt sulfate (nss-SO4=), ammonium (NH4+), nitrate (NO3−), black carbon (BC), sea-salt, dust, primary and secondary organics (POA and SOA) with a focus on the importance of secondary organic aerosols. Our calculations show that the aerosol optical depth (AOD) has increased by about 21% since preindustrial times. This enhancement of AOD is attributed to a rise in the atmospheric load of BC, nss-SO4=, NO3, POA and SOA by factors of 3.3, 2.6, 2.7, 2.3 and 1.2, respectively, whereas we assumed that the natural dust and sea-salt sources remained constant. The nowadays increase in carbonaceous aerosol loading is dampened by a 34–42% faster conversion of hydrophobic to hydrophilic carbonaceous aerosol leading to higher removal rates. These changes between the various aerosol components resulted in significant modifications of the aerosol chemical composition. The relative importance of the various aerosol components is critical for the aerosol climatic effect, since atmospheric aerosols behave differently when their chemical composition changes. According to this study, the aerosol composition changed significantly over the different continents and with height since preindustrial times. The presence of anthropogenically emitted primary particles in the atmosphere facilitates the condensation of the semi-volatile species that form SOA onto the aerosol phase, particularly in the boundary layer. The SOA burden that is dominated by the natural component has increased by 24% while its contribution to the AOD has increased by 11%. The increase in oxidant levels and preexisting aerosol mass since preindustrial times is the reason of the burden change, since emissions have not changed significantly. The computed aerosol composition changes translate into about 2.5 times more water associated with non sea-salt aerosol. Additionally, aerosols contain 2.7 times more inorganic components nowadays than during the preindustrial times. We find that the increase in emissions of inorganic aerosol precursors is much larger than the corresponding aerosol increase, reflecting a non-linear atmospheric response.

The aerosol dynamics module MADE has been coupled to the general circulation model ECHAM4 to simulate the chemical composition, number concentration, and size distribution of the global submicrometer aerosol. The present publication describes the new model system ECHAM4/MADE and presents model results in comparison with observations. The new model is able to simulate the full life cycle of particulate matter and various gaseous particle precursors including emissions of primary particles and trace gases, advection, convection, diffusion, coagulation, condensation, nucleation of sulfuric acid vapor, aerosol chemistry, cloud processing, and size-dependent dry and wet deposition. Aerosol components considered are sulfate (SO4), ammonium (NH4), nitrate (NO3), black carbon (BC), particulate organic matter (POM), sea salt, mineral dust, and aerosol liquid water. The model is numerically efficient enough to allow long term simulations, which is an essential requirement for application in general circulation models. Since the current study is focusing on the submicrometer aerosol, a coarse mode is not being simulated. The model is run in a passive mode, i.e. no feedbacks between the MADE aerosols and clouds or radiation are considered yet. This allows the investigation of the effect of aerosol dynamics, not interfered by feedbacks of the altered aerosols on clouds, radiation, and on the model dynamics. In order to evaluate the results obtained with this new model system, calculated mass concentrations, particle number concentrations, and size distributions are compared to observations. The intercomparison shows, that ECHAM4/MADE is able to reproduce the major features of the geographical patterns, seasonal cycle, and vertical distributions of the basic aerosol parameters. In particular, the model performs well under polluted continental conditions in the northern hemispheric lower and middle troposphere. However, in comparatively clean remote areas, e.g. in the upper troposphere or in the southern hemispheric marine boundary layer, the current model version tends to underestimate particle number concentrations.

No abstract available.