ALBERT

Beschreibung: The diagnosis of the conservation state of monumental structures from constraints to the spatial distribution of their physical properties on shallow and inner materials represents one of the key objectives in the application of non-invasive techniques. In situ, CRP and 3D ultrasonic tomography can provide an effective coverage of stone materials in space and time. The intrinsic characteristics of the materials that make up a monumental structure and affect the two properties (i.e., reflectivity, longitudinal velocity) through the above methods substantially differ. Consequently, the content of their information is mainly complementary rather than redundant. In this study we present the integrated application of different non-destructive techniques i.e., Close Range Photogrammetry (CRP), and low frequency (24 KHz) ultrasonic tomography complemented by petrographycal analysis based essentially on Optical Microscopy (OM). This integrated methodology has been applied to a Carrara marble column of the Basilica of San Saturnino, in Byzantine-Proto-Romanesque style, which is part of the Paleo Christian complex of the V-VI century. This complex also includes the adjacent Christian necropolis in the square of San Cosimo in the city of Cagliari, Sardinia, Italy. The column under study is made of bare material dating back probably to the first century A.D., it was subjected to various traumas due to disassembly and transport to the site, including damage caused by the close blast of a WWII fragmentation bomb. High resolution 3D modelling of the studied artifact was computed starting from the integration of proximal sensing techniques such as CRP based on Structure from Motion (SfM), with which information about the geometrical anomalies and reflectivity of the investigated marble column surface was obtained. On the other hand, the inner parts of the studied body were successfully inspected in a non-invasive way by computing the velocity pattern of the ultrasonic signal through the investigated materials using 3D ultrasonic tomography. This technique gives information on the elastic properties of the material related with mechanical properties and a number of factors, such as presence of fractures, voids, and flaws. Extracting information on such factors from the elastic wave velocity using 3D tomography provides a non-invasive approach to analyse the property changes of the inner material of the ancient column. The integrated application of in situ CRP and ultrasonic techniques provides a full 3D high resolution model of the investigated artifact. This model enhanced by the knowledge of the petrographic characteristics of the materials, improves the diagnostic process and affords reliable information on the state of conservation of the materials used in the construction processes of the studied monumental structure. The integrated use of the non-destructive techniques described above also provides suitable data for a possible restoration and future preservation.

Beschreibung: Copernicus

Beschreibung: Published

Beschreibung: On line

Beschreibung: 5T. Sismologia, geofisica e geologia per l'ingegneria sismica

Beschreibung: Originating from the boreal forest and often transported over large distances, driftwood characterises many Arctic coastlines. Here we present a combined assessment of radiocarbon (14C) and dendrochronological (ring width) age estimates of driftwood samples to constrain the progradation of two Holocene beach-ridge systems near the Lena Delta in the Siberian Arctic (Laptev Sea). Our data show that the 14C ages obtained on syndepositional driftwood from beach deposits yield surprisingly coherent chronologies for the coastal evolution of the field sites. The dendrochronological analysis of wood from modern driftlines revealed the origin and recent delivery of the wood from the Lena River catchments. This finding suggests that the duration transport lies within the uncertainty of state-of-the-art 14C dating and thus substantiates the validity of age indication obtained from driftwood. This observation will help to better understand changes in similar coastal environments, and to improve our knowledge about the response of coastal systems to past climate and sea-level changes.

Beschreibung: Earth system and climate modelling involves the simulation of processes on a wide range of scales and within and across various compartments of the Earth system. In practice, component models are often developed independently by different research groups, adapted by others to their special interests and then combined using a dedicated coupling software. This procedure not only leads to a strongly growing number of available versions of model components and coupled setups but also to model- and high-performance computing (HPC)-system-dependent ways of obtaining, configuring, building and operating them. Therefore, implementing these Earth system models (ESMs) can be challenging and extremely time consuming, especially for less experienced modellers or scientists aiming to use different ESMs as in the case of intercomparison projects. To assist researchers and modellers by reducing avoidable complexity, we developed the ESM-Tools software, which provides a standard way for downloading, configuring, compiling, running and monitoring different models on a variety of HPC systems. It should be noted that ESM-Tools is not a coupling software itself but a workflow and infrastructure management tool to provide access to increase usability of already existing components and coupled setups. As coupled ESMs are technically the more challenging tasks, we will focus on coupled setups, always implying that stand-alone models can benefit in the same way. With ESM-Tools, the user is only required to provide a short script consisting of only the experiment-specific definitions, while the software executes all the phases of a simulation in the correct order. The software, which is well documented and easy to install and use, currently supports four ocean models, three atmosphere models, two biogeochemistry models, an ice sheet model, an isostatic adjustment model, a hydrology model and a land-surface model. Compared to previous versions, ESM-Tools has lately been entirely recoded in a high-level programming language (Python) and provides researchers with an even more user-friendly interface for Earth system modelling. ESM-Tools was developed within the framework of the Advanced Earth System Model Capacity project, supported by the Helmholtz Association.

Beschreibung: Numerous studies have addressed the possible existence of large floating ice sheets in the glacial Arctic Ocean from theoretical, modelling, or seafloor morphology perspectives. Here, we add evidence from the sediment record that support the existence of such freshwater ice caps in certain intervals, and we discuss their implications for possible non-linear and rapid behaviour of such a system in the high latitudes. We present sedimentary activities of 230Th together with 234U/238U ratios, the concentrations of manganese, sulphur and calcium in the context of lithological information and records of microfossils and their isotope composition. New analyses (PS51/038, PS72/396) and a re-analysis of existing marine sediment records (PS1533, PS1235, PS2185, PS2200, amongst others) in view of the naturally occurring radionuclide 230Thex and, where available, 10Be from the Arctic Ocean and the Nordic Seas reveal the widespread occurrence of intervals with a specific geochemical signature. The pattern of these parameters in a pan-Arctic view can best be explained when assuming the repeated presence of freshwater in frozen and liquid form across large parts of the Arctic Ocean and the Nordic Seas. Based on the sedimentary evidence and known environmental constraints at the time, we develop a glacial scenario that explains how these ice sheets, together with eustatic sea-level changes, may have affected the past oceanography of the Arctic Ocean in a fundamental way that must have led to a drastic and non-linear response to external forcing. This concept offers a possibility to explain and to some extent reconcile contrasting age models for the Late Pleistocene in the Arctic Ocean. Our view, if adopted, offers a coherent dating approach across the Arctic Ocean and the Nordic Seas, linked to events outside the Arctic.

Beschreibung: The modeling of paleoclimate, using physically based tools, is increasingly seen as a strong out-of-sample test of the models that are used for the projection of future climate changes. New to the Coupled Model Intercomparison Project (CMIP6) is the Tier 1 Last Interglacial experiment for 127 000 years ago (lig127k), designed to address the climate responses to stronger orbital forcing than the midHolocene experiment, using the same state-of-the-art models as for the future and following a common experimental protocol. Here we present a first analysis of a multi-model ensemble of 17 climate models, all of which have completed the CMIP6 DECK (Diagnostic, Evaluation and Characterization of Klima) experiments. The equilibrium climate sensitivity (ECS) of these models varies from 1.8 to 5.6 ∘C. The seasonal character of the insolation anomalies results in strong summer warming over the Northern Hemisphere continents in the lig127k ensemble as compared to the CMIP6 piControl and much-reduced minimum sea ice in the Arctic. The multi-model results indicate enhanced summer monsoonal precipitation in the Northern Hemisphere and reductions in the Southern Hemisphere. These responses are greater in the lig127k than the CMIP6 midHolocene simulations as expected from the larger insolation anomalies at 127 than 6 ka. New synthesis for surface temperature and precipitation, targeted for 127 ka, have been developed for comparison to the multi-model ensemble. The lig127k model ensemble and data reconstructions are in good agreement for summer temperature anomalies over Canada, Scandinavia, and the North Atlantic and for precipitation over the Northern Hemisphere continents. The model–data comparisons and mismatches point to further study of the sensitivity of the simulations to uncertainties in the boundary conditions and of the uncertainties and sparse coverage in current proxy reconstructions. The CMIP6–Paleoclimate Modeling Intercomparison Project (PMIP4) lig127k simulations, in combination with the proxy record, improve our confidence in future projections of monsoons, surface temperature, and Arctic sea ice, thus providing a key target for model evaluation and optimization.

Beschreibung: In order to investigate the impact of spatial resolution on the discrepancy between simulated δ18O and observed δ18O in Greenland ice cores, regional climate simulations are performed with the isotope-enabled regional climate model (RCM) COSMO_iso. For this purpose, isotope-enabled general circulation model (GCM) simulations with the ECHAM5-wiso general circulation model (GCM) under present-day conditions and the MPI-ESM-wiso GCM under mid-Holocene conditions are dynamically downscaled with COSMO_iso for the Arctic region. The capability of COSMO_iso to reproduce observed isotopic ratios in Greenland ice cores for these two periods is investigated by comparing the simulation results to measured δ18O ratios from snow pit samples, Global Network of Isotopes in Precipitation (GNIP) stations and ice cores. To our knowledge, this is the first time that a mid-Holocene isotope-enabled RCM simulation is performed for the Arctic region. Under present-day conditions, a dynamical downscaling of ECHAM5-wiso (1.1◦ × 1.1◦) with COSMO_iso to a spatial resolution of 50km improves the agreement with the measured δ18O ratios for 14 of 19 observational data sets. A further increase in the spatial resolution to 7km does not yield substantial improvements except for the coastal areas with its complex terrain. For the mid-Holocene, a fully coupled MPI-ESM-wiso time slice simulation is downscaled with COSMO_iso to a spatial resolution of 50km. In the mid-Holocene, MPI-ESM-wiso already agrees well with observations in Greenland and a downscaling with COSMO_iso does not further improve the model–data agreement. Despite this lack of improvement in model biases, the study shows that in both periods, observed δ18O values at measurement sites constitute isotope ratios which are mainly within the subgrid-scale variability of the global ECHAM5-wiso and MPI-ESM-wiso simulation results. The correct δ18O ratios are consequently not resolved in the GCM simulation results and need to be extracted by a refinement with an RCM. In this context, the RCM simulations provide a spatial δ18O distribution by which the effects of local uncertainties can be taken into account in the comparison between point measurements and model outputs. Thus, an isotope-enabled GCM–RCM model chain with realistically implemented fractionating processes constitutes a useful supplement to reconstruct regional paleo-climate conditions during the mid-Holocene in Greenland. Such model chains might also be applied to reveal the full potential of GCMs in other regions and climate periods, in which large deviations relative to observed isotope ratios are simulated.

Beschreibung: Proxy climate records are an invaluable source of information about the earth’s climate prior to the instrumental record. The temporal- and spatial-coverage of records continues to increase, however, these records of past climate are associated with significant uncertainties due to non-climate processes that influence the recorded and measured proxy values. Generally, these uncertainties are timescale-dependent and correlated in time. Accounting for structure in the errors is essential to providing realistic error estimates for smoothed or stacked records, detection of anomalies and identifying trends, but this structure is seldom accounted for. In the first of these companion articles we outlined a theoretical framework for handling proxy uncertainties by deriving the power spectrum of proxy error components from which it is possible to obtain timescale-dependent error estimates. Here in part II, we demonstrate the practical application of this theoretical framework using the example of marine sediment cores. We consider how to obtain estimates for the required parameters and give examples of the application of this approach for typical marine sediment proxy records. Our new approach of estimating and providing timescale-dependent proxy errors overcomes the limitations of simplistic single value error estimates. We aim to provide the conceptual basis for a more quantitative use of paleo-records for applications such as model-data comparison, regional and global synthesis of past climate states and data assimilation.

Beschreibung: The mid-Pliocene warm period (mPWP; ∼3.2 million years ago) is seen as the most recent time period characterized by a warm climate state, with similar to modern geography and ∼400 ppmv atmospheric CO2 concentration, and is therefore often considered an interesting analogue for near-future climate projections. Paleoenvironmental reconstructions indicate higher surface temperatures, decreasing tropical deserts, and a more humid climate in West Africa characterized by a strengthened West African Monsoon (WAM). Using model results from the second phase of the Pliocene Modelling Intercomparison Project (PlioMIP2) ensemble, we analyse changes of the WAM rainfall during the mPWP by comparing them with the control simulations for the pre-industrial period. The ensemble shows a robust increase in the summer rainfall over West Africa and the Sahara region, with an average increase of 2.5 mm/d, contrasted by a rainfall decrease over the equatorial Atlantic. An anomalous warming of the Sahara and deepening of the Saharan Heat Low, seen in 〉90 % of the models, leads to a strengthening of the WAM and an increased monsoonal flow into the continent. A similar warming of the Sahara is seen in future projections using both phase 3 and 5 of the Coupled Model Intercomparison Project (CMIP3 and CMIP5). Though previous studies of future projections indicate a west–east drying–wetting contrast over the Sahel, PlioMIP2 simulations indicate a uniform rainfall increase in that region in warm climates characterized by increasing greenhouse gas forcing. We note that this effect will further depend on the long-term response of the vegetation to the CO2 forcing.

Beschreibung: Due to its dryness, the subtropical free troposphere plays a critical role in the radiative balance of the Earth's climate system. But the complex interactions of the dynamical and physical processes controlling the variability in the moisture budget of this sensitive region of the subtropical atmosphere are still not fully understood. Stable water isotopes can provide important information about several of the latter processes, namely subsidence drying, turbulent mixing, and dry and moist convective moistening. In this study, we use high-resolution simulations of the isotope-enabled version of the regional weather and climate prediction model of the Consortium for Small-Scale Modelling (COSMOiso) to investigate predominant moisture transport pathways in the Canary Islands region in the eastern subtropical North Atlantic. Comparison of the simulated isotope signals with multi-platform isotope observations (aircraft, ground- and space-based remote sensing) from a field campaign in summer 2013 shows that COSMOiso can reproduce the observed variability of stable water vapour isotopes on timescales of hours to days, thus allowing us to study the mechanisms that control the subtropical free-tropospheric humidity. Changes in isotopic signals along backward trajectories from the Canary Islands region reveal the physical processes behind the synoptic-scale isotope variability. We identify four predominant moisture transport pathways of mid-tropospheric air, each with distinct isotopic signatures: - air parcels originating from the convective boundary layer of the Saharan heat low (SHL) – these are characterised by a homogeneous isotopic composition with a particularly high δD (median mid-tropospheric δD=−122‰), which results from dry convective mixing of low-level moisture of diverse origin advected into the SHL; - air parcels originating from the free troposphere above the SHL – although experiencing the largest changes in humidity and δD during their subsidence over West Africa, these air parcels typically have lower δD values (median δD=−148‰) than air parcels originating from the boundary layer of the SHL; - air parcels originating from outside the SHL region, typically descending from tropical upper levels south of the SHL, which are often affected by moist convective injections from mesoscale convective systems in the Sahel – their isotopic composition is much less enriched in heavy isotopes (median δD=−175‰) than those from the SHL region; - air parcels subsiding from the upper-level extratropical North Atlantic – this pathway leads to the driest and most depleted conditions (median δD=−255‰) in the middle troposphere near the Canary Islands. The alternation of these transport pathways explains the observed high variability in humidity and δD on synoptic timescales to a large degree. We further show that the four different transport pathways are related to specific large-scale flow conditions. In particular, distinct differences in the location of the North African mid-level anticyclone and of extratropical Rossby wave patterns occur between the four transport pathways. Overall, this study demonstrates that the adopted Lagrangian isotope perspective enhances our understanding of air mass transport and mixing and offers a sound interpretation of the free-tropospheric variability of specific humidity and isotope composition on timescales of hours to days in contrasting atmospheric conditions over the eastern subtropical North Atlantic.

Beschreibung: Hyrrokkin sarcophaga is a parasitic foraminifera that is commonly found in cold-water coral reefs where it infests the file clam Acesta excavata and the scleractinian coral Desmophyllum pertusum (formerly known as Lophelia pertusa). Here, we present measurements of the trace element and isotopic composition of these parasitic foraminifera, analyzed by inductively coupled optical emission spectrometry (ICP-OES), electron probe microanalysis (EPMA) and mass spectrometry (gas-source MS and inductively-coupled-plasma MS). Our results reveal that the geochemical signature of H. sarcophaga depends on the host organism it infests. Sr / Ca ratios are 1.1 mmol mol−1 higher in H. sarcophaga that infest D. pertusum, which could be an indication that dissolved host carbonate material is utilized in shell calcification, given that the aragonite of D. pertusum has a naturally higher Sr concentration compared to the calcite of A. excavata. Similarly, we measure 3.1 ‰ lower δ13C and 0.25 ‰ lower δ18O values in H. sarcophaga that lived on D. pertusum, which might be caused by the direct uptake of the host's carbonate material with a more negative isotopic composition or different pH regimes in these foraminifera (pH can exert a control on the extent of CO2 hydration/hydroxylation) due to the uptake of body fluids of the host. We also observe higher Mn / Ca ratios in foraminifera that lived on A. excavata but did not penetrate the host shell compared to specimen that penetrated the shell, which could be interpreted as a change in food source, changes in the calcification rate, Rayleigh fractionation or changing oxygen conditions. While our measurements provide an interesting insight into the calcification process of this unusual foraminifera, these data also indicate that the geochemistry of this parasitic foraminifera is unlikely to be a reliable indicator of paleoenvironmental conditions using Sr / Ca, Mn / Ca, δ18O or δ13C unless the host organism is known and its geochemical composition can be accounted for.

Beschreibung: In this work we have performed a detailed study of vectors to ore to a representative volcanic-rock-hosted replacive volcanogenic massive sulfide (VMS) deposit located in the northern Iberian Pyrite Belt (Spain), the Aguas Teñidas deposit. The investigated vectors include the following: (1) mineralogical zoning, (2) host sequence characterization and mineralized unit identification based on whole rock geochemistry discrimination diagrams, (3) study of the characteristics and behaviour of whole rock geochemical anomalies around the ore (e.g. alteration-related compositional changes, characteristics and extent of geochemical halos of indicative elements such as Cu, Zn, Pb, Sb, Tl, and Ba around the deposit), and (4) application of portable X-ray fluorescence (p-XRF) analysis to the detection of the previous vectors. In the footwall, a concentric cone-shaped hydrothermal alteration zone bearing the stockwork passes laterally, from core to edge, from quartz (only local) to chlorite–quartz, sericite–chlorite–quartz, and sericite–quartz alteration zones. The hydrothermal alteration is also found in the hanging wall despite being tectonically allochthonous to the orebody: a proximal sericite alteration zone is followed by a more distal albite-rich one. Whole rock major elements show an increase in alteration indexes (e.g. AI, CCPI) towards the mineralization, a general SiO2 enrichment, and FeO enrichment as well as K2O and Na2O depletion towards the centre of the hydrothermal system, with MgO showing a less systematic behaviour. K2O and Na2O leached from the centre of the system are transported and deposited in more external areas. Copper, Pb, and Zn produce proximal anomalies around mineralized areas, with the more mobile Sb, Tl, and Ba generating wider halos. Whereas Sb and Tl halos form around all mineralized areas, Ba anomalies are restricted to areas around the massive sulfide body. Our results show that proposed vectors, or adaptations designed to overcome p-XRF limitations, can be confidently used by analysing unprepared hand specimens, including the external rough curved surface of drill cores. The data presented in this work are not only applicable to VMS exploration in the Iberian Pyrite Belt, but on a broader scale they will also contribute to improving our general understanding of vectors to ore in replacive-type VMS deposits.

Beschreibung: We combine satellite data products to provide a first and general overview of the physical sea ice conditions along the drift of the international Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) expedition and a comparison with previous years (2005–2006 to 2018–2019). We find that the MOSAiC drift was around 20 % faster than the climatological mean drift, as a consequence of large-scale low-pressure anomalies prevailing around the Barents–Kara–Laptev sea region between January and March. In winter (October–April), satellite observations show that the sea ice in the vicinity of the Central Observatory (CO; 50 km radius) was rather thin compared to the previous years along the same trajectory. Unlike ice thickness, satellite-derived sea ice concentration, lead frequency and snow thickness during winter months were close to the long-term mean with little variability. With the onset of spring and decreasing distance to the Fram Strait, variability in ice concentration and lead activity increased. In addition, the frequency and strength of deformation events (divergence, convergence and shear) were higher during summer than during winter. Overall, we find that sea ice conditions observed within 5 km distance of the CO are representative for the wider (50 and 100 km) surroundings. An exception is the ice thickness; here we find that sea ice within 50 km radius of the CO was thinner than sea ice within a 100 km radius by a small but consistent factor (4 %) for successive monthly averages. Moreover, satellite acquisitions indicate that the formation of large melt ponds began earlier on the MOSAiC floe than on neighbouring floes.

Beschreibung: Across the Qinghai–Tibet Plateau (QTP) there is a narrow engineering corridor with widely distributed slopes called the Qinghai–Tibet Engineering Corridor (QTEC), where a variety of important infrastructures are concentrated. These facilities are transportation routes for people, materials, energy, etc. from inland China to the Tibet Autonomous Region. From Golmud to Lhasa, the engineering corridor covers 632 km of permafrost containing the densely developed Qinghai–Tibet Railway and Qinghai–Tibet Highway, as well as power and communication towers. Slope failure in permafrost regions, caused by permafrost degradation, ground ice melting, etc., affects the engineering construction and permafrost environments in the QTEC. We implement a variety of sensors to monitor the hydrological and thermal deformation between permafrost slopes and permafrost engineering projects in the corridor. In addition to soil temperature and moisture sensors, the global navigation satellite system (GNSS), terrestrial laser scanning (TLS), and unmanned aerial vehicles (UAVs) were adopted to monitor the spatial distribution and changes in thermal deformation. An integrated dataset of hydrological and thermal deformation in permafrost engineering and slopes in the QTEC from the 1950s to 2020, including meteorological and ground observations, TLS point cloud data, and RGB and thermal infrared (TIR) images, can be of great value for estimating the hydrological and thermal impact and stability between engineering and slopes under the influence of climate change and engineering disturbance. The dataset and code were uploaded to the Zenodo repository and can be accessed through https://zenodo.org/communities/qtec (last access: 23 June 2021), including meteorological and ground observations at https://doi.org/10.5281/zenodo.5009871 (Luo et al., 2020d), TLS measurements at https://doi.org/10.5281/zenodo.5009558 (Luo et al., 2020a), UAV RGB and TIR images at https://doi.org/10.5281/zenodo.5016192 (Luo et al., 2020b), and R code for permafrost indices and visualisation at https://doi.org/10.5281/zenodo.5002981 (Luo et al., 2020c).

Beschreibung: We present the first incorporation of the Common Representative Intermediates version 2.2 tropospheric chemistry mechanism, CRI v2.2, combined with stratospheric chemistry, into the global chemistry–climate United Kingdom Chemistry and Aerosols (UKCA) model to give the CRI-Strat 2 mechanism. A rigorous comparison of CRI-Strat 2 with the earlier version, CRI-Strat, is performed in UKCA in addition to an evaluation of three mechanisms, CRI-Strat 2, CRI-Strat and the standard UKCA chemical mechanism, StratTrop v1.0, against a wide array of surface and airborne chemical data. CRI-Strat 2 comprises a state-of-the-art isoprene scheme, optimized against the Master Chemical Mechanism v3.3.1, which includes isoprene peroxy radical isomerization, HOx recycling through the addition of photolabile hydroperoxy aldehydes (HPALDs), and isoprene epoxy diol (IEPOX) formation. CRI-Strat 2 also features updates to several rate constants for the inorganic chemistry, including the reactions of inorganic nitrogen and O(1D). The update to the isoprene chemistry in CRI-Strat 2 increases OH over the lowest 500 m in tropical forested regions by 30 %–50 % relative to CRI-Strat, leading to an improvement in model–observation comparisons for surface OH and isoprene relative to CRI-Strat and StratTrop. Enhanced oxidants also cause a 25 % reduction in isoprene burden and an increase in oxidation fluxes of isoprene and other biogenic volatile organic compounds (BVOCs) at low altitudes with likely impacts on subsequent aerosol formation, atmospheric lifetime, and climate. By contrast, updates to the rate constants of O(1D) with its main reactants relative to CRI-Strat reduces OH in much of the free troposphere, producing a 2 % increase in the methane lifetime, and increases the tropospheric ozone burden by 8 %, primarily from reduced loss via O(1D)+H2O. The changes to inorganic nitrogen reaction rate constants increase the NOx burden by 4 % and shift the distribution of nitrated species closer to that simulated by StratTrop. CRI-Strat 2 is suitable for multi-decadal model integrations and the improved representation of isoprene chemistry provides an opportunity to explore the consequences of HOx recycling in the United Kingdom Earth System Model (UKESM1). This new mechanism will enable a re-evaluation of the impact of BVOCs on the chemical composition of the atmosphere and further probe the feedback between the biosphere and the climate.

Beschreibung: The use of mass flow simulations in volcanic hazard zonation and mapping is often limited by model complexity (i.e. uncertainty in correct values of model parameters), a lack of model uncertainty quantification, and limited approaches to incorporate this uncertainty into hazard maps. When quantified, mass flow simulation errors are typically evaluated on a pixel-pair basis, using the difference between simulated and observed (“actual”) map-cell values to evaluate the performance of a model. However, these comparisons conflate location and quantification errors, neglecting possible spatial autocorrelation of evaluated errors. As a result, model performance assessments typically yield moderate accuracy values. In this paper, similarly moderate accuracy values were found in a performance assessment of three depth-averaged numerical models using the 2012 debris avalanche from the Upper Te Maari crater, Tongariro Volcano, as a benchmark. To provide a fairer assessment of performance and evaluate spatial covariance of errors, we use a fuzzy set approach to indicate the proximity of similarly valued map cells. This “fuzzification” of simulated results yields improvements in targeted performance metrics relative to a length scale parameter at the expense of decreases in opposing metrics (e.g. fewer false negatives result in more false positives) and a reduction in resolution. The use of this approach to generate hazard zones incorporating the identified uncertainty and associated trade-offs is demonstrated and indicates a potential use for informed stakeholders by reducing the complexity of uncertainty estimation and supporting decision-making from simulated data.

Beschreibung: In this study, we analyse the climatology of ionosphere over Nepal based on GPS-derived vertical total electron content (VTEC) observed from four stations as defined in Table 1: KKN4 (27.80∘ N, 85.27∘ E), GRHI (27.95∘ N, 82.49∘ E), JMSM (28.80∘ N, 83.74∘ E) and DLPA (28.98∘ N, 82.81∘ E) during the years 2008 to 2018. The study illustrates the diurnal, monthly, annual, seasonal and solar cycle variations in VTEC during all times of solar cycle 24. The results clearly reveal the presence of equinoctial asymmetry in TEC, which is more pronounced in maximum phases of solar cycle in the year 2014 at KKN4 station, followed by descending, ascending and minimum phases. Diurnal variations in VTEC showed the short-lived day minimum which occurs between 05:00 to 06:00 LT (local time) at all the stations considered, with diurnal peaks between 12:00 and 15:00 LT. The maximum value of TEC is observed more often during the spring equinox than the autumn equinox, with a few asymmetries. Seasonal variation in TEC is observed to be a manifestation of variations in solar flux, particularly regarding the level of solar flux in consecutive solstices.

Beschreibung: We report on applications of the ultraviolet-light-emitting-diode-based incoherent broadband cavity-enhanced absorption spectroscopy (UV-LED-IBBCEAS) technique for optical monitoring of HONO, NO2 and CH2O in a simulation chamber. Performance intercomparison of UV-LED-IBBCEAS with a wet chemistry-based NitroMAC sensor and a Fourier transform infrared (FTIR) spectrometer has been carried out on real-time simultaneous measurement of HONO, NO2 and CH2O concentrations during the reaction of NO2 with H2O vapour in CESAM (French acronym for Experimental Multiphasic Atmospheric Simulation Chamber). The 1σ (signal-to-noise ratio (SNR) = 1) detection limits of 112 pptv for NO2, 56 pptv for HONO and 41 ppbv for CH2O over 120 s were found for the UV-LED-IBBCEAS measurement. On the contrary to many set-ups where cavities are installed outside the simulation chamber, we describe here an original in situ permanent installation. The intercomparison results demonstrate that IBBCEAS is a very well suitable technique for in situ simultaneous measurements of multiple chemically reactive species with high sensitivity and high precision even if the absorption bands of these species are overlapped. It offers excellent capacity for non-invasive optical monitoring of chemical reactions without any perturbation. For the application to simulation chambers, it has the advantage to provide a spatially integrated measurement across the reactor and hence to avoid point-sampling-related artefacts.

Beschreibung: Assimilation of weather radar measurements including radar reflectivity and radial wind data has been operational at the Deutscher Wetterdienst, with a diagonal observation error (OE) covariance matrix. For an implementation of a full OE covariance matrix, the statistics of the OE have to be a priori estimated, for which the Desroziers method has been often used. However, the resulted statistics consists of contributions from different error sources and are difficult to interpret. In this work, we use an approach that is based on samples for truncation error in radar observation space to approximate the representation error due to unresolved scales and processes (RE) and compare its statistics with the OE statistics estimated by the Desroziers method. It is found that the statistics of the RE help the understanding of several important features in the variances and correlation length scales of the OE for both reflectivity and radial wind data and the other error sources from the microphysical scheme, radar observation operator and the superobbing technique may also contribute, for instance, to differences among different elevations and observation types. The statistics presented here can serve as a guideline for selecting which observations are assimilated and for assignment of the OE covariance matrix that can be diagonal or full and correlated.

Beschreibung: Determining controls on the temperature sensitivity of heterotrophic soil respiration remains critical to incorporating soil–climate feedbacks into climate models. Most information on soil respiratory responses to temperature comes from laboratory incubations of isolated soils and typically subsamples of individual horizons. Inconsistencies between field and laboratory results may be explained by microbial priming supported by cross-horizon exchange of labile C or N. Such exchange is feasible in intact soil profiles but is absent when soils are isolated from surrounding depths. Here we assess the role of soil horizon connectivity, by which we mean the degree to which horizons remain layered and associated with each other as they are in situ, on microbial C and N substrate use and its relationship to the temperature sensitivity of respiration. We accomplished this by exploring changes in C : N, soil organic matter composition (via C : N, amino acid composition and concentration, and nuclear magnetic resonance spectroscopy), and the δ13C of respiratory CO2 during incubations of organic horizons collected across boreal forests in different climate regions where soil C and N compositions differ. The experiments consisted of two treatments: soil incubated (1) with each organic horizon separately and (2) as a whole organic profile, permitting cross-horizon exchange of substrates during the incubation. The soils were incubated at 5 and 15 ∘C for over 430 d. Enhanced microbial use of labile C-rich, but not N-rich, substrates were responsible for enhanced, whole-horizon respiratory responses to temperature relative to individual soil horizons. This impact of a labile C priming mechanism was most emergent in soils from the warmer region, consistent with these soils' lower C bioreactivity relative to soils from the colder region. Specifically, cross-horizon exchange within whole soil profiles prompted increases in mineralization of carbohydrates and more 13C-enriched substrates and increased soil respiratory responses to warming relative to soil horizons incubated in isolation. These findings highlight that soil horizon connectivity can impact microbial substrate use in ways that affect how soil effluxes of CO2 are controlled by temperature. The degree to which this mechanism exerts itself in other soils remains unknown, but these results highlight the importance of understanding mechanisms that operate in intact soil profiles – only rarely studied – in regulating a key soil–climate feedback.

Beschreibung: Plumes from the boreal spring biomass burning (BB) in northern peninsular Southeast Asia (nPSEA) are lifted into the subtropical jet stream and transported and deposited across nPSEA, South China, Taiwan and even the western North Pacific Ocean. This paper as part of the Seven SouthEast Asian Studies (7-SEAS) project effort attempts to improve the chemical weather prediction capability of the Weather Research and Forecasting coupled with the Community Multiscale for Air Quality (WRF–CMAQ) model over a vast region, from the mountainous near-source burning sites at nPSEA to its downwind region. Several sensitivity analyses of plume rise are compared in the paper, and it is discovered that the initial vertical allocation profile of BB plumes and the plume rise module (PLMRIM) are the main reasons causing the inaccuracies of the WRF–CMAQ simulations. The smoldering emission from the Western Regional Air Partnership (WRAP) empirical algorithm included has improved the accuracies of PM10, O3 and CO at the source. The best performance at the downwind sites is achieved with the inline PLMRIM, which accounts for the atmospheric stratification at the mountainous source region with the FINN burning emission dataset. Such a setup greatly improves not only the BB aerosol concentration prediction over near-source and receptor ground-based measurement sites but also the aerosol vertical distribution and column aerosol optical depth of the BB aerosol along the transport route. The BB aerosols from nPSEA are carried by the subtropical westerlies in the free troposphere to the western North Pacific, while BB aerosol has been found to interact with the local pollutants in the Taiwan region through three conditions: (a) overpassing western Taiwan and entering the central mountain area, (b) mixing down to western Taiwan, (c) transport of local pollutants upwards and mixing with a BB plume on higher ground. The second condition, which involves the prevailing high-pressure system from Asian cold surge, is able to impact most of the population in Taiwan.

Beschreibung: The German Bight located within the central North Sea is a hydro- and morphodynamically highly complex system of estuaries, barrier islands, and part of the world's largest coherent tidal flats, the Wadden Sea. To identify and understand challenges faced by coastal stakeholders, such as harbor operators or governmental agencies, to maintain waterways and employ numerical models for further analyses, it is imperative to have a consistent database for both bathymetry and surface sedimentology. Current commercial and public data products are insufficient in spatial and temporal resolution and coverage for recent analysis methods. Thus, this first part of a two-part publication series of the German joint project EasyGSH-DB describes annual bathymetric digital terrain models at a 10 m gridded resolution for the German North Sea coast and German Bight from 1996 to 2016 (Sievers et al., 2020a, https://doi.org/10.48437/02.2020.K2.7000.0001), as well as surface sedimentological models of discretized cumulative grain size distribution functions for 1996, 2006, and 2016 on 100 m grids (Sievers et al., 2020b, https://doi.org/10.48437/02.2020.K2.7000.0005). Furthermore, basic morphodynamic and sedimentological processing analyses, such as the estimation of, for example, bathymetric stability or surface maps of sedimentological parameters, are provided (Sievers et al., 2020a, b, see respective download links).

Beschreibung: The Phanerozoic tectonothermal evolution of the SW slope of the East European Platform (EEP) in Poland is reconstructed by means of thermal maturity, low-temperature thermochronometry, and thermal modelling. We provide a set of new thermochronometric data and integrate stratigraphic and thermal maturity information to constrain the burial and thermal history of sediments. Apatite fission track (AFT) analysis and zircon (U-Th)/He (ZHe) thermochronology have been carried out on samples of sandstones, bentonites, diabase, and crystalline basement rocks collected from 17 boreholes located in central and NE Poland. They penetrated sedimentary cover of the EEP subdivided from the north to south into the Baltic, Podlasie, and Lublin basins. The average ZHe ages from Proterozoic basement rocks as well as Ordovician to Silurian bentonites and Cambrian to lower Carboniferous sandstones range from 848 ± 81 to 255 ± 22 Ma with a single early Permian age of 288 Ma, corresponding to cooling after a thermal event. The remaining ZHe ages represent partial reset or source ages. The AFT ages of samples are dispersed in the range of 235.8 ± 17.3 Ma (Middle Triassic) to 42.1 ± 11.1 Ma (Paleogene) providing a record of Mesozoic and Cenozoic cooling. The highest frequency of the AFT ages is in the Jurassic and Early Cretaceous prior to Alpine basin inversion. Thermal maturity results are consistent with the SW-ward increase of the Paleozoic and Mesozoic sediments thickness. An important break in a thermal maturity profile exists across the base Permian–Mesozoic unconformity. Thermal modelling showed that significant heating of Ediacaran to Carboniferous sedimentary successions occurred before the Permian with maximum paleotemperatures in the earliest and latest Carboniferous for Baltic–Podlasie and Lublin basins, respectively. The results obtained suggest an important role of early Carboniferous uplift and exhumation at the SW margin of the EEP. The SW slope of the latter was afterward overridden in the Lublin Basin by the Variscan orogenic wedge. Its tectonic loading interrupted Carboniferous uplift and caused resumption of sedimentation in the late Viséan. Consequently, a thermal history of the Lublin Basin is different from that in the Podlasie and Baltic basins but similar to other sections of the Variscan foreland, characterized by maximum burial at the end of Carboniferous. The Mesozoic thermal history was characterized by gradual cooling from peak temperatures at the transition from Triassic to Jurassic due to decreasing heat flow. Burial caused maximum paleotemperatures in the SW part of the study area, where the EEP was covered by an extensive sedimentary pile. However, further NE, due to low temperatures caused by shallow burial, the impact of fluids can be detected by vitrinite reflectance, illite/smectite, and thermochronological data. Our new results emphasize the importance of using multiple low-temperature thermochronometers and thermal modelling in connection with thermal maturity analysis to elucidate the near-surface evolution of platform margins.

Beschreibung: Snow stands out from materials at the Earth’s surface owing to its unique optical properties. Snow optical properties are sensitive to the snow microstructure, triggering potent climate feedbacks. The impacts of snow microstructure on its optical properties such as reflectance are, to date, only partially understood. However, precise modelling of snow reflectance, particularly bidirectional reflectance, are required in many problems, e.g. to correctly process satellite data over snow-covered areas. This study presents a dataset that combines bidirectional reflectance measurements over 500–2500 nm and the X-ray tomography of the snow microstructure for three snow samples of two different morphological types. The dataset is used to evaluate the stereological approach from Malinka (2014) that relates snow optical properties to the chord length distribution in the snow microstructure. The mean chord length and specific surface area (SSA) retrieved with this approach from the albedo spectrum and those measured by the X-ray tomography are in excellent agreement. The analysis of the 3D images has shown that the random chords of the ice phase obey the gamma distribution with the shape parameter m taking the value approximately equal to or a little greater than 2. For weak and intermediate absorption (high and medium albedo), the simulated bidirectional reflectances reproduce the measured ones accurately but tend to slightly overestimate the anisotropy of the radiation. For such absorptions the use of the exponential law for the ice chord length distribution instead of the one measured with the X-ray tomography does not affect the simulated reflectance. In contrast, under high absorption (albedo of a few percent), snow microstructure and especially facet orientation at the surface play a significant role in the reflectance, particularly at oblique viewing and incidence.

Beschreibung: Attribution in its general definition aims to quantify drivers of change in a system. According to IPCC Working Group II (WGII) a change in a natural, human or managed system is attributed to climate change by quantifying the difference between the observed state of the system and a counterfactual baseline that characterizes the system's behavior in the absence of climate change, where “climate change refers to any long-term trend in climate, irrespective of its cause” (IPCC, 2014). Impact attribution following this definition remains a challenge because the counterfactual baseline, which characterizes the system behavior in the hypothetical absence of climate change, cannot be observed. Process-based and empirical impact models can fill this gap as they allow us to simulate the counterfactual climate impact baseline. In those simulations, the models are forced by observed direct (human) drivers such as land use changes, changes in water or agricultural management but a counterfactual climate without long-term changes. We here present ATTRICI (ATTRIbuting Climate Impacts), an approach to construct the required counterfactual stationary climate data from observational (factual) climate data. Our method identifies the long-term shifts in the considered daily climate variables that are correlated to global mean temperature change assuming a smooth annual cycle of the associated scaling coefficients for each day of the year. The produced counterfactual climate datasets are used as forcing data within the impact attribution setup of the Inter-Sectoral Impact Model Intercomparison Project (ISIMIP3a). Our method preserves the internal variability of the observed data in the sense that factual and counterfactual data for a given day have the same rank in their respective statistical distributions. The associated impact model simulations allow for quantifying the contribution of climate change to observed long-term changes in impact indicators and for quantifying the contribution of the observed trend in climate to the magnitude of individual impact events. Attribution of climate impacts to anthropogenic forcing would need an additional step separating anthropogenic climate forcing from other sources of climate trends, which is not covered by our method.

Beschreibung: Biocides used in film protection products leaching from facades are known to be a potential threat to the environment. This study identifies individual sources and entry pathways in a small-scale urban area. We investigate emissions of commonly used biocides (terbutryn, diuron, and octylisothiazolinone – OIT) and some of their transformation products (TPs; diuron-desmethyl, terbumeton, terbuthylazine-2-hydroxy, and terbutryn-desethyl) from a 2 ha residential area 13 years after construction has ended. Sampling utilizes existing urban water infrastructure representative for decentralized storm water management in central and northern Europe and applies a two-step approach to (a) determine the occurrence of biocides above water quality limits (i.e., predicted no-effect concentration, PNEC) and (b) identify source areas and characterize entry pathways into surface and groundwater. Monitoring focuses on the analysis of selected biocides and TPs by liquid chromatography–mass spectrometry/mass spectrometry (LC-MS/MS) in water samples taken from facades, rainwater pipes, drainage, and storm water infiltration systems. In standing water in a swale, we found high concentrations of diuron (174 ng L−1) and terbutryn (40 ng L−1) above PNEC for surface water. We confirmed expected sources, i.e., facades. Sampling of rain downpipes from flat roofs identified additional sources of all biocides and two TPs of terbutryn and one TP of diuron. Diuron and terbutryn were found in three drainage pipes representing different entry pathways of biocides. In one drainage pipe collecting road runoff, only diuron-desmethyl and terbutryn-desethyl were detected. In two other drainage pipes collecting infiltrated water through soil, terbuthylazine-2-hydroxy was additionally detected. One of the pipes collecting infiltrated water through soil concentration showed the highest concentrations of terbutryn and two of its TPs (terbutryn-desethyl and terbuthylazine-2-hydroxy). This suggests a high leaching potential of terbutryn. The applied two-step approach determined sources and pathways of biocide and their TPs. This study contributes to expanding knowledge on their entry and distribution and, thus, eventually towards reducing emissions.

Beschreibung: Regional anomalies of steric sea level are either due to redistribution of heat and freshwater anomalies or due to ocean–atmosphere buoyancy fluxes. Interannual to decadal variability in sea level across the tropical Pacific is mainly due to steric variations driven by wind stress anomalies. The importance of air–sea buoyancy fluxes is less clear. We use a global, eddy-permitting ocean model and a series of sensitivity experiments with quasi-climatological momentum and buoyancy fluxes to identify the contribution of buoyancy fluxes for interannual to decadal sea level variability in the tropical Pacific. We find their contribution on interannual timescales to be strongest in the central tropical Pacific at around a 10∘ latitude in both hemispheres and also relevant in the very east of the tropical domain. Buoyancy-flux-forced anomalies are correlated with variations driven by wind stress changes, but their effect on the prevailing anomalies and the importance of heat and freshwater fluxes vary locally. In the eastern tropical basin, interannual sea level variability is amplified by anomalous heat fluxes, while the importance of freshwater fluxes is small, and neither has any impact on decadal timescales. In the western tropical Pacific, the variability on interannual and decadal timescales is dampened by both heat and freshwater fluxes. The mechanism involves westward-propagating Rossby waves that are triggered during El Niño–Southern Oscillation (ENSO) events by anomalous buoyancy fluxes in the central tropical Pacific and counteract the prevailing sea level anomalies once they reach the western part of the basin.

Beschreibung: The Nioghalvfjerdsfjorden glacier (also known as the 79∘ North Glacier) drains approximately 8 % of the Greenland Ice Sheet. Supraglacial lakes (SGLs), or surface melt ponds, are a persistent summertime feature and are thought to drain rapidly to the base of the glacier and influence seasonal ice velocity. However, seasonal development and spatial distribution of SGLs in the north-east of Greenland are poorly understood, leaving a substantial error in the estimate of meltwater and its impacts on ice velocity. Using results from an automated detection of melt ponds, atmospheric and surface mass balance modelling, and reanalysis products, we investigate the role of specific climatic conditions in melt onset, extent, and duration from 2016 to 2019. The summers of 2016 and 2019 were characterised by above-average air temperatures, particularly in June, as well as a number of rainfall events, which led to extensive melt ponds to elevations up to 1600 m. Conversely, 2018 was particularly cold, with a large accumulated snowpack, which limited the development of lakes to altitudes less than 800 m. There is evidence of inland expansion and increases in the total area of lakes compared to the early 2000s, as projected by future global warming scenarios.

Beschreibung: Coincident wide-angle and multi-channel seismic data acquired within the scope of the PAMELA Moz3-5 project allow us to reconsider the formation mechanism of East African margins offshore of southern Mozambique. This study specifically focuses on the sedimentary and deep-crustal architecture of the Limpopo margin (LM) that fringes the eastern edge of the Mozambique’s Coastal Plain (MCP) and its offshore southern prolongation the North Natal Valley (NNV). It relies primarily on the MZ3 profile that runs obliquely from the northeastern NNV towards the Mozambique basin (MB) with additional inputs from a tectonostratigraphy analysis of industrial onshore–offshore seismic lines and nearby or crossing velocity models from companion studies. Over its entire N–S extension the LM appears segmented into (1) a western domain that shows the progressive eastward crustal thinning and termination of the MCP/NNV continental crust and its overlying pre-Neocomian volcano-sedimentary basement and (2) a central corridor of anomalous crust bounded to the east by the Mozambique fracture zone (MFZ) and the oceanic crust of the MB. A prominent basement high marks the boundary between these two domains. Its development was most probably controlled by a steep and deeply rooted fault, i.e., the Limpopo fault. We infer that strike-slip or slightly transtensional rifting occurred along the LM and was accommodated along this Limpopo fault. At depth we propose that ductile shearing was responsible for the thinning of the continental crust and an oceanward flow of lower crustal material. This process was accompanied by intense magmatism that extruded to form the volcanic basement and gave the corridor its peculiar structure and mixed nature. The whole region remained at a relative high level during the rifting period and a shallow marine environment dominated the pre-Neocomian period during the early phase of continent–ocean interaction. It is only some time after break-up in the MB and the initiation of the MFZ that decoupling occurred between the MCP/NNV and the corridor, allowing for the latter to subside and become covered by deep marine sediments. A scenario for the early evolution and formation of the LM is proposed taking into account both recent kinematic and geological constraints. It implies that no or little change in extensional direction occurred between the intra-continental rifting and subsequent phase of continent–ocean interaction.

Beschreibung: Models are an important tool to predict Earth system dynamics. An accurate prediction of future states of ecosystems depends on not only model structures but also parameterizations. Model parameters can be constrained by data assimilation. However, applications of data assimilation to ecology are restricted by highly technical requirements such as model-dependent coding. To alleviate this technical burden, we developed a model-independent data assimilation (MIDA) module. MIDA works in three steps including data preparation, execution of data assimilation, and visualization. The first step prepares prior ranges of parameter values, a defined number of iterations, and directory paths to access files of observations and models. The execution step calibrates parameter values to best fit the observations and estimates the parameter posterior distributions. The final step automatically visualizes the calibration performance and posterior distributions. MIDA is model independent, and modelers can use MIDA for an accurate and efficient data assimilation in a simple and interactive way without modification of their original models. We applied MIDA to four types of ecological models: the data assimilation linked ecosystem carbon (DALEC) model, a surrogate-based energy exascale earth system model: the land component (ELM), nine phenological models and a stand-alone biome ecological strategy simulator (BiomeE). The applications indicate that MIDA can effectively solve data assimilation problems for different ecological models. Additionally, the easy implementation and model-independent feature of MIDA breaks the technical barrier of applications of data–model fusion in ecology. MIDA facilitates the assimilation of various observations into models for uncertainty reduction in ecological modeling and forecasting.

Beschreibung: We assess the potential damage and smoke production associated with the detonation of small nuclear weapons in modern megacities. While the number of nuclear warheads in the world has fallen by about a factor of three since its peak in 1986, the number of nuclear weapons states is increasing and the potential exists for numerous regional nuclear arms races. Eight countries are known to have nuclear weapons, 2 are constructing them, and an additional 32 nations already have the fissile material needed to build substantial arsenals of low-yield (Hiroshima-sized) explosives. Population and economic activity worldwide are congregated to an increasing extent in megacities, which might be targeted in a nuclear conflict. Our analysis shows that, per kiloton of yield, low yield weapons can produce 100 times as many fatalities and 100 times as much smoke from fires as high-yield weapons, if they are targeted at city centers. A single "small'' nuclear detonation in an urban center could lead to more fatalities, in some cases by orders of magnitude, than have occurred in the major historical conflicts of many countries. We analyze the likely outcome of a regional nuclear exchange involving 100 15-kt explosions (less than 0.1% of the explosive yield of the current global nuclear arsenal). We find that such an exchange could produce direct fatalities comparable to all of those worldwide in World War II, or to those once estimated for a "counterforce'' nuclear war between the superpowers. Megacities exposed to atmospheric fallout of long-lived radionuclides would likely be abandoned indefinitely, with severe national and international implications. Our analysis shows that smoke from urban firestorms in a regional war would rise into the upper troposphere due to pyro-convection. Robock et al. (2006) show that the smoke would subsequently rise deep into the stratosphere due to atmospheric heating, and then might induce significant climatic anomalies on global scales.We also anticipate substantial perturbations of global ozone. While there are many uncertainties in the predictions we make here, the principal unknowns are the type and scale of conflict that might occur. The scope and severity of the hazards identified pose a significant threat to the global community. They deserve careful analysis by governments worldwide advised by a broad section of the world scientific community, as well as widespread public debate.

Beschreibung: We briefly present in this short paper a new SIze REsolved Aerosol Model (SIREAM) which simulates the evolution of atmospheric aerosol by solving the General Dynamic Equation (GDE). SIREAM segregates the aerosol size distribution into sections and solves the GDE by splitting coagulation and condensation/evaporation. A moving sectional approach is used to describe the size distribution change due to condensation/evaporation and a hybrid method has been developed to lower the computational burden. SIREAM uses the same physical parameterizations as those used in the Modal Aerosol Model, MAM sartelet05development. It is hosted in the modeling system POLYPHEMUS (Mallet et al., 2006) but can be linked to any other three-dimensional Chemistry-Transport Model.

Beschreibung: The results from three 45-year simulations of a coupled chemistry climate model are analysed for solar cycle influences on ozone and temperature. The simulations include UV forcing at the top of the atmosphere, which includes a generic 27-day solar rotation effect as well as the observed monthly values of the solar fluxes. The results are analysed for the 27-day and 11-year cycles in temperature and ozone. In accordance with previous results, the 27-day cycle results are in good qualitative agreement with observations, particularly for ozone. However, the results show significant variations, typically a factor of two or more in sensitivity to solar flux, depending on the solar cycle. We show for the first time good agreement also between the observed 11-year cycle and model results for the ozone vertical profile, which both indicate a minimum in solar response near 20 hPa. In comparison, simulations of the model with fixed solar phase (solar maximum/solar mean) and climatological sea surface temperatures lead to a poor simulation of the solar response in the ozone vertical profile. The results indicate the need for variable phase simulations in solar sensitivity experiments and the role of sea surface temperatures is discussed.

Beschreibung: The aerosol chemical mass closure is revisited and a simple and inexpensive methodology is proposed. This methodology relies on data obtained for aerosol mass, and concentration of the major ions and the two main carbon components, the organic carbon (OC) and the black carbon (BC). Atmospheric particles are separated into coarse (AD〉2µm) and fine (AD

Beschreibung: Knowledge of molecular photolysis cross sections is important for determining atmospheric lifetimes and fates of many species. A method and laser apparatus for measurement of these cross sections in the near-ultraviolet (UV) region is described. The technique is based on action spectroscopy, where the yield of a photodissociation product (in this case OH) is measured as a function of excitation energy. For compounds yielding OH, this method can be used to measure near-UV photodissociation cross section as low as 10−23 cm2 molecule−1. The method is applied to determine the photodissociation cross sections for methyl hydroperoxide (CH3OOH; MHP) and hydroxymethyl hydroperoxide (HOCH2OOH; HMHP) in the 305–365 nm wavelength range. The measured cross sections are in good agreement with previous measurements of absorption cross sections.

Beschreibung: We describe and begin to evaluate a parameterization to include the vertical transport of hot gases and particles emitted from biomass burning in low resolution atmospheric-chemistry transport models. This sub-grid transport mechanism is simulated by embedding a 1-D cloud-resolving model with appropriate lower boundary conditions in each column of the 3-D host model. Through assimilation of remote sensing fire products, we recognize which columns have fires. Using a land use dataset appropriate fire properties are selected. The host model provides the environmental conditions, allowing the plume rise to be simulated explicitly. The derived height of the plume is then used in the source emission field of the host model to determine the effective injection height, releasing the material emitted during the flaming phase at this height. Model results are compared with CO aircraft profiles from an Amazon basin field campaign and with satellite data, showing the huge impact that this mechanism has on model performance. We also show the relative role of each main vertical transport mechanisms, shallow and deep moist convection and the pyro-convection (dry or moist) induced by vegetation fires, on the distribution of biomass burning CO emissions in the troposphere.

Beschreibung: We use a modern climate model and new estimates of smoke generated by fires in contemporary cities to calculate the response of the climate system to a regional nuclear war between emerging third world nuclear powers using 100 Hiroshima-size bombs (less than 0.03% of the explosive yield of the current global nuclear arsenal) on cities in the subtropics. We find significant cooling and reductions of precipitation lasting years, which would impact the global food supply. The climate changes are large and long-lasting because the fuel loadings in modern cities are quite high and the subtropical solar insolation heats the resulting smoke cloud and lofts it into the high stratosphere, where removal mechanisms are slow. While the climate changes are less dramatic than found in previous "nuclear winter'' simulations of a massive nuclear exchange between the superpowers, because less smoke is emitted, the changes are more long-lasting because the older models did not adequately represent the stratospheric plume rise.

Beschreibung: Retrieved aerosol optical thickness (AOT) based on data obtained by the Sea viewing Wide Field Sensor (SeaWiFS) is combined with surface wind speed, obtained at the European Centre for Medium-Range Weather Forecasts (ECMWFs), over the North Pacific for September 2001. In this study a cloud screening approach is introduced in an attempt to exclude pixels partly or fully covered by clouds. The relatively broad swath width for which the nadir looking SeaWiFS instrument scanned over the North Pacific means that the AOT can be estimated according to relatively large range of wind speeds for each of the scenes analyzed. The sensitivity in AOT due to sea salt and hygroscopic growth of the marine aerosols has also been investigated. The validation of the results is based on previous parameterization in combination with the environmental quantities wind speed, RH and boundary layer height (BLH), estimated at the ECMWF. In this study a factor of 2 higher mean AOT is obtained for a wind speed up to about 13 m s−1 for September 2001 over remote ocean areas. Furthermore, a factor of 2 higher AOT is more or less supported by the validation of the results. Approximately, 50% of the enhancement seems to be due to hygroscopic growth of the marine aerosols and the remaining part due to increase in the sea salt particle mass concentrations, caused by a wind driven water vapor and sea salt flux, respectively. Reasonable agreement occurs also between satellites retrieved aerosol optical thickness and AOT observed at several AERONET (Aerosol Robotic NETwork) ground-based remote sensing stations. Finally, possible reasons why relatively large standard deviations occur around the mean values of AOT estimated for a single scene are discussed.

Beschreibung: Improving the constraints on the atmospheric fate and depletion rates of acidic compounds persistently emitted by non-erupting (quiescent) volcanoes is important for quantitatively predicting the environmental impact of volcanic gas plumes. Here, we present new experimental data coupled with modelling studies to investigate the chemical processing of acidic volcanogenic species during tropospheric dispersion. Diffusive tube samplers were deployed at Mount Etna, a very active open-conduit basaltic volcano in eastern Sicily, and Vulcano Island, a closed-conduit quiescent volcano in the Aeolian Islands (northern Sicily). Sulphur dioxide (SO2), hydrogen sulphide (H2S), hydrogen chloride (HCl) and hydrogen fluoride (HF) concentrations in the volcanic plumes (typically several minutes to a few hours old) were repeatedly determined at distances from the summit vents ranging from 0.1 to ~10 km, and under different environmental conditions. At both volcanoes, acidic gas concentrations were found to decrease exponentially with distance from the summit vents (e.g., SO2 decreases from ~10 000 μg/m3 at 0.1 km from Etna's vents down to ~7 μg/m3 at ~10 km distance), reflecting the atmospheric dilution of the plume within the acid gas-free background troposphere. Conversely, SO2/HCl, SO2/HF, and SO2/H2S ratios in the plume showed no systematic changes with plume aging, and fit source compositions within analytical error. Assuming that SO2 losses by reaction are small during short-range atmospheric transport within quiescent (ash-free) volcanic plumes, our observations suggest that, for these short transport distances, atmospheric reactions for H2S and halogens are also negligible. The one-dimensional model MISTRA was used to simulate quantitatively the evolution of halogen and sulphur compounds in the plume of Mt. Etna. Model predictions support the hypothesis of minor HCl chemical processing during plume transport, at least in cloud-free conditions. Larger variations in the modelled SO2/HCl ratios were predicted under cloudy conditions, due to heterogeneous chlorine cycling in the aerosol phase. The modelled evolution of the SO2/H2S ratios is found to be substantially dependent on whether or not the interactions of H2S with halogens are included in the model. In the former case, H2S is assumed to be oxidized in the atmosphere mainly by OH, which results in minor chemical loss for H2S during plume aging and produces a fair match between modelled and measured SO2/H2S ratios. In the latter case, fast oxidation of H2S by Cl leads to H2S chemical lifetimes in the early plume of a few seconds, and thus SO2 to H2S ratios that increase sharply during plume transport. This disagreement between modelled and observed plume compositions suggests that more in-detail kinetic investigations are required for a proper evaluation of H2S chemical processing in volcanic plumes.

Beschreibung: The Active Tracer High-resolution Atmospheric Model (ATHAM) has been adopted to examine the aerosol indirect effect in contrasting clean and polluted cloudy boundary layers during the Second Aerosol Characterization Experiment (ACE-2). Model results are in good agreement with available in-situ observations, which provides confidence in the results of ATHAM. Sensitivity tests have been conducted to examine the response of the cloud fraction (CF), cloud liquid water path (LWP), and cloud optical depth (COD) to changes in aerosols in the clean and polluted cases. It is shown for two cases that CF and LWP would decrease or remain nearly constant with an increase in aerosols, a result which shows that the second aerosol indirect effect is positive or negligibly small in these cases. Further investigation indicates that the background meteorological conditions play a critical role in the response of CF and LWP to aerosols. When large-scale subsidence is weak as in the clean case, the dry overlying air above the cloud is more efficiently entrained into the cloud, and in so doing, removes cloud water more efficiently, and results in lower CF and LWP when aerosol burden increases. However, when the large-scale subsidence is strong as in the polluted case, the growth of the cloud top is suppressed and the entrainment drying makes no significant difference when aerosol burden increases. Therefore, the CF and LWP remain nearly constant. In both the clean and polluted cases, the COD tends to increase with aerosols, and the total aerosol indirect effect (AIE) is negative even when the CF and LWP decrease with an increase in aerosols. Therefore, the first AIE dominates the response of the cloud to aerosols.

Beschreibung: We use a global chemical transport model (GEOS-Chem) to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flash counts improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 5±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils) and VOCs (biomass burning). The top-down biomass burning inventory is larger by a factor of 2 for HCHO and alkenes, and by 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4) is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv due to enhanced convective detrainment in the upper troposphere. Heterogeneous uptake of HNO3 on aerosols reduces simulated O3 by 5–7 ppbv, reducing a model bias versus in situ observations over and downwind of deserts. Exclusion of HO2 uptake on aerosols improves O3 by 5 ppbv in biomass burning regions.

Beschreibung: The mechanisms responsible for the extreme dryness of the stratosphere have been debated for decades. A key difficulty has been the lack of models which are able to reproduce the observations. Here we examine results from a new atmospheric chemistry general circulation model (ECHAM5/MESSy1) together with satellite observations. Our model results match observed temperatures in the tropical lower stratosphere and realistically represent recurrent features such as the semi-annual oscillation (SAO) and the quasi-biennual oscillation (QBO), indicating that dynamical and radiation processes are simulated accurately. The model reproduces the very low water vapor mixing ratios (1–2 ppmv) periodically observed at the tropical tropopause near 100 hPa, as well as the characteristic tape recorder signal up to about 10 hPa, providing evidence that the dehydration mechanism is well-captured, albeit that the model underestimates convective overshooting and consequent moistening events. Our results show that the entry of tropospheric air into the stratosphere at low latitudes is forced by large-scale wave dynamics; however, radiative cooling can regionally limit the upwelling or even cause downwelling. In the cold air above cumulonimbus anvils thin cirrus desiccates the air through the sedimentation of ice particles, similar to polar stratospheric clouds. Transport deeper into the stratosphere occurs in regions where radiative heating becomes dominant, to a large extent in the subtropics. During summer the stratosphere is moistened by the monsoon, most strongly over Southeast Asia.

Beschreibung: Spores and related chemical compounds from actively spore-discharging Ascomycota (AAM) and actively spore-discharging Basidiomycota (ABM) are primary biogenic components of air particulate matter (characteristic size range 1–10 μm). Measurement results and budget calculations based on investigations in Amazonia (Balbina, Brazil, July 2001) indicate that the forcible discharge of fungal spores may account for a large proportion of coarse air particulate matter in tropical rainforest regions during the wet season. For the particle diameter range of 1–10 μm, the estimated proportions are ~25% during day-time, ~45% at night, and ~35% on average. For the sugar alcohol, mannitol, the budget calculations indicate that it is suitable for use as a molecular tracer for actively discharged basidiospores (ABS), and that the literature-derived emission ratio of about 5 pg per ABS may be taken as a representative average. ABM emissions may account for most of the atmospheric abundance of mannitol, and can explain the observed diurnal cycle (higher abundance at night). ABM emissions of hexose carbohydrates might also account for a significant proportion of glucose and fructose in air particulate matter, but the literature-derived ratios are not consistent with the observed diurnal cycle (lower abundance at night). AAM emissions appear to account for a large proportion of potassium in air particulate matter over tropical rainforest regions during the wet season, and they can also explain the observed diurnal cycle (higher abundance at night). The results of our investigations and budget calculations for tropical rainforest aerosols are consistent with measurements performed at other locations. Based on the average abundance of mannitol in particulate matter, which is consistent with the above emission ratio and the observed abundance of ABS, we have also calculated a value of ~17 Tg yr−1 as a first estimate for the global average emission rate of ABS over land surfaces. Comparisons with estimated rates of emission and formation of other major types of organic aerosol (~47 Tg yr−1 of anthropogenic primary organic aerosol; 12–70 Tg yr−1 of secondary organic aerosol) indicate that emissions from actively spore-discharging fungi should be taken into account as a significant source of organic aerosol. Their effects might be particularly important in tropical regions, where both physicochemical processes in the atmosphere and biological activity at the Earth's surface are particularly intense, and where the abundance of fungal spores and related chemical compounds are typically higher than in extratropical regions.

Beschreibung: The upwelling planetary wave activity (PW) from the troposphere controls the intensity of the equator to pole transport of stratospheric ozone by the Brewer-Dobson circulation and thereby modulates the total ozone content at mid- and high-latitudes. Rayleigh lidar temperature data obtained from 1981 to 2001 at mid-latitude were used to study the interannual variability of PW activity in winter (October to April). The spectrum of stratospheric temperature fluctuations exhibits 2 peaks corresponding to 2 dominant modes of free travelling Rossby waves known as 16 day- and 12 day-waves. The 12 day-wave activity is shown to be anticorrelated with the equatorial QBO wind at 40 hPa. During the period 1981–2000 the global PW activity shows a negative trend for months October to January and a positive trend in March and April.

Beschreibung: The use of SAGE III multiwavelength aerosol extinction coefficient measurements to infer PSC type is contingent on the robustness of both the extinction magnitude and its spectral variation. Past validation with SAGE II and other similar measurements has shown that the SAGE III extinction coefficient measurements are reliable though the comparisons have been greatly weighted toward measurements made at mid-latitudes. Some aerosol comparisons made in the Arctic winter as a part of SOLVE II suggested that SAGE III values, particularly at longer wavelengths, are too small with the implication that both the magnitude and the wavelength dependence are not reliable. Comparisons with POAM III have also suggested a similar discrepancy. Herein, we use SAGE II data as a common standard for comparison of SAGE III and POAM III measurements in the Arctic winters of 2002/2003 through 2004/2005. During the winter, SAGE II measurements are made infrequently at the same latitudes as these instruments. We have mitigated this problem through the use potential vorticity as a spatial coordinate and thus greatly increased the number of coincident events. We find that SAGE II and III extinction coefficient measurements show a high degree of compatibility at both 1020 nm and 450 nm except a 10–20% bias at both wavelengths. In addition, the 452 to 1020 nm extinction ratio shows a consistent bias of ~30% throughout the lower stratosphere. We also find that SAGE II and POAM III are on average consistent though the comparisons show a much higher variability and larger bias than SAGE II/III comparisons. In addition, we find that the two data sets are not well correlated below 18 km. Overall, we find both the extinction values and the spectral dependence from SAGE III are robust and we find no evidence of a significant defect within the Arctic vortex.

Beschreibung: In this paper, we study the transport of air mass to San Pietro Capofiume (SPC) in Po Valley, Italy, by means of back trajectory analysis. Our main aim is to investigate whether air masses originate from different regions on nucleation event days and on nonevent days, during three years when nucleation events have been continuously recorded at SPC. The results indicate that nucleation events occur frequently in air masses arriving form Central Europe, whereas event frequency is much lower in air transported from southern directions and from the Atlantic Ocean. We also analyzed the behaviour of meteorological parameters during 96 h transport to SPC, and found that on average, event trajectories undergo stronger subsidence during the last 12 h before the arrival at SPC than nonevent trajectories. This causes a reversal in the temperature and relative humidity (RH) differences between event and nonevent trajectories: between 96 and 12 h back time, temperatures are lower and RH's higher for event than nonevent trajectories and between 12 and 0 h vice versa. Boundary layer mixing is stronger along the event trajectories compared to nonevent trajectories. The absolute humidity (AH) is similar for the event and nonevent trajectories between about 96 h and about 60 h back time, but after that, the event trajectories AH becomes lower due to stronger rain. We also studied transport of SO2 to SPC, and conclude that although sources in Po Valley most probably dominate the measured concentrations, certain Central and Eastern European sources can also have a non-negligible contribution.

Beschreibung: Reactive halogens are responsible for boundary-layer ozone depletion and mercury deposition in Polar Regions during springtime. To investigate the source of reactive halogens in the air arriving at Barrow, Alaska, we measured BrO, a marker of reactive halogen chemistry, and correlated its abundance with airmass histories derived from meteorological back trajectories and remotely sensed sea ice properties. The BrO is found to be positively correlated to first-year sea-ice contact (R2=0.55), and weakly negatively correlated to potential frost flower (PFF) contact (R2=0.04). These data indicate that snow contaminated with sea salts on first-year sea ice is a more probable bromine source than are frost flowers. Recent climate-driven changes in Arctic sea ice are likely to alter frost flower and first year sea ice prevalence, suggesting a significant change in reactive halogen abundance, which will alter the chemistry of the overlying Arctic atmosphere.

Beschreibung: Systematic analyses of interannual and seasonal variations of tropospheric NO2 vertical column densities (VCDs) based on GOME satellite data and the regional scale chemical transport model (CTM), Community Multi-scale Air Quality (CMAQ), are presented over eastern Asia between 1996 and June 2003. A newly developed year-by-year emission inventory (REAS) was used in CMAQ. The horizontal distribution of annual averaged GOME NO2 VCDs generally agrees well with the CMAQ results. However, CMAQ/REAS results underestimate the GOME retrievals with factors of 2–4 over polluted industrial regions such as Central East China (CEC), a major part of Korea, Hong Kong, and central and western Japan. For the Japan region, GOME and CMAQ NO2 data show good agreement with respect to interannual variation and show no clear increasing trend. For CEC, GOME and CMAQ NO2 data show good agreement and indicate a very rapid increasing trend from 2000. Analyses of the seasonal cycle of NO2 VCDs show that GOME data have systematically larger dips than CMAQ NO2 during February–April and September–November. Sensitivity experiments with fixed emission intensity reveal that the detection of emission trends from satellite in fall or winter have a larger error caused by the variability of meteorology. Examination during summer time and annual averaged NO2 VCDs are robust with respect to variability of meteorology and are therefore more suitable for analyses of emission trends. Analysis of recent trends of annual emissions in China shows that the increasing trends of 1996–1998 and 2000–2002 for GOME and CMAQ/REAS show good agreement, but the rate of increase by GOME is approximately 10–11% yr−1 after 2000; it is slightly steeper than CMAQ/REAS (8–9% yr−1). The greatest difference was apparent between the years 1998 and 2000: CMAQ/REAS only shows a few percentage points of increase, whereas GOME gives a greater than 8% yr−1 increase. The exact reason remains unclear, but the most likely explanation is that the emission trend based on the Chinese emission related statistics underestimates the rapid growth of emissions.

Beschreibung: The heterogeneous processing of organic aerosols by trace oxidants has many implications to atmospheric chemistry and climate regulation. This review covers a model heterogeneous reaction system (HRS): the oleic acid-ozone HRS and other reaction systems featuring fatty acids, and their derivatives. The analysis of the primary products of ozonolysis (azelaic acid, nonanoic acid, 9-oxononanoic acid, nonanal) is described. Anomalies in the relative product yields are noted and explained by the observation of secondary chemical reactions. The secondary reaction products arising from reactive Criegee intermediates are mainly peroxidic, notably secondary ozonides and α-acyloxyalkyl hydroperoxide polymers. These highly oxygenated products are of low volatility and hydrophilic which may enhance the ability of particles to act as cloud condensation nuclei. The kinetic description of this HRS is critically reviewed. Most kinetic studies suggest this oxidative processing is either a near surface reaction that is limited by the diffusion of ozone or a surface based reaction. Internally mixed particles and coatings represent the next stage in the progression towards more realistic proxies of tropospheric organic aerosols and a description of the products and the kinetics resulting from the ozonolysis of these proxies, which are based on fatty acids or their derivatives, is presented. Finally, a series of atmospheric implications of oxidative processing of particulate containing fatty acids is presented. These implications include the extended lifetime of unsaturated species in the troposphere facilitated by the presence of solids, semisolids or viscous phases, and an enhanced rate of ozone uptake by particulate unsaturates compared to corresponding gas phase organics. Ozonolysis of oleic acid enhances its CCN activity, which implies that oxidatively processed particulate may contribute to indirect forcing of radiation. Other effects, including the potential role of aldehydic products of ozonolysis in increasing the oxidative capacity of the troposphere, are also discussed.

Beschreibung: The speciation of iodine in atmospheric aerosol is currently poorly understood. Models predict negligible iodide concentrations and accumulation of iodate in aerosol, both of which is not confirmed by recent measurements. We present an updated aqueous phase iodine chemistry scheme for use in atmospheric chemistry models and discuss sensitivity studies with the marine boundary layer model MISTRA. These studies show that iodate can be reduced in acidic aerosol by inorganic reactions, i.e., iodate does not necessarily accumulate in particles. Furthermore, the transformation of particulate iodide to volatile iodine species likely has been overestimated in previous model studies due to negligence of collision-induced upper limits for the reaction rates. However, inorganic reaction cycles still do not seem to be sufficient to reproduce the observed range of iodide – iodate speciation in atmospheric aerosol. Therefore, we also investigate the effects of the recently suggested reaction of HOI with dissolved organic matter to produce iodide. If this reaction is fast enough to compete with the inorganic mechanism, it would not only directly lead to enhanced iodide concentrations but, indirectly via speed-up of the inorganic iodate reduction cycles, also to a decrease in iodate concentrations. Hence, according to our model studies, organic iodine chemistry, combined with inorganic reaction cycles, is able to reproduce observations. The presented chemistry cycles are highly dependent on pH and thus offer an explanation for the large observed variability of the iodide – iodate speciation in atmospheric aerosol.

Beschreibung: In order to improve the representation of the shortwave radiative transfer in the MAECHAM5 general circulation model, the spectral resolution of the shortwave radiation parameterization used in the model has been increased and extended in the UV-B and UV-C bands. The upgraded shortwave parameterization is first validated offline with a 4 stream discrete-ordinate line-by-line model. Thereafter, two 20-years simulations with the MAECHAM5 middle atmosphere general circulation model are performed to evaluate the temperature changes and the dynamical feedbacks arising from the newly introduced parameterization. The offline clear-sky comparison of the standard and upgraded parameterizations with the discrete ordinate model shows considerable improvement for the upgraded parameterization in terms of shortwave fluxes and heating rates. In the simulation with the upgraded ratiation parameterization, we report a significant warming of almost the entire atmosphere, largest at 1 hPa at the stratopause, and stronger zonal mean zonal winds in the middle atmosphere. The warming at the summer stratopause alleviates the cold bias present in the model when the standard radiation scheme is used. The stronger zonal mean zonal winds induce a dynamical feedback that results in a dynamical warming (cooling) of the polar winter (summer) mesosphere, caused by an increased downward (upward) circulation in the winter (summer) hemisphere. In the troposphere, the changes in the spectral resolution and the associated changes in the cloud optical parameters introduce a relatively small warming and, consistenly, a moisteneing. The warming occurs mostly in the upper troposphere and can contribute to a possible improvement of the model temperature climatology.

Beschreibung: This study investigates the connections between atmospheric sulphuric acid and new particle formation during QUEST III and BACCI/QUEST IV campaigns. The campaigns have been conducted in Heidelberg (2004) and Hyytiälä (2005), the first representing a polluted site surrounded by deciduous forest, and the second a rural site in a boreal forest environment. We have studied the role of sulphuric acid in particle formation and growth by determining 1) the power-law dependencies between sulphuric acid ([H2SO4]), and particle concentrations (N3–6) or formation rates at 1 nm and 3 nm (J1 and J3; 2) the time delays between [H2SO4] and N3–6 or J3, and the growth rates for 1–3 nm particles; 3) the empirical nucleation coefficients A and K in relations J1=A[H2SO4] and J1=K[H2SO4]2, respectively; 4) theoretical predictions for J1 and J3 for the days when no significant particle formation is observed, based on the observed sulphuric acid concentrations and condensation sinks. In both environments, N3–6 or J3 and [H2SO4] were linked via a power-law relation with exponents typically ranging from 1 to 2. The result suggests that the cluster activation theory and kinetic nucleation have the potential to explain the observed particle formation. However, some differences between the sites existed: The 1–3 nm growth rates were slightly higher and the nucleation coefficients about an order of magnitude greater in Heidelberg than in Hyytiälä conditions. The time lags between J3 and [H2SO4] were consistently lower than the corresponding delays between N3–6 and [H2SO4]. The exponents in the J3∝[H2SO4]nJ3-connection were consistently higher than or equal to the exponents in the relation N3–6∝[H2SO4]nN36. In the J1 values, no significant differences were found between the observed rates on particle formation event days and the predictions on non-event days. The J3 values predicted by the cluster activation or kinetic nucleation hypotheses, on the other hand, were considerably lower on non-event days than the rates observed on particle formation event days. This study provides clear evidence implying that the main process limiting the observable particle formation is the competition between the growth of the freshly formed particles and their loss by scavenging, rather than the initial particle production by nucleation of sulphuric acid. In general, it can be concluded that the simple models based on sulphuric acid concentrations and particle formation by cluster activation or kinetic nucleation can predict the occurence of atmospheric particle formation and growth well, if the particle scavenging is accurately accounted for.

Beschreibung: Atmospheric cloud condensation nuclei (CCN) concentrations are a key uncertainty in the assessment of the effect of anthropogenic aerosols on clouds and climate. The ability of new ultrafine particles to grow to become CCN varies throughout the atmosphere and must be understood in order to understand CCN formation. We have developed the Probability of Ultrafine particle Growth (PUG) model to answer questions regarding which growth and sink mechanisms control this growth, how the growth varies between different parts of the atmosphere and how uncertainties with respect to the magnitude and size distribution of ultrafine emissions translates into uncertainty in CCN generation. It was found in most cases that condensation is the dominant growth mechanism and coagulation with larger particles is the dominant sink mechanism for ultrafine particles. In this work we found that the probability of a new ultrafine particle generating a CCN varies from 90% in different parts of the atmosphere, though in the boundary layer a large fraction of ultrafine particles have a probability between 5% and 40%. Some regions, such as the tropical free troposphere, are areas with high probabilities; however, variability within regions makes it difficult to predict which regions of the atmosphere are most efficient for generating CCN from ultrafine particles. For a given mass of primary ultrafine aerosol, an uncertainty of a factor of two in the modal diameter can lead to an uncertainty in the number of CCN generated as high as a factor for eight. It was found that no single moment of the primary aerosol size distribution, such as total mass or number, is a robust predictor of the number of CCN ultimately generated. Therefore, a complete description of the size distribution is generally required for global aerosol microphysics models.

Beschreibung: Long-range atmospheric transport to Svalbard has been studied with a compilation of 4 years of daily trajectories to determine how the atmospheric flow patterns influence the observed methane (CH4) at Mt. Zeppelin station (475 m.a.s.l.) in Ny-Ålesund (78°54' N, 11°53' E). The flow patterns were determined through cluster analysis of 5-day back-trajectories arriving at Ny-Ålesund twice a day (00:00 and 12:00 UTC) for the period 2000–2003. Eight cluster patterns were obtained and used in the analysis of the continuous methane measurements at Mt. Zeppelin station. The analysis shows a shift in frequencies eastward into the Arctic compared to identical studies of transport for 1992–2001. Higher concentrations of methane are mainly seen in clusters with transport from Europe and Russia in contrast to air following transport pathways within the Arctic Basin. The vertical motion of the trajectories has been investigated and shows that it has an effect on the methane concentration at the Mt. Zeppelin station. This is consistent with previous similar studies of CO2 and of other anthropogenic species. Seasonal variation in trajectory frequency can be seen, like for instance more trajectories from Europe and Siberia during winter, and short trajectories from the Arctic region in summer. The identified seasonal and indications of decadal shifts in transport pathways translate into shifts in source areas sampled by a single station. To determine shifts in regional source (and sink) strengths it is necessary to correct for transport pathway shifts when interpreting time series data.

Beschreibung: An intercomparison of three Fourier transform spectrometers (FTSs) with significantly different resolutions is presented. The highest-resolution instrument has a maximum optical path difference of 250 cm, and the two lower-resolution instruments have maximum optical path differences of 50 cm and 25 cm. The results indicate that the two lower-resolution instruments can retrieve total column amounts of O3, HCl, N2O and CH4 using the SFIT2 retrieval code with percent differences from the high-resolution instrument generally better than 3%, with respect to the high-resolution FTS. Total column amounts of the stratospheric species (O3 and HCl) have larger differences than those of the tropospheric species (N2O and CH4). Instrument line shape (ILS) information is found to be of critical importance when retrieving total columns of stratospheric gases from the lower-resolution instruments. Including the ILS information in the retrievals significantly reduces the difference in total column amounts between the three instruments. The remaining errors for stratospheric species total column amounts can be attributed to the lower sensitivity of the lower-resolution FTSs to the stratosphere.

Beschreibung: There is increasing evidence that there exist interstellar-terrestrial relations and that the heliosphere's effectivity to serve as a protecting shield for the Earth, specifically against cosmic rays, is varying in time. Nonetheless, a debate is going on whether, amongst other drivers, the Sun or the cosmic rays are influencing the terrestrial climate, particularly on periods of hundred years and shorter. As the modelling of the transport of cosmic rays in the heliosphere has evolved from pure test particle simulations to far more consistent treatments, one can explain various correlations within the framework of physical models and one can make quantitative predictions regarding terrestrial indicators of interstellar-terrestrial relations. This level of understanding and modelling allows to identify a criterion with which one can discriminate between solar and cosmic ray forcing on a period of several decades. We define such a criterion and discuss related existing observations.

Beschreibung: Because of its ubiquitous release on land and well-characterized atmospheric loss, radon-222 has been very useful for deducing fluxes of greenhouse gases such as CO2, CH4, and N2O. It is shown here that the radon-tracer method, used in previous studies to calculate regional-scale greenhouse gas fluxes, returns a weighted-average flux (the flux field F weighted by the sensitivity of the measurements to that flux field, f) rather than an evenly-weighted spatial average flux. A synthetic data study using a Lagrangian particle dispersion model and modeled CO2 fluxes suggests that the discrepancy between the sensitivity-weighted average flux and evenly-weighted spatial average flux can be significant in the case of CO2, due to covariance between F and f for biospheric CO2 fluxes during the growing season and also for anthropogenic CO2 fluxes in general. A technique is presented to correct the radon-tracer derived fluxes to yield an estimate of evenly-weighted spatial average CO2 fluxes. A new method is also introduced for correcting the CO2 flux estimates for the effects of radon-222 radioactive decay in the radon-tracer method.

Beschreibung: The role of the retention coefficient (i.e. the fraction of a dissolved trace gas which is retained in hydrometeors during freezing) for the scavenging and redistribution of highly soluble trace gases by deep convective cloud systems is investigated using a modified version of the Weather Research and Forecasting (WRF) model. Results from cloud system resolving model runs (in which deep convection is initiated by small random perturbations in association with so-called "large scale forcings (LSF)") for a tropical oceanic (TOGA COARE) and a mid-latitude continental case (ARM) are compared to two runs in which bubbles are used to initiate deep convection (STERAO, ARM). In the LSF runs scavenging is found to almost entirely prevent a highly soluble tracer initially located in the lowest 1.5 km of the troposphere from reaching the upper troposphere, independent of the retention coefficient. The release of gases from freezing hydrometeors leads to mixing ratio increases in the upper troposphere comparable to those calculated for insoluble trace gases only in runs in which bubbles are used to initiate deep convection. This result indicates that previous cloud resolving model studies using bubbles to initiate deep convection may possibly have over-estimated the influence of the retention coefficient on the vertical transport of highly soluble tracers. The retention coefficient is, however, found to play an important role for the scavenging and redistribution of highly soluble trace gases with a (chemical) source in the free troposphere and also for trace gases for which even relatively inefficient transport may be important.

Beschreibung: This paper gives an overview of the MIPAS Level 1B (L1B) processor whose main objective is to calibrate atmospheric measurements radiometrically, spectrally and geo-located. It presents also the results of instrument characterization done during the first years in-flight. MIPAS has shown very good performance and stability.

Beschreibung: We present the adjoint of the global chemical transport model GEOS-Chem, focusing on the chemical and thermodynamic relationships between sulfate – ammonium – nitrate aerosols and their gas-phase precursors. The adjoint model is constructed from a combination of manually and automatically derived discrete adjoint algorithms and numerical solutions to continuous adjoint equations. Explicit inclusion of the processes that govern secondary formation of inorganic aerosol is shown to afford efficient calculation of model sensitivities such as the dependence of sulfate and nitrate aerosol concentrations on emissions of SOx, NOx, and NH3. The adjoint model is extensively validated by comparing adjoint to finite difference sensitivities, which are shown to agree within acceptable tolerances; most sets of comparisons have a nearly 1:1 correlation and R2〉0.9. We explore the robustness of these results, noting how insufficient observations or nonlinearities in the advection routine can degrade the adjoint model performance. The potential for inverse modeling using the adjoint of GEOS-Chem is assessed in a data assimilation framework through a series of tests using simulated observations, demonstrating the feasibility of exploiting gas- and aerosol-phase measurements for optimizing emission inventories of aerosol precursors.

Beschreibung: Principal component analysis provides a fast and robust method to reduce the data dimensionality of an aerosol size distribution data set. Here we describe a methodology for applying principal component analysis to aerosol size distribution measurements. We illustrate the method by applying it to data obtained during five field studies. Most variations in the sub-micrometer aerosol size distribution over periods of weeks can be described using 5 components. Using 6 to 8 components preserves virtually all the information in the original data. A key aspect of our approach is the introduction of a new method to weight the data; this preserves the orthogonality of the components while taking the measurement uncertainties into account. We also describe a new method for identifying the approximate number of aerosol components needed to represent the measurement quantitatively. Applying Varimax rotation to the resultant components decomposes a distribution into independent monomodal distributions. Normalizing the components provides physical meaning to the component scores. The method is relatively simply, computationally fast, and numerically robust. The resulting data simplification provides an efficient method of representing complex data sets and should greatly assist in the analysis of size distribution data.

Beschreibung: We have estimated impacts of alternative aviation routings on the radiative forcing. Changes in ozone and OH have been estimated in four Chemistry Transport Models (CTMs) participating in the TRADEOFF project. Radiative forcings due to ozone and methane have been calculated accordingly. In addition radiative forcing due to CO2 is estimated based on fuel consumption. Three alternative routing cases are investigated; one scenario assuming additional polar routes and two scenarios assuming aircraft cruising at higher (+2000 ft) and lower (−6000 ft) altitudes. Results from the base case in year 2000 are included as a reference. Taking first a steady state backward looking approach, adding the changes in the forcing from ozone, CO2 and CH4, the ranges of the models used in this work are −0.8 to −1.8 and 0.3 to 0.6 m Wm−2 in the lower (−6000 ft) and higher (+2000 ft) cruise levels, respectively. In relative terms, flying 6000ft lower reduces the forcing by 5–10% compared to the current flight pattern, whereas flying higher, while saving fuel and presumably flying time, increases the forcing by about 2–3%. Taking next a forward looking approach we have estimated the integrated forcing (m Wm−2 yr) over 20 and 100 years time horizons. The relative contributions from each of the three climate gases are somewhat different from the backward looking approach. The differences are moderate adopting 100 year time horizon, whereas under the 20 year horizon CO2 naturally becomes less important relatively. Thus the forcing agents impact climate differently on various time scales. Also, we have found significant differences between the models for ozone and methane. We conclude that we are not yet at a point where we can include non-CO2 effects of aviation in emission trading schemes. Nevertheless, the rerouting cases that have been studied here yield relatively small changes in the radiative forcing due to the radiatively active gases.

Beschreibung: The Tropospheric ORganic CHemistry experiment (TORCH) took place during the heatwave of summer 2003 at Writtle College, a site 2 miles west of Chelmsford in Essex and 25 miles north east of London. The experiment was one of the most highly instrumented to date. A combination of a large number of days of simultaneous, collocated measurements, a consequent wealth of model constraints and a highly detailed chemical mechanism, allowed the atmospheric chemistry of this site to be studied in detail. The concentrations of the hydroxyl radical, the hydroperoxy radical and the sum of peroxy radicals, were measured between 25 July and 31 August using laser-induced fluorescence at low pressure and the peroxy radical chemical amplifier techniques. The concentrations of the radical species were predicted using a zero-dimensional box model based on the Master Chemical Mechanism version 3.1, which was constrained with the observed concentrations of relatively long-lived species. The model included a detailed parameterisation to account for heterogeneous loss of hydroperoxy radicals onto aerosol particles. Quantile-quantile plots were used to assess the model performance in respect of the measured radical concentrations. On average, measured hydroxyl radical concentrations were over-predicted by 24%. Modelled and measured hydroperoxy radical concentrations agreed very well, with the model over-predicting on average by only 7%. The sum of peroxy radicals was under-predicted when compared with the respective measurements by 22%. OH initiation was dominated by the reactions of excited oxygen atoms with water, nitrous acid photolysis and the ozone reaction with alkene species. Photolysis of aldehyde species was the main initiation route for HO2 and RO2. Termination, under all conditions, primarily involved reactions with NOx for OH and heterogeneous chemistry on aerosol surfaces for HO2. The OH chain length varied between 2 and 8 cycles, the longer chain lengths occurring before and after the most polluted part of the campaign. Peak local ozone production of 17 ppb hr−1 occurred on 3 and 5 August, signifying the importance of local chemical processes to ozone production on these days. On the whole, agreement between model and measured radicals is good, giving confidence that our understanding of atmospheres influenced by nearby urban sources is adequate.

Beschreibung: New atmospheric particles with diameters of 3–10 nm and their subsequent growth to cloud condensation nucleus have been observed at various places in the European boundary layer. These events have been observed simultaneously within wide geographical areas (over 1000 km) in connection to specific weather systems, the cold air behind cyclones. Here we show that atmospheric aerosol formation (i.e. nucleation and initial growth) is favoured by the outbreak of cold Arctic air over northern Europe. Aerosol formation was about twice as common in Arctic air as in sub-Polar air, and even more so compared to other air masses. The most important general factor favouring aerosol formation in Arctic air and marine air was weaker competing condensational sink (CS) for the precursor gases (less pre-existing aerosols), while high CS prevented aerosol formation in heated sub-Polar air and mid-latitude air. High SO2 levels favoured nucleation in continental air and high UV-B radiation in sub-tropical air. The critical factor that determined if aerosol formation would start on a day with Arctic air was the UV-B radiation. The same applied to sub-Polar air and continental air, while increased SO2 concentration could trigger formation in heated sub-Polar and mid-latitude air, and reduced CS could cause formation in mid-latitude, marine or mixed/transient air. We speculate that strong emissions of volatile organic compounds from the Boreal forest and strong boundary layer dynamics may have caused aerosol formation in sub-Polar air masses and air in transition from a marine to a continental character. The monthly frequency of Arctic air masses and the probability for photo-chemically driven aerosol formation explains the observed annual cycle in monthly particle formation frequency as well as much of the inter annual variability. The same cyclones that transport cold, clean air from the Arctic to Europe will also transport warm polluted air in the other direction, which help cause the Arctic Haze phenomena. The cyclones have a key role for the atmospheric aerosol life cycle in mid to high latitudes. Due to the observed growth to the size of CCN in one to two days, there is a potential feed back from the effects on the CCN population and cloud albedo even within the same weather system, but also on the climatic time scale.

Beschreibung: It is important to obtain the year-to-year trend of stratospheric minor species in the context of global changes. An important example is the trend in global ozone depletion. The purpose of this paper is to report the accuracy and precision of measurements of stratospheric chemical species that are made at our Poker Flat site in Alaska (65° N, 147° W). Since 1999, minor atmospheric molecules have been observed using a Fourier-Transform solar-absorption infrared Spectrometer (FTS) at Poker Flat. Vertical profiles of the abundances of ozone, HNO3, HCl, and HF for the period from 2001 to 2003 were retrieved from the FTS spectra by using Rodgers' formulation of the Optimal Estimation Method (OEM). The accuracy and precision of the retrievals were estimated by formal error analysis. Errors for the total column were estimated to be 5.3%, 3.4%, 5.9%, and 5.3% for ozone, HNO3, HCl, and HF, respectively. The ozone vertical profiles were in good agreement with profiles derived from collocated ozonesonde measurements that were smoothed with averaging kernel functions that had been obtained with the retrieval procedure used in the analysis of spectra from the ground-based FTS (gb-FTS). The O3, HCl, and HF columns that were retrieved from the FTS measurements were consistent with Earth Probe/Total Ozone Mapping Spectrometer (TOMS) and HALogen Occultation Experiment (HALOE) data over Alaska within the error limits of all the respective datasets. This is the first report from the Poker Flat FTS observation site on a number of stratospheric gas profiles including a comprehensive error analysis.

Beschreibung: The volatility of sub-micrometer atmospheric aerosol particles was studied in a rural background environment in Finland using a combination of a heating tube and a scanning mobility particle sizer. The analysis focused on nano-particles formed from nucleation bursts which were subsequently observed during their growth in the diameter range between 5 and 60 nm. During the 6 days of new particle formation shown in detail, the concentrations of newly formed particles increased up to 10 000 cm−3. The number of nucleation mode particles measured after volatilization in the heating tube at 280°C was up to 90% of the total number under ambient conditions. Taking into account the absolute accuracy of the size distribution measurements, all ambient particles found in the rural atmosphere could have a non-volatile core after volatilization at 280°C. As the regional new particle formation events developed over time as a result of further vapor condensation, the newly formed particles grew at an average growth rate of 2.4±0.3 nm h−1. Importantly, the non-volatile cores of nucleation mode particles were also observed to grow over time, however, at a lower average growth rate of 0.6±0.3 nm h−1. One implication of the volatility analysis is that the newly formed particles, which have reached ambient diameters of 15 nm, are unlikely to consist of sulfuric acid, ammonium sulfate, and water alone. A relatively constant ratio between the growth rate of the ambient particles as well as their non-volatile cores indicates that non-volatile matter is formed only gradually in the growing particles. The non-volatile fraction of the particles showed some correlation with the ambient temperature. The composition and formation mechanism of this non-volatile material in nucleation mode particles are, to date, not known.

Beschreibung: The temperature dependence of secondary organic aerosol (SOA) formation from ozonolysis of β-pinene was studied in a flow reactor at 263–303 K and 1007 hPa. The observed SOA yields were of similar magnitude as predicted by a two-product model based on detailed gas phase chemistry (Jenkin, 2004), reaching maximum values of 0.22–0.39 at high particle mass concentrations. However, the measurement data exhibited significant deviations (up to 50%) from the predicted linear dependence on inverse temperature. When fitting the measurement data with a two-product model, we found that both the partitioning coefficients (Kom,i) and the stoichiometric yields (αi) of the low-volatile and semi-volatile species vary with temperature. The results indicate that not only the reaction product vapour pressures but also the relative contributions of different gas-phase or multiphase reaction channels are dependent on temperature. We suggest that the modelling of secondary organic aerosol formation in the atmosphere needs to take into account the effects of temperature on the pathways and kinetics of the involved chemical reactions as well as on the gas-particle partitioning of the reaction products.

Beschreibung: Absolute principal component analysis can be applied, with suitable modifications, to atmospheric aerosol size distribution measurements. This method quickly and conveniently reduces the dimensionality of a data set. The resulting representation of the data is much simpler, but preserves virtually all the information present in the original measurements. Here we demonstrate how to combine the simplified size distribution data with trace gas measurements and meteorological data to determine the origins of the measured particulate matter using absolute principal component analysis. We have applied the analysis to four different sets of field measurements that were conducted at three sites in southern Ontario. Several common factors were observed at all the sites; these were identified as photochemically produced secondary aerosol particles, regional pollutants (including accumulation mode aerosol particles), and trace gas variations associated with boundary layer dynamics. Each site also exhibited a factor associated specifically with that site: local industrial emissions in Hamilton (urban site), processed nucleation mode particles at Simcoe (polluted rural site), and transported fine particles at Egbert (downwind from Toronto).

Beschreibung: Boundary layer concenrations of several volatile organic compounds (VOC) were measured during two campaigns in springs of 2003 and 2006. Measurements were conducted over boreal forests near SMEAR II measurement station in Hyytiälä, Southern Finland. In 2003 the measuremens were performed using light aircraft and in 2006 using hot air ballon. Isoprene concentrarions were low, usually below detection limit. This is explained by low biogenic production due to cold weather. Monoterpenes were observed frequently. Average total monoterpene concentration in the boundary layer was 33 pptv. Many anthropogenic compounds e.g. benzene, xylene and toluene, were observed in high amounts. Ecosystem scale surface emissions were estimated using simple mixed box budget methodology. Total monoterpene fluxes varied up to 80 μg m−2 h−1, α-pinene contributing typically more than two thirds of that. Highest fluxes of anthropogenic compounds were those of p/m xylene.

Beschreibung: The performance of a new chemical ionization reaction time-of-flight mass spectrometer (CIR-TOF-MS) utilising the environment chamber SAPHIR (Simulation of Atmospheric Photochemistry In a large Reaction Chamber – Forschungzentrum Jülich, Germany) is described. The work took place as part of the ACCENT (Atmospheric Composition and Change the European NeTwork for excellence) supported oxygenated volatile organic compound (OVOC) measurement intercomparison during January 2005. The experiment entailed the measurement of 14 different atmospherically significant OVOCs at various mixing ratios in the approximate range 10.0–0.6 ppbV. The CIR-TOF-MS operated throughout the exercise with the hydronium ion (H3O+) as the primary chemical ionization (CI) reagent in order to facilitate proton transfer to the analyte OVOCs. The results show the CIR time-of-flight mass spectrometer is capable of detecting a wide range of atmospheric OVOCs down to sub-ppbV mixing ratios with high accuracy and precision. It is demonstrated that the technique has rapid multi-channel response at the required sensitivity, accuracy and precision for atmospheric OVOC measurements.

Beschreibung: A fire storm that occured on 28 May 2001 devastated the town of Chisholm, ~150 km north of Edmonton, Alberta, induced a violent fire-invigorated cumulonimbus cloud. This pyro-cumulonimbus (pyro-Cb) had overshooting tops of 2.5–3 km above the tropopause, and injected massive amounts of smoke into the lower stratosphere. Fortunately, this event occurred under good coverage of radar, rain gauge, lightning and satellite measurements, which allowed in-depth documentation of the event. The combination of heat and smoke created a cloud with extremely small drops, which ascended rapidly in violent updrafts. There appeared to be little freezing up to the homogeneous freezing isotherm level of –38°C. A cloud with such small and short-lived highly supercooled drops is incapable of producing precipitation except for few large graupel and hail, which produced the observed radar echoes and charged the cloud with positive lightning. The small cloud drops froze homogeneously to equally small ice particles, for which there is no mechanism to aggregate into precipitation particles that hence remain in the anvil. The small precipitation efficiency implies that only a small fraction of the smoke is scavenged, so that most of it is exhausted through the anvil to the upper troposphere and lower stratosphere. Comparisons with other cases suggest that a pyro-Cb does not have to be as violent as the Chisholm case to have strongly suppressed precipitation. However, this level of convective vigor is necessary to create the overshooting updraft that injects the smoke into the lower stratosphere.

Beschreibung: The results of a comparison exercise of radiative transfer models (RTM) of various international research groups for Multiple AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) viewing geometry are presented. In contrast to previous comparison exercises, box-air-mass-factors (box-AMFs) for various atmospheric height layers were modelled, which describe the sensitivity of the measurements as a function of altitude. In addition, radiances were calculated allowing the identification of potential errors, which might be overlooked if only AMFs are compared. Accurate modelling of radiances is also a prerequisite for the correct interpretation of satellite observations, for which the received radiance can strongly vary across the large ground pixels, and might be also important for the retrieval of aerosol properties as a future application of MAX-DOAS. The comparison exercises included different wavelengths and atmospheric scenarios (with and without aerosols). The results were systematically investigated with respect to their dependence on the telescope's elevation angle and the azimuth angle. For both dependencies, a strong and systematic influence of aerosol scattering was found indicating that from MAX-DOAS observations also information on atmospheric aerosols can be retrieved. During the various iterations of the exercises, the results from all models showed a substantial convergence, and the final data sets agreed for most cases within about 5%. Larger deviations were found for cases with low atmospheric optical depth, for which the photon path lengths along the line of sight of the instrument can become very large. The differences occurred between models including full spherical geometry and those using only plane parallel approximation indicating that the correct treatment of the Earth's sphericity becomes indispensable. The modelled box-AMFs constitute an universal data base for the calculation of arbitrary (total) AMFs by simple convolution with a given trace gas concentration profile. Together with the modelled radiances and the specified settings for the various exercises, they can serve as test cases for future RTM developments.

Beschreibung: Odin-SMR is a limb-sounder operating in the 500 region with the capability of performing measurements down to altitudes of about 10 with relatively low influence of ice clouds. Until now spectra from tropospheric tangent altitudes have been disregarded due to inadequate handling of scattering. A first method to extract upper tropospheric quantities has now been developed, yielding the humidity in two layers around 200 and 130 and information on cloud ice content above 200. The main concern for these retrievals is the calibration performance. A careful analysis indicates a systematic calibration error of about 1 K, but also a random component that differs between the two bands. The random calibration uncertainty results in retrieval errors of 10–60% depending on humidity and band. Presently this prohibits use of single retrievals, but averages can be presented with good accuracy. The fixed calibration error can largely be removed, leaving the spectroscopic uncertainties to dominate the humidity retrieval accuracy, estimated to be around 20%. First results are presented that are in agreement with seasonal structure obtained from other satellite measurements. An encouraging comparison between MOZAIC data and measurements for the 200 layer gives further confidence in the capability of Odin-SMR to measure humidity in the upper tropical troposphere.

Beschreibung: We present the first detailed microphysical simulations which are performed online within the framework of a global 3-D chemical transport model (CTM) with full chemistry. The model describes the formation and evolution of four types of polar stratospheric cloud (PSC) particles. Aerosol freezing and other relevant microphysical processes are treated in a full explicit way. Each particle type is described by a binned size distribution for the number density and chemical composition. This set-up allows for an accurate treatment of sedimentation and for detailed calculation of surface area densities and optical properties. Simulations are presented for the Antarctic winter of 2003 and comparisons are made to a diverse set of satellite observations (optical and chemical measurements of POAM III and MIPAS) to illustrate the capabilities of the model. This study shows that a combined resolution approach where microphysical processes are simulated in coarse-grained conditions gives good results for PSC formation and its large-scale effect on the chemical environment through processes such as denitrification, dehydration and ozone loss. It is also shown that the influence of microphysical parameters can be measured directly from these processes.

Beschreibung: We report in situ and remote observations proving occasional occurrence of solid particles in the tropical lowest stratosphere, far away from deep convective events. The particles were found during field campaigns in Southeast Brazil (49.03 W 22.36 S). They occur in the altitude range from 17.5 to 20.8 km, at temperatures up to at least 10 K above the expected frost point temperature. While stability of ice particles at these altitudes is unexpected from a theoretical point of view, it is argued that these observations are indications of tropospheric air masses penetrating into the stratosphere during convective overshoots. It is concluded that the intrusion of tropospheric air must have carried a large amount of water with it, which effectively hydrated the lowest stratosphere, and consequently suppressed sublimation. This conclusion is further supported by a separate water vapor mixing ratio profile obtained at the same observation site.

Beschreibung: More than three years of measurements of aerosol size-distribution and different gas and meteorological parameters made in Po Valley, Italy were analysed for this study to examine which of the meteorological and trace gas variables effect on the emergence of nucleation events. As the analysis method, we used discriminant analysis with non-parametric Epanechnikov kernel, included in non-parametric density estimation method. The best classification result in our data was reached with the combination of relative humidity, ozone concentration and a third degree polynomial of radiation. RH appeared to have a preventing effect on the new particle formation whereas the effects of O3 and radiation were more conductive. The concentration of SO2 and NO2 also appeared to have significant effect on the emergence of nucleation events but because of the great amount of missing observations, we had to exclude them from the final analysis.

Beschreibung: Aerosol spectral measurements by sunphotometers can be characterized by three independent pieces of information: 1) the optical thickness (AOT), a measure of the column aerosol concentration, 2) the optical thickness average spectral dependence, given by the Angstrom exponent (α), and 3) the spectral curvature of α (δα). We propose a simple graphical method to visually convert (α, δα) to the contribution of fine aerosol to the AOT and the size of the fine aerosols. This information can be used to track mixtures of pollution aerosol with dust, to distinguish aerosol growth from cloud contamination and to observe aerosol humidification. The graphical method is applied to the analysis of yearly records at 8 sites in 3 continents, characterized by different levels of pollution, biomass burning and mineral dust concentrations. Results depict the dominance of fine mode aerosols in driving the AOT at polluted sites. In stable meteorological conditions, we see an increase in the size of the fine aerosol as the pollution stagnates and increases in optical thickness. Coexistence of coarse and fine particles is evidenced at the polluted sites downwind of arid regions.

Beschreibung: The properties of atmospheric aerosol particles in Marseille and Athens were investigated. The studies were performed in Marseille, France during July 2002 and in Athens Greece during June 2003. The aerosol size distribution and the formation and growth rates of newly formed particles were characterized using Differential Mobility Particle Sizers. Hygroscopic properties were observed using a Hygroscopic Tandem Differential Mobility Analyzer setup. During both campaigns, the observations were performed at suburban, almost rural sites, and the sites can be considered to show general regional background behavior depending on the wind direction. At both sites there were clear pattern for both aerosol number concentration and hygroscopic properties. Nucleation mode number concentration increased during the morning hours indicating new particle formation, which was observed during more than 30% of the days. The observed formation rate was typically more than 1 cm−3 s−1, and the growth rate was between 1.2–9.9 nm h−1. Based on hygroscopicity measurements in Athens, the nucleation mode size increase was due to condensation of both water insoluble and water soluble material. However, during a period of less anthropogenic influence, the growth was to a larger extent due to water insoluble components. When urban pollution was more pronounced, growth due to condensation of water soluble material dominated.

Beschreibung: A statistical synthesis of marine aerosol measurements from experiments in four different oceans is used to evaluate a global aerosol microphysics model (GLOMAP). We compare the model against observed size resolved particle concentrations, probability distributions, and the temporal persistence of different size particles. We attempt to explain the observed size distributions in terms of sulfate and sea spray and quantify the possible contributions of anthropogenic sulfate and carbonaceous material to the number and mass distribution. The model predicts a bimodal size distribution that agrees well with observations as a grand average over all regions, but there are large regional differences. Notably, observed Aitken mode number concentrations are more than a factor 10 higher than in the model for the N Atlantic but a factor 7 lower than the model in the NW Pacific. We also find that modelled Aitken mode and accumulation mode geometric mean diameters are generally smaller in the model by 10–30%. Comparison with observed free tropospheric Aitken mode distributions suggests that the model underpredicts growth of these particles during descent to the MBL. Recent observations of a substantial organic component of free tropospheric aerosol could explain this discrepancy. We find that anthropogenic continental material makes a substantial contribution to N Atlantic marine boundary layer (MBL) aerosol, with typically 60–90% of sulfate across the particle size range coming from anthropogenic sources, even if we analyse air that has spent an average of 〉120 h away from land. However, anthropogenic primary black carbon and organic carbon particles do not explain the large discrepancies in Aitken mode number. Several explanations for the discrepancy are suggested. The lack of lower atmospheric particle formation in the model may explain low N Atlantic particle concentrations. However, the observed and modelled particle persistence at Cape Grim in the Southern Ocean, does not reveal a diurnal cycle consistent with a photochemically driven local particle source. We also show that a physically based cloud drop activation scheme is needed to explain the observed change in accumulation mode geometric mean diameter with particle number.

Beschreibung: In this study, we evaluate the ability of the BRAMS mesoscale model compared to ECMWF global analysis to simulate the observed vertical variations of water vapour in the tropical upper troposphere and lower stratosphere (UTLS). The observations are balloon-borne measurements of water vapour mixing ratio and temperature from micro-SDLA (Tunable Diode Laser Spectrometer) instrument. Data from two balloon flights performed during the 2004 HIBISCUS field campaign are used to compare with the mesoscale simulations and to ECMWF analysis. The mesoscale model performs significantly better than ECMWF analysis for water vapour in the upper troposphere and similarly or slightly worse for temperature. The improvement provided by the mesoscale model for water vapour comes mainly from (i) the enhanced vertical resolution in the UTLS (250 m for BRAMS and ~1 km for ECMWF model) and (ii) the more detailed microphysical parameterization providing ice supersaturations as in the observations. The ECMWF vertical resolution (~1 km) is too coarse to capture the observed fine scale vertical variations of water vapour in the UTLS. In near saturated or supersaturated layers, the mesoscale model relative humidity with respect to ice saturation is close to observations provided that the temperature profile is realistic. For temperature, ECMWF analysis gives good results partly thanks to data assimilation. The analysis of the mesoscale model results showed that in undersaturated layers, the water vapour profile depends mainly on the dynamics. In saturated/supersaturated layers, microphysical processes play an important role and have to be taken into account on top of the dynamical processes to understand the water vapour profiles. In the lower stratosphere, the ECMWF model and the BRAMS model give very similar water vapour profiles that are significantly dryer than micro-SDLA measurements. This similarity comes from the fact that BRAMS is initialised using ECMWF analysis and that no mesoscale process acts in the stratosphere leading to no modification of the BRAMS results with respect to ECMWF analysis.

Beschreibung: We present a simple method to perform degradation correction to Global Ozone Monitoring Experiment (GOME) reflectance spectra by comparing the average reflectance for 60° N–60° S with that at the beginning of GOME observations after removing the dependences on solar zenith angle and seasonal variation. The results indicate positive degradation of up to ~15–25% in the wavelength range 289–370 nm during 2000–2002; the degradation also exhibits significant dependence on wavelength and view zenith angle. These results are consistent with previous studies using radiative transfer models and ozone observations or climatology. The degradation causes retrieval biases of up to ~3% (10 DU, 1 DU=2.69×1016 molecules cm−2), 30% (10 DU), 10%, and 40% in total column ozone, tropospheric column ozone, stratospheric ozone and tropospheric ozone, respectively, from our GOME ozone profile retrieval algorithm. The application of this degradation correction generally improves the retrievals relative to Dobson and ozonesonde measurements during 2000–2003 and improves the retrieval consistency during 1996–2003.

Beschreibung: The authors introduce the radiative transfer model CLOUD for reflection, transmission, and absorption characteristics of terrestrial clouds and discuss the accuracy of the approximations used within the model. A Fortran implementation of CLOUD is available for download. This model is fast, accurate, and capable of calculating multiple raditiative transfer characteristics of cloudy media including the spherical and plane albedo, reflection and transmission functions, absorptance as well as global and diffuse transmittance. The approximations are based on the asymptotic solutions of the radiative transfer equations. While the analytic part of the solutions is treated in the code in an approximate way, the correspondent reflection function (RF) of a semi-infinite water cloud R∞ is calculated using numerical solutions of the radiative transfer equations in the assumption of Deirmendjian's cloud C1 model. In the case of ice clouds, the fractal ice crystal model is used. The resulting values of R∞ with respect to the viewing geometry are stored in a look-up table (LUT).

Beschreibung: The Lagrangian transport model COMET has been developed to evaluate emission estimates based on atmospheric concentration observations. This paper describes the model and its application in modelling the methane concentrations at the European stations Cabauw and Macehead. The COMET model captures in most cases both synoptic and diurnal variations of the concentrations as a function of time and in absolute size quite well. The explained variability by COMET of the mixed layer concentration for Cabauw varies from 50% to 84%; for all hourly observations in 2002 the explained variability is 71% with a RMSE of 112 ppb. The explained variability for Macehead is 48%. The most important model parameters were tested for their influence on model performance, but in general the model is not very sensitive to variations within acceptable limits. For a regionally and locally polluted continental site the COMET model shows only a small bias and a moderate random error, and therefore is considered to capture the influence of the sources on the concentration variations quite well. It is therefore concluded that inverse methods and more specifically the COMET model is suitable to be applied in deriving independent estimates of greenhouse gas emissions using Source-Receptor relationships.

Beschreibung: A light aircraft was equipped with a bank of Condensation Particle Counters (CPCs) (50% cut from 3–5.4–9.6 nm) and a nano-Scanning Mobility Particle Sizer (nSMPS) and deployed along the west coast of Ireland, in the vicinity of Mace Head. The objective of the exercise was to provide high resolution micro-physical measurements of the coastal nucleation mode in order to map the spatial extent of new particle production regions and to evaluate the evolution, and associated growth rates of the coastal nucleation-mode aerosol plume. Results indicate that coastal new particle production is occurring over most areas along the land-sea interface with peak concentrations at the coastal plume-head in excess of 106 cm−3. Pseudo-Lagrangian studies of the coastal plume evolution illustrated significant growth of new particles to sizes in excess of 8 nm approximately 10 km downwind of the source region. Close to the plume head (

Beschreibung: MonteCarlo simulations have been performed to evaluate the importance of multiple scattering effects in co- and cross-polar radar returns for 94GHz radars in Cloudsat and airborne configurations. Thousands of vertically structured profiles derived from some different cloud resolving models are used as a test-bed. Mie theory is used to derive the single scattering properties of the atmospheric hydrometeors. Multiple scattering effects in the cross polar channel (reflectivity enhancement) are particularly elusive, especially in airborne configuration. They can be quite consistent in satellite configurations, like Cloudsat, especially in regions of high attenuation and in the presence of highly forward scattering layers associated with snow and graupel particles. When the cross polar returns are analysed, high LDR values appear both in space and in airborne configurations. The LDR signatures are footprints of multiple scattering effects since they cannot be explained by single scattering computations, even including non-spherical particles. We see these signatures confirmed by some experimental data collected during the Wakasa Bay experiment. Multiple scattering effects can be important for Clousat applications like rainfall and snowfall retrievals since single scattering based algorithms will be otherwise burdened by positive biases.

Beschreibung: Contrary to tropospheric CO2 whose oxygen isotopic composition follows a standard mass dependent relationship, i.e. δ17O~0.5 δ18O, stratospheric CO2 is preferentially enriched in 17O, leading to a strikingly different relation with δ17O~1.7δ18O. The isotope anomaly is likely inherited from O3 via photolytically produced O(1D) that undergoes isotope exchange with CO2 and the anomaly may well serve as a tracer of stratospheric chemistry if details of the exchange mechanism are understood. We have studied the photochemical isotope equilibrium in UV-irradiated O2-CO2 and O3-CO2 mixtures to quantify the transfer of the anomaly from O3 to CO2 at room temperature. By following the time evolution of the oxygen isotopic compositions of CO2 and O2 under varying initial isotopic compositions of both, O2/O3 and CO2, the isotope equilibria between the two reservoirs were determined. A very strong dependence of the isotope equilibrium on the O2/CO2-ratio was established. Equilibrium enrichments of 17O and 18O in CO2 relative to O2 diminish with increasing CO2 content, and this reduction in the equilibrium enrichments does not follow a standard mass dependent relation. When molecular oxygen exceeds the amount of CO2 by a factor of about 20, 17O and 18O in equilibrated CO2 are enriched by (142±4) and (146±4), respectively, at room temperature and at a pressure of 225 hPa, independent of the initial isotopic compositions of CO2 and O2 or O3. From these findings we derive a simple and general relation between the starting isotopic compositions and amounts of O2 and CO2 and the observed slope in a three oxygen isotope diagram. Predictions from this relation are compared with published laboratory and atmospheric data.

Beschreibung: Night-time chemistry in the Marine Boundary Layer has been modelled using a number of observationally constrained zero-dimensional box-models. The models were based upon the Master Chemical Mechanism (MCM) and the measurements were taken during the North Atlantic Marine Boundary Layer Experiment (NAMBLEX) campaign at Mace Head, Ireland in July–September 2002. The model could reproduce, within the combined uncertainties, the measured concentration of HO2 (within 30–40%) during the night 31 August–1 September and of HO2+RO2 (within 15–30%) during several nights of the campaign. The model always overestimated the NO3 measurements made by Differential Optical Absorption Spectroscopy (DOAS) by up to an order of magnitude or more, but agreed with the NO3 Cavity Ring-Down Spectroscopy (CRDS) measurements to within 30–50%. The most likely explanation of the discrepancy between the two instruments and the model is reaction of the nitrate radical with inhomogeneously distributed NO, which was measured at concentrations of up to 10 ppt, even though this is not enough to fully explain the difference between the DOAS measurements and the model. A rate of production and destruction analysis showed that radicals were generated during the night mainly by the reaction of ozone with light alkenes. The cycling between HO2/RO2 and OH was maintained during the night by the low concentrations of NO and the overall radical concentration was limited by slow loss of peroxy radicals to form peroxides. A strong peak in [NO2] during the night 31 August–1 September allowed an insight into the radical fluxes and the connections between the HOx and the NO3 cycles.

Beschreibung: In this study, we investigate the aerosol optical properties, namely aerosol optical thickness (AOT), Angström parameter (α440–870 and size distribution parameters over the Eastern Mediterranean Basin, using spectral measurements from the recently established FORTH (Foundation for Research and Technology-Hellas) AERONET station in Crete, for the two-year period 2003–2004. The location of the FORTH-AERONET station offers a unique opportunity to monitor aerosols from different sources. The AOT is maximum during spring, because of the high dust load transported mainly from African deserts, and minimum in winter. There are secondary maxima in AOT at 870 and 1020 nm in October, attributed to dust transport events occurring in autumn. Large values of AOT at 340 and 500 nm persisting during summer are associated with transport of fine aerosols of urban/industrial and biomass burning origin. The dust events are characterised by a drastic increase in AOT at all wavelengths accompanied by a drastic decrease in Angström parameter to values below 0.3. The mean annual values of AOT340, AOT500, AOT870 and α440–870, are equal to 0.34±0.14, 0.21±0.11, 0.11±0.09 and 1.17±0.53 respectively. The scatterplots of Angström parameter versus aerosol optical thickness indicate a great variety of aerosol types over the study region including dust, urban-industrial/biomass burning, maritime, as well as mixed aerosol types. This is supported by back-trajectory analyses, and agrees with the measurements of experimental campaigns that took place in Crete during summer. The aerosol volume-size distributions are bimodal over all seasons, with a fine and a coarse mode having effective mean radius of 0.13 μm and 2.12 μm, respectively, and columnar volume concentrations of about 0.038 and 0.061 μm3/μm2. There is a general dominance of coarse to fine mode in terms of aerosol volume, in agreement with other maritime locations persisting through the year except for summer. Our analysis shows that the highest values of AOT are related to wind directions from the east, southeast and south, as well as from northwest. Northwestern winds are associated with maximum fine aerosol loads from industrial areas, while eastern, southeastern and southern winds are related to maximum coarse aerosol loads, namely sea salt and desert dust.

Beschreibung: Atmosphere and Ocean General Circulation Model (AOGCM) experiments for the Intergovernmental Panel on Climate Change Fourth Assessment Report are analyzed using both 20th and 21st century model output to better understand model variability and assess the importance of various forcing mechanisms on stratospheric trends. While models represent the climatology of the stratosphere reasonably well in comparison with NCEP reanalysis, there are biases and large variability among models. In general, AOGCMs are cooler than NCEP throughout the stratosphere, with the largest differences in the tropics. Around half the AOGCMs have a top level beneath ~2 hPa and show a significant cold bias in their upper levels (~10 hPa) compared to NCEP, suggesting that these models may have compromised simulations near 10 hPa due to a low model top or insufficient stratospheric levels. In the lower stratosphere (50 hPa), the temperature variability associated with large volcanic eruptions is either absent (in about half of the models) or the warming is overestimated in the models that do include volcanic aerosols. There is general agreement on the vertical structure of temperature trends over the last few decades, differences between models are explained by the inclusion of different forcing mechanisms, such as stratospheric ozone depletion and volcanic aerosols. However, even when human and natural forcing agents are included in the simulations, significant differences remain between observations and model trends, particularly in the upper tropical troposphere (200 hPa–100 hPa), where, since 1979, models show a warming trend and the observations a cooling trend.

Beschreibung: Radiosonde temperature profiles from Belgrano (78° S) and other Antarctic stations have been compared with European Centre for Medium-Range Weather Forecasts (ECMWF) data during the winter of 2003. Results show a bias in the operational model which is height and temperature dependent, being too cold at layers peaking at 80 and 25–30 hPa, and hence resulting in an overestimation of the predicted potential PSC areas. Here we show the results of the comparison by considering the possibility of a bias in the sondes at extremely low temperatures and discuss the potential implications that this bias might have on the ozone depletion computed by Climate Transport Model based on ECMWF temperature fields.

Beschreibung: First results of a multiannual integration with the new global aerosol model system ECHAM4/MADE are presented. This model system enables explicit simulations of the particle number concentration and size-distribution, which is a fundamental innovation compared to previous global model studies considering aerosol mass cycles only. The data calculated by the model provide detailed insights into the properties of the global submicrometer aerosol regarding global burden, chemical composition, atmospheric lifetime, particle number concentration and aerosol size-distribution. The model takes into account sulfate (SO4), nitrate (NO3), ammonium (NH4), black carbon (BC), organic matter (OM), mineral dust, sea salt and aerosol water. The simulated climatological annual mean global atmospheric burdens (lifetime) of the dominant submicrometer aerosol components are 2.25 Tg (4.5 d) for SO4, 0.46 Tg (4.5 d) for NH4, 0.26 Tg (5.6 d) for BC, and 1.77 Tg (6.5 d) for OM. The contributions of individual processes such as emission, nucleation, condensation or dry and wet deposition to the global sources and sinks of a specific aerosol component and particle number concentration are quantified. Based on this analysis, the significance of aerosol dynamical processes (nucleation, condensation, coagulation) is evaluated by comparison to the importance of other processes relevant for the submicrometer aerosol on the global scale. The results reveal that aerosol dynamics are essential for the simulation of the particle number concentration and important but not vital for the simulation of particle mass concentration. Hence aerosol dynamics should be taken into account in simulations of atmospheric processes showing a significant dependence on aerosol particle number concentration.

Beschreibung: Consecutive reactions of adducts, resulting from OH radicals and aromatics, with the tropospheric scavenger molecules O2, NO and NO2 have been studied for benzene, toluene, m- and p-xylene, hexamethylbenzene, phenol, m-cresol and aniline by observing decays of OH at temperatures where the thermal back-decomposition to OH is faster than 3 s−1, typically between 300 and 340 K. The experimental technique was resonance fluorescence with flash photolysis of water as source of OH. Biexponential decays were observed in the presence of either O2 or NO, and triexponential decays were obtained in the presence of NO2. The kinetic analysis was performed by fitting the relevant rate constants of the reaction mechanism to whole sets of decays obtained at various concentrations of aromatic and scavenger. In the case of hexamethylbenzene, the biexponential decays suggest the existence of the ipso-adduct, and the slightly higher necessary temperatures show that it is even more stable. In addition, smog chamber experiments at O2 concentrations from atmospheric composition down to well below 100 ppm have been carried out for benzene, toluene and p-xylene. The drop of the effective rate constant of removal by OH occurs at reasonable O2 levels, given the FP/RF results. Comparison of the adduct reactivities shows for all aromatics of this study that the reaction with O2 predominates over that with NO2 under all tropospheric conditions, and that a reaction with NO may only occur after the reaction with O2.

Beschreibung: Eight super-pressure balloons floating at constant level between 50 and 80 hPa and three Infra-Red Montgolfier balloons of variable altitude (15 hPa daytime, 40–80 hPa night time) have been launched at 22° S from Brazil in February–May 2004 in the frame of the HIBISCUS project. The flights lasted for 7 to 79 days residing mainly in the tropics, but some of them passed the tropical barrier and went to southern midlatitudes. Compared to the balloon measurements just above the tropical tropopause the ECMWF operational temperatures show a systematic cold bias of 0.9 K and the easterly zonal winds are too strong by 0.7 m/s. This bias in the zonal wind adds to the ECMWF trajectory errors, but they still are relatively small with e.g. about an error of 700 km after 5 days. The NCEP/NCAR reanalysis trajectory errors are substantially larger (1300 km after 5 days). In the southern midlatitudes the cold bias is the same, but the zonal wind bias is almost zero. The trajectories are generally more accurate than in the tropics, but for one balloon a lot of the calculated trajectories end up on the wrong side of the tropical barrier and this leads to large trajectory errors.