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: Volcanoes represent an important natural source of several trace elements to the atmosphere. For some species (e.g., As, Cd, Pb and Se) they may be the main natural source and thereby strongly influencing geochemical cycles from the local to the global scale. Mount Etna is one of the most actively degassing volcanoes in the world, and it is considered to be, on the long-term average, the major atmospheric point source of many environmental harmful compounds. Their emission occurs either through continuous passive degassing from open-conduit activity or through sporadic paroxysmal eruptive activity, in the form of gases, aerosols or particulate. To estimate the environmental impact of magma-derived trace metals and their depositions processes, rainwater and snow samples were collected at Mount Etna area. Five bulk collectors have been deployed at various altitudes on the upper flanks around the summit craters of the volcano; samples were collected every two week for a period of one year and analyzed for the main chemical-physical parameters (electric conductivity and pH) and for major and trace elements concentrations. Chemical analysis of rainwater clearly shows that the volcanic contribution is always prevailing in the sampling site closest to the summit crater (about 1.5 km). In the distal sites (5.5-10 km from the summit) and downwind of the summit craters, the volcanic contribution is also detectable but often overwhelmed by anthropogenic or other natural (seawater spray, geogenic dust) contributions. Volcanic contribution may derive from both dry and wet deposition of gases and aerosols from the volcanic plume, but sometimes also from leaching of freshly emitted volcanic ashes. In fact, in our background site (7.5 km in the upwind direction) volcanic contribution has been detected only following an ash deposition event. About 30 samples of fresh snow were collected in the upper part of the volcano, during the winters 2006 and 2007 to estimate deposition processes at high altitude during cold periods. Some of the samples were collected immediately after a major explosive event from the summit craters to understand the interaction between snow and fresh erupted ash. Sulphur, Chlorine and Fluorine, are the major elements that prevailingly characterize the volcanic contribution in atmospheric precipitation on Mount Etna, but high concentrations of many trace elements are also detected in the studied samples. In particular, bulk deposition samples display high concentration of Al, Fe, Ti, Cu, As, Rb, Pb, Tl, Cd, Cr, U and Ag, in the site most exposed to the volcanic emissions: median concentration values are about two orders of magnitude higher than those measured in our background site. Also in the snow samples the volcanic signature is clearly detectable and decreases with distance from the summit craters. Some of the analysed elements display very high enrichment values with respect to the average crust and, in the closest site to the summit craters, also deposition values higher than those measured in polluted urban or industrial sites.

Beschreibung: Published

Beschreibung: Vienna, Austria

Beschreibung: 4.5. Degassamento naturale

Beschreibung: open

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: 〈b〉Foraminiferal response to environmental changes in Kiel Fjord, SW Baltic Sea〈/b〉〈br〉 A. Nikulina, I. Polovodova, and J. Schönfeld〈br〉 eEarth, 3, 37-49, doi:10.5194/ee-3-37-2008, 2008〈br〉 The living benthic foraminiferal assemblages in Kiel Fjord (SW Baltic Sea) were investigated in the years 2005 and 2006. The faunal studies were accomplished by geochemical analyses of surface sediments. In general, sediment pollution by copper, zinc, tin and lead is assessed as moderate in comparison with levels reported from other areas of the Baltic Sea. However, the inner Kiel Fjord is still exposed to a high load of metals and organic matter due to enhanced accumulation of fine-grained sediments in conjunction with potential pollution sources as shipyards, harbours and intensive traffic. The results of our survey show that the dominant environmental forcing of benthic foraminifera is nutrients availability coupled with human impact. A comparison with faunal data from the 1960s reveals apparent changes in species composition and population densities. The stress-tolerant species 〈i〉Ammonia beccarii〈/i〉 invaded Kiel Fjord. 〈i〉Ammotium cassis〈/i〉 had disappeared that reflects apparently the changes in salinity over the last 10 years. These changes in foraminiferal community and a significant increase of test abnormalities indicate an intensified environmental stress since the 1960s.

Beschreibung: 〈b〉Foraminiferal response to environmental changes in Kiel Fjord, SW Baltic Sea〈/b〉〈br〉 A. Nikulina, I. Polovodova, and J. Schönfeld〈br〉 eEarth, 3, 37-49, doi:10.5194/ee-3-37-2008, 2008〈br〉 The living benthic foraminiferal assemblages in Kiel Fjord (SW Baltic Sea) were investigated in the years 2005 and 2006. The faunal studies were accomplished by geochemical analyses of surface sediments. In general, sediment pollution by copper, zinc, tin and lead is assessed as moderate in comparison with levels reported from other areas of the Baltic Sea. However, the inner Kiel Fjord is still exposed to a high load of metals and organic matter due to enhanced accumulation of fine-grained sediments in conjunction with potential pollution sources as shipyards, harbours and intensive traffic. The results of our survey show that the dominant environmental forcing of benthic foraminifera is nutrients availability coupled with human impact. A comparison with faunal data from the 1960s reveals apparent changes in species composition and population densities. The stress-tolerant species 〈i〉Ammonia beccarii〈/i〉 invaded Kiel Fjord. 〈i〉Ammotium cassis〈/i〉 had disappeared that reflects apparently the changes in salinity over the last 10 years. These changes in foraminiferal community and a significant increase of test abnormalities indicate an intensified environmental stress since the 1960s.

Beschreibung: 〈b〉Decline of coral reefs during late Paleocene to early Eocene global warming〈/b〉〈br〉 C. Scheibner and R. P. Speijer〈br〉 eEarth, 3, 19-26, doi:10.5194/ee-3-19-2008, 2008〈br〉 Since the 1980s the frequency of warming events has intensified and simultaneously widespread coral bleaching, and enhanced coral mortality have been observed. Yet, it remains unpredictable how tropical coral reef communities will react to prolonged adverse conditions. Possibly, coral reef systems are sufficiently robust to withstand continued environmental pressures. But if coral mortality increases, what will platform communities of the future look like? The co-evolution of early Paleogene carbonate platforms and palaeoclimate may provide insight. Here we document the impact of early Paleogene global warming on shallow-water carbonate platforms in the Tethys. Between 59 and 55 Ma, three discrete stages in platform development can be identified Tethys-wide: during the first stage carbonate platforms mainly consisted of coralgal reefs; during the second – transitional – stage coralgal reefs thrived only at middle latitudes and gave way to larger foraminifera as dominant carbonate producer in low latitudes; finally, during the third stage, newly developing larger foraminifera lineages completely took over the role as main carbonate-producing organisms in low to middle latitudes. We postulate that rising temperatures led to a stepwise demise of Paleocene coral reefs, giving way to an unprecedented expansion of larger foraminifera, dominating Tethyan platforms during the early Eocene.

Beschreibung: 〈b〉Palaeomagnetic investigations of sediments cores from Axios zone (N. Greece): implications of low inclinations in the Aegean〈/b〉〈br〉 E. Aidona, D. Kondopoulou, R. Scholger, A. Georgakopoulos, and A. Vafeidis〈br〉 eEarth, 3, 7-18, doi:10.5194/ee-3-7-2008, 2008〈br〉 Sediment cores from 13 deep boreholes (1–4.1 km) distributed within Axios zone in Northern Greece have been studied by means of palaeomagnetism. Both low field magnetic susceptibility and intensity of the natural remanent magnetization (NRM) indicate rather weakly magnetised materials. A set of 390 samples have been subjected to thermal and alternative field demagnetization. Isothermal remanent magnetization (IRM) acquisition curves and thermomagnetic analysis suggest the dominance of magnetite. Thin sections from 30 selected samples were studied in order to more precisely characterise their magnetic mineralogy. This investigation also reveals the presence of magnetite and pyrite in framboidal form. An attempt to re-orient some of the samples was partially successful by using the viscous component and the anisotropy method. These techniques were applied in order to correct the palaeomagnetic directions due to the orientation ambiguity of the core samples. The corrected mean direction converges towards an eastward value, in agreement with the overall pattern of the onshore results from previous investigations in the study area. 〈br〉〈br〉 Finally, the observed inclinations of characteristic remanences in these rocks are much lower than the expected ones but converge with those obtained from formations on land.

Beschreibung: 〈b〉Zoogeography of the bottom Foraminifera of the West-African coast〈/b〉〈br〉 V. Mikhalevich〈br〉 eEarth Discuss., 3, 1-9, doi:10.5194/eed-3-1-2008, 2008〈br〉 〈b〉Revised manuscript has not been submitted〈/b〉 (discussion: closed, 8 comments)〈br〉 The sediment samples from the continental shelf of West-Equatorial Africa (from the Strait of Gibraltar to the Niger estuary), depths ranging from 0 to 69 m were found to contain 176 bottom foraminiferal species. For the majority of them (126 species), their areas of occurrences were mapped and the peculiar features of the geographical range and distribution were studied. The species natural habitats were established based on the taxonomical revision of the species in study all over the World Ocean based on the collections of the Zoological Institute RAS and wide literary data. The method of perforated cards was used to mark the geographical locations of all of the species studied. In order to establish the species geographic zonal distribution (together with their depth habitat) the five characteristic groups of the species were separated: 1. pan-oceanic (cosmopolitan), 2. widely spread tropical-boreal, 3. tropical-law boreal, 4. tropical-subtropical, 5. tropical. The percent of the species of each group among the species composition was established for the fauna of each station and for the whole region.

Beschreibung: 〈b〉Zoogeography of the bottom Foraminifera of the West-African coast〈/b〉〈br〉 V. Mikhalevich〈br〉 eEarth Discuss., 3, 1-9, doi:10.5194/eed-3-1-2008, 2008〈br〉 〈b〉Revised manuscript has not been submitted〈/b〉 (discussion: closed, 8 comments)〈br〉 The sediment samples from the continental shelf of West-Equatorial Africa (from the Strait of Gibraltar to the Niger estuary), depths ranging from 0 to 69 m were found to contain 176 bottom foraminiferal species. For the majority of them (126 species), their areas of occurrences were mapped and the peculiar features of the geographical range and distribution were studied. The species natural habitats were established based on the taxonomical revision of the species in study all over the World Ocean based on the collections of the Zoological Institute RAS and wide literary data. The method of perforated cards was used to mark the geographical locations of all of the species studied. In order to establish the species geographic zonal distribution (together with their depth habitat) the five characteristic groups of the species were separated: 1. pan-oceanic (cosmopolitan), 2. widely spread tropical-boreal, 3. tropical-law boreal, 4. tropical-subtropical, 5. tropical. The percent of the species of each group among the species composition was established for the fauna of each station and for the whole region.

Beschreibung: 〈b〉Use of remote sensing and GIS in mapping the environmental sensitivity areas for desertification of Egyptian territory〈/b〉〈br〉 A. Gad and I. Lotfy〈br〉 eEarth Discuss., 3, 41-85, doi:10.5194/eed-3-41-2008, 2008〈br〉 〈b〉Revised manuscript has not been submitted〈/b〉 (discussion: closed, 3 comments)〈br〉 Desertification is defined in the first art of the convention to combat desertification as 〈i〉"land degradation in arid, semiarid and dry sub-humid areas resulting from climatic variations and human activities".〈/i〉 Its consequence include a set of important processes which are active in arid and semi arid environment, where water is the main limiting factor of land use performance in such ecosystem . Desertification indicators or the groups of associated indicators should be focused on a single process. They should be based on available reliable information sources, including remotely sensed images, topographic data (maps or DEM'S), climate, soils and geological data. The current work aims to map the Environmental Sensitivity Areas (ESA's) to desertification in whole territory of Egypt at a scale of 1:1 000 000. 〈br〉〈br〉 ETM satellite images, geologic and soil maps were used as main sources for calculating the index of Environmental Sensitivity Areas (ESAI) for desertification. The algorism is adopted from MEDALLUS methodology as follows; 〈br〉〈br〉 ESAI = (SQI * CQI * VQI)〈sup〉1/3〈/sup〉 〈br〉〈br〉 Where SQI is the soil quality index, CQI is the climate quality index and VQI is the vegetation quality index. The SQI is based on rating the parent material, slope, soil texture, and soil depth. The VQI is computed on bases of rating three categories (i.e. erosion protection, drought resistance and plant cover). The CQI is based on the aridity index, derived from values of annual rainfall and potential evapotranspiration. Arc-GIS 9 software was used for the computation and sensitivity maps production. 〈br〉〈br〉 The results show that the soil of the Nile Valley are characterized by a moderate SQI, however the those in the interference zone are low soil quality indexed. The dense vegetation of the valley has raised its VQI to be good, however coastal areas are average and interference zones are low. The maps of ESA's for desertification show that 86.1% of Egyptian territory is classified as very sensitive areas, while 4.3% as Moderately sensitive, and 9.6% as sensitive. 〈br〉〈br〉 It can be concluded that implementing the maps of sensitivity to desertification is rather useful in the arid and semi arid areas as they give more likely quantitative trend for frequency of sensitive areas. The integration of different factors contributing to desertification sensitivity may lead to plan a successful combating. The usage of space data and GIS proved to be suitable tools to rely estimation and to fulfill the needed large computational requirements. They are also useful in visualizing the sensitivity situation of different desertification parameters.

Beschreibung: 〈b〉Palaeomagnetic investigations of sediments cores from Axios zone (N. Greece): implications of low inclinations in the Aegean〈/b〉〈br〉 E. Aidona, D. Kondopoulou, R. Scholger, A. Georgakopoulos, and A. Vafeidis〈br〉 eEarth, 3, 7-18, doi:10.5194/ee-3-7-2008, 2008〈br〉 Sediment cores from 13 deep boreholes (1–4.1 km) distributed within Axios zone in Northern Greece have been studied by means of palaeomagnetism. Both low field magnetic susceptibility and intensity of the natural remanent magnetization (NRM) indicate rather weakly magnetised materials. A set of 390 samples have been subjected to thermal and alternative field demagnetization. Isothermal remanent magnetization (IRM) acquisition curves and thermomagnetic analysis suggest the dominance of magnetite. Thin sections from 30 selected samples were studied in order to more precisely characterise their magnetic mineralogy. This investigation also reveals the presence of magnetite and pyrite in framboidal form. An attempt to re-orient some of the samples was partially successful by using the viscous component and the anisotropy method. These techniques were applied in order to correct the palaeomagnetic directions due to the orientation ambiguity of the core samples. The corrected mean direction converges towards an eastward value, in agreement with the overall pattern of the onshore results from previous investigations in the study area. 〈br〉〈br〉 Finally, the observed inclinations of characteristic remanences in these rocks are much lower than the expected ones but converge with those obtained from formations on land.

Beschreibung: 〈b〉Geometry of the Turkey-Arabia and Africa-Arabia plate boundaries in the latest Miocene to Mid-Pliocene: the role of the Malatya-Ovacık Fault Zone in eastern Turkey〈/b〉〈br〉 R. Westaway, T. Demir, and A. Seyrek〈br〉 eEarth, 3, 27-35, doi:10.5194/ee-3-27-2008, 2008〈br〉 We suggest a working hypothesis for the geometry of the strike-slip faults that formed the boundaries between the Turkish, African and Arabian plates in the latest Miocene to Mid-Pliocene (LMMP), between ~7–6 Ma and ~3.5 Ma. This geometry differed significantly from the modern geometry; the northern Dead Sea Fault Zone (DSFZ) was located east of its present line and the TR-AR boundary was formed by the Malatya-Ovacık Fault Zone (MOFZ), located well north of the modern East Anatolian Fault Zone (EAFZ). The MOFZ is potentially the most problematic aspect of such a scheme, given the dramatically different interpretations of it that have been proposed. However, the presently-available evidence, albeit limited, is consistent with our proposed interpretation. Significant differences between the proposed LMMP fault geometry and the modern geometry include, first, the transtensional geometry of the MOFZ, the modern EAFZ being typically a left-lateral transform fault zone but with localized transpression. Second, the MOFZ slip rate was much lower than the ~9–10 mm a〈sup〉−1〈/sup〉 EAFZ slip rate; it is estimated as ~2–3 mm a〈sup〉−1〈/sup〉, having produced no more than ~8 km of slip during its approximately three million year long activity. The Euler vector is tentatively inferred to have involved relative rotation between the Turkish and Arabian Plates at ~0.85±0.15° Ma〈sup〉−1〈/sup〉 about a pole at ~37.75±0.15° N, ~38.8±0.3° E. Third, unlike at present, there was no throughgoing linkage of left-lateral faulting between the LMMP DSFZ and the MOFZ; instead, the DSFZ terminated northward, and the MOFZ terminated southward, in a zone of localised crustal shortening adjoining the suture of the former Neotethys Ocean in the Kahramanmaraş-Pazarcık region of SE Turkey. The different motion of the Turkish plate relative to Arabia, and, thus, relative to Eurasia, means that senses and rates of crustal deformation can be expected to have been different during the LMMP phase from at present, throughout the eastern Mediterranean region.

Beschreibung: 〈b〉Decline of coral reefs during late Paleocene to early Eocene global warming〈/b〉〈br〉 C. Scheibner and R. P. Speijer〈br〉 eEarth, 3, 19-26, doi:10.5194/ee-3-19-2008, 2008〈br〉 Since the 1980s the frequency of warming events has intensified and simultaneously widespread coral bleaching, and enhanced coral mortality have been observed. Yet, it remains unpredictable how tropical coral reef communities will react to prolonged adverse conditions. Possibly, coral reef systems are sufficiently robust to withstand continued environmental pressures. But if coral mortality increases, what will platform communities of the future look like? The co-evolution of early Paleogene carbonate platforms and palaeoclimate may provide insight. Here we document the impact of early Paleogene global warming on shallow-water carbonate platforms in the Tethys. Between 59 and 55 Ma, three discrete stages in platform development can be identified Tethys-wide: during the first stage carbonate platforms mainly consisted of coralgal reefs; during the second – transitional – stage coralgal reefs thrived only at middle latitudes and gave way to larger foraminifera as dominant carbonate producer in low latitudes; finally, during the third stage, newly developing larger foraminifera lineages completely took over the role as main carbonate-producing organisms in low to middle latitudes. We postulate that rising temperatures led to a stepwise demise of Paleocene coral reefs, giving way to an unprecedented expansion of larger foraminifera, dominating Tethyan platforms during the early Eocene.

Beschreibung: 〈b〉Characteristics of chlorites in seismogenic fault zones: the Taiwan Chelungpu Fault Drilling Project (TCDP) core sample〈/b〉〈br〉 Y. Hashimoto, O. Tadai, M. Tanimizu, W. Tanikawa, T. Hirono, W. Lin, T. Mishima, M. Sakaguchi, W. Soh, S. R. Song, K. Aoike, T. Ishikawa, M. Murayama, K. Fujimoto, T. Fukuchi, M. Ikehara, H. Ito, H. Kikuta, M. Kinoshita, K. Masuda, T. Matsubara, O. Matsubayashi, K. Mizoguchi, N. Nakamura, K. Otsuki, T. Shimamoto, H. Sone, and M. Takahashi〈br〉 eEarth, 3, 1-6, doi:10.5194/ee-3-1-2008, 2008〈br〉 The iron content and the asymmetry of iron and magnesium ions in chlorites are examined for the Chelungpu Fault in Taiwan, which is a seismogenic fault. The samples are collected from the cores drilled for the Taiwan Chelungpu Fault Drilling Project (TCDP, borehole B). Three fault zones are recognized as candidates for the source of seismogenic materials. The fault zones are composed of fractured-damaged rocks, breccia, gray gouge, black gouge, and black material. Chlorite from each type of rock was analyzed by using X-ray diffraction (XRD). The iron content and asymmetry of the iron and magnesium ions in the chlorites were estimated from the XRD peak ratios. The hydroxide and silicate layers of chlorite in the black gouge and black material have low iron contents. Many studies have suggested that a temperature rise occurred at the fault zones. In addition, the temperature rise can result in the production of iron oxides such as magnetite or maghemite, as reported by other studies. However, the temperature rise cannot explain the low value of iron content in the chlorites. Another reason for the low value of iron content is the variation in the pH of the fluid, which can be controlled by radical reactions. Therefore, on the basis of chlorite characteristics, the reactions at the seismogenic fault are due not only to the thermal decomposition resulting from the temperature rise and but also to rock-fluid interactions.

Beschreibung: 〈b〉Characteristics of chlorites in seismogenic fault zones: the Taiwan Chelungpu Fault Drilling Project (TCDP) core sample〈/b〉〈br〉 Y. Hashimoto, O. Tadai, M. Tanimizu, W. Tanikawa, T. Hirono, W. Lin, T. Mishima, M. Sakaguchi, W. Soh, S. R. Song, K. Aoike, T. Ishikawa, M. Murayama, K. Fujimoto, T. Fukuchi, M. Ikehara, H. Ito, H. Kikuta, M. Kinoshita, K. Masuda, T. Matsubara, O. Matsubayashi, K. Mizoguchi, N. Nakamura, K. Otsuki, T. Shimamoto, H. Sone, and M. Takahashi〈br〉 eEarth, 3, 1-6, doi:10.5194/ee-3-1-2008, 2008〈br〉 The iron content and the asymmetry of iron and magnesium ions in chlorites are examined for the Chelungpu Fault in Taiwan, which is a seismogenic fault. The samples are collected from the cores drilled for the Taiwan Chelungpu Fault Drilling Project (TCDP, borehole B). Three fault zones are recognized as candidates for the source of seismogenic materials. The fault zones are composed of fractured-damaged rocks, breccia, gray gouge, black gouge, and black material. Chlorite from each type of rock was analyzed by using X-ray diffraction (XRD). The iron content and asymmetry of the iron and magnesium ions in the chlorites were estimated from the XRD peak ratios. The hydroxide and silicate layers of chlorite in the black gouge and black material have low iron contents. Many studies have suggested that a temperature rise occurred at the fault zones. In addition, the temperature rise can result in the production of iron oxides such as magnetite or maghemite, as reported by other studies. However, the temperature rise cannot explain the low value of iron content in the chlorites. Another reason for the low value of iron content is the variation in the pH of the fluid, which can be controlled by radical reactions. Therefore, on the basis of chlorite characteristics, the reactions at the seismogenic fault are due not only to the thermal decomposition resulting from the temperature rise and but also to rock-fluid interactions.

Beschreibung: 〈b〉Geometry of the Turkey-Arabia and Africa-Arabia plate boundaries in the latest Miocene to Mid-Pliocene: the role of the Malatya-Ovacık Fault Zone in eastern Turkey〈/b〉〈br〉 R. Westaway, T. Demir, and A. Seyrek〈br〉 eEarth, 3, 27-35, doi:10.5194/ee-3-27-2008, 2008〈br〉 We suggest a working hypothesis for the geometry of the strike-slip faults that formed the boundaries between the Turkish, African and Arabian plates in the latest Miocene to Mid-Pliocene (LMMP), between ~7–6 Ma and ~3.5 Ma. This geometry differed significantly from the modern geometry; the northern Dead Sea Fault Zone (DSFZ) was located east of its present line and the TR-AR boundary was formed by the Malatya-Ovacık Fault Zone (MOFZ), located well north of the modern East Anatolian Fault Zone (EAFZ). The MOFZ is potentially the most problematic aspect of such a scheme, given the dramatically different interpretations of it that have been proposed. However, the presently-available evidence, albeit limited, is consistent with our proposed interpretation. Significant differences between the proposed LMMP fault geometry and the modern geometry include, first, the transtensional geometry of the MOFZ, the modern EAFZ being typically a left-lateral transform fault zone but with localized transpression. Second, the MOFZ slip rate was much lower than the ~9–10 mm a〈sup〉−1〈/sup〉 EAFZ slip rate; it is estimated as ~2–3 mm a〈sup〉−1〈/sup〉, having produced no more than ~8 km of slip during its approximately three million year long activity. The Euler vector is tentatively inferred to have involved relative rotation between the Turkish and Arabian Plates at ~0.85±0.15° Ma〈sup〉−1〈/sup〉 about a pole at ~37.75±0.15° N, ~38.8±0.3° E. Third, unlike at present, there was no throughgoing linkage of left-lateral faulting between the LMMP DSFZ and the MOFZ; instead, the DSFZ terminated northward, and the MOFZ terminated southward, in a zone of localised crustal shortening adjoining the suture of the former Neotethys Ocean in the Kahramanmaraş-Pazarcık region of SE Turkey. The different motion of the Turkish plate relative to Arabia, and, thus, relative to Eurasia, means that senses and rates of crustal deformation can be expected to have been different during the LMMP phase from at present, throughout the eastern Mediterranean region.

Beschreibung: 〈b〉Use of remote sensing and GIS in mapping the environmental sensitivity areas for desertification of Egyptian territory〈/b〉〈br〉 A. Gad and I. Lotfy〈br〉 eEarth Discuss., 3, 41-85, doi:10.5194/eed-3-41-2008, 2008〈br〉 〈b〉Revised manuscript has not been submitted〈/b〉 (discussion: closed, 3 comments)〈br〉 Desertification is defined in the first art of the convention to combat desertification as 〈i〉"land degradation in arid, semiarid and dry sub-humid areas resulting from climatic variations and human activities".〈/i〉 Its consequence include a set of important processes which are active in arid and semi arid environment, where water is the main limiting factor of land use performance in such ecosystem . Desertification indicators or the groups of associated indicators should be focused on a single process. They should be based on available reliable information sources, including remotely sensed images, topographic data (maps or DEM'S), climate, soils and geological data. The current work aims to map the Environmental Sensitivity Areas (ESA's) to desertification in whole territory of Egypt at a scale of 1:1 000 000. 〈br〉〈br〉 ETM satellite images, geologic and soil maps were used as main sources for calculating the index of Environmental Sensitivity Areas (ESAI) for desertification. The algorism is adopted from MEDALLUS methodology as follows; 〈br〉〈br〉 ESAI = (SQI * CQI * VQI)〈sup〉1/3〈/sup〉 〈br〉〈br〉 Where SQI is the soil quality index, CQI is the climate quality index and VQI is the vegetation quality index. The SQI is based on rating the parent material, slope, soil texture, and soil depth. The VQI is computed on bases of rating three categories (i.e. erosion protection, drought resistance and plant cover). The CQI is based on the aridity index, derived from values of annual rainfall and potential evapotranspiration. Arc-GIS 9 software was used for the computation and sensitivity maps production. 〈br〉〈br〉 The results show that the soil of the Nile Valley are characterized by a moderate SQI, however the those in the interference zone are low soil quality indexed. The dense vegetation of the valley has raised its VQI to be good, however coastal areas are average and interference zones are low. The maps of ESA's for desertification show that 86.1% of Egyptian territory is classified as very sensitive areas, while 4.3% as Moderately sensitive, and 9.6% as sensitive. 〈br〉〈br〉 It can be concluded that implementing the maps of sensitivity to desertification is rather useful in the arid and semi arid areas as they give more likely quantitative trend for frequency of sensitive areas. The integration of different factors contributing to desertification sensitivity may lead to plan a successful combating. The usage of space data and GIS proved to be suitable tools to rely estimation and to fulfill the needed large computational requirements. They are also useful in visualizing the sensitivity situation of different desertification parameters.

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: The atmospheric chemistry general circulation model ECHAM5/MESSy1 has been extended by processes that parameterize particle precipitation. Several types of particle precipitation that directly affect NOy and HOx concentrations in the middle atmosphere are accounted for and discussed in a series of papers. In the companion paper, the ECHAM5/MESSy1 solar proton event parameterization is discussed, while in the current paper we focus on low energy electrons (LEE) that produce NOx in the upper atmosphere. For the flux of LEE NOx into the top of the model domain a novel technique which can be applied to most atmospheric chemistry general circulation models has been developed and is presented here. The technique is particularly useful for models with an upper boundary between the stratopause and mesopause and therefore cannot directly incorporate upper atmospheric NOx production. The additional NOx source parametrization is based on a measure of geomagnetic activity, the Ap index, which has been shown to be a good proxy for LEE NOx interannual variations. HALOE measurements of LEE NOx that has been transported into the stratosphere are used to develop a scaling function which yields a flux of NOx that is applied to the model top. We describe the implementation of the parameterization as the submodel SPACENOX in ECHAM5/MESSy1 and discuss the results from test simulations. The NOx enhancements and associated effects on ozone are shown to be in good agreement with independent measurements. Ap index data is available for almost one century, thus the parameterization is suitable for simulations of the recent climate.

Beschreibung: Water vapor is an important constituent of the atmosphere. Because of its abundance it plays an important role for the radiation budget of the atmosphere and has major influence on weather and climate. In this work the integrated water vapor (IWV) measurements derived from the measurements of two satellite sensors, SCIAMACHY and AMSU-B, and two ground-based sensors, a Fourier-transform spectrometer (FTIR) and an O3 microwave ozone sensor (RAM), are compared to radio-sonde measurements in Ny Ålesund, 79° N. All four remote sensors exploit different principles and work in different wavelength regions. Combined they deliver a comprehensive picture of the IWV above Ny Ålesund. The ground-based FTIR reproduces the radio-sonde measurements very well and also shows a high correlation and very little scatter of about 10%. The other remote sensing instruments show a good correlation with the coincident radio-sonde measurements but show high scatter of about 20% (standard deviation). The ground-based RAM performs similar to the satellite instruments, which is somewhat surprising, because measuring IWV is only a by-product for this sensor. The RAM sensor records a measurement every hour and is therefore suited to observe the diurnal variation. As measured by the RAM and FTIR the variance within 4 h is often in excess of 50% (minimum – maximum of the measured IWV). This large variance in the integrated water vapor renders the comparison of different sensors a difficult task. The derived variance of the instruments when compared to radio-sonde measurements can be explained by the high natural variability of IWV.

Beschreibung: This paper analyses a stratospheric injection by deep convection of biomass fire emissions over North America (Alaska, Yukon and Northwest Territories) on 24 June 2004 and its long-range transport over the eastern coast of the United States and the eastern Atlantic. The case study is done using MOZAIC observations of ozone, carbon monoxide, nitrogen oxides (NOx+PAN) and water vapour during the crossing of the southernmost tip of an upper level trough over the Eastern Atlantic on 30 June 03:00 UTC and 10:00 UTC and in a vertical profile over Washington DC on 30 June 17:00 UTC, and by lidar observations of aerosol backscattering at Madison (University of Wisconsin) on 28 June. Attribution of the plumes to the boreal fires is achieved by backward simulations with a Lagrangian particle dispersion model (FLEXPART). A simulation with the Meso-NH model for the source region shows that a boundary layer tracer, mimicking the boreal forest fire smoke, is lofted into the lowermost stratosphere (2–5 pvu layer) during the diurnal convective cycle. The isentropic levels (above 335 K) correspond to those of the downstream MOZAIC observations. The parameterized convective detrainment flux is intense enough to fill the volume of a model mesh (20 km horizontal, 500 m vertical) above the tropopause with pure boundary layer air in a time period compatible with the convective diurnal cycle, i.e. about 5 h. The maximum instantaneous detrainment fluxes deposited about 15–20% of the initial boundary layer tracer concentration at 335 K, which according to the 275-ppbv carbon monoxide maximum mixing ratio observed by MOZAIC over eastern Atlantic, would be associated with a 1.4–1.8 ppmv carbon monoxide mixing ratio in the boundary layer over the source region.

Beschreibung: Chamber studies of glyoxal uptake onto neutral ammonium sulphate aerosol were performed under dark and irradiated conditions to gain further insight into processes controlling glyoxal uptake onto ambient aerosol. Organic fragments from glyoxal dimers and trimers were observed within the aerosol under dark and irradiated conditions; glyoxal oligomer formation and overall organic growth were found to be reversible under dark conditions. Analysis of high-resolution time-of-flight aerosol mass spectra provides evidence for irreversible formation of carbon-nitrogen (C-N) compounds in the aerosol. These compounds are likely to be imidazoles formed by reaction of glyoxal with the ammonium sulphate seed. To the authors' knowledge, this is the first time C-N compounds resulting from condensed phase reactions with ammonium sulphate seed have been detected in aerosol. Organosulphates were not detected under dark conditions. However, active oxidative photochemistry, similar to that found in cloud processing, was found to occur within aerosol during irradiated experiments. Organosulphates, carboxylic acids, and organic esters were identified within the aerosol. Our study suggests that both C-N compound formation and photochemical processes should be considered in models of secondary organic aerosol formation via glyoxal.

Beschreibung: We present the first single particle results obtained using an Aerodyne time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS). The instrument was deployed at the T1 ground site approximately 40 km northeast of the Mexico City Metropolitan Area (MCMA) as part of the MILAGRO field study in March of 2006. The instrument was operated as a standard AMS from 12–30 March, acquiring average chemical composition and size distributions for the ambient aerosol, and in single particle mode from 27–30 March. Over a 75-h sampling period, 12 853 single particle mass spectra were optically triggered, saved, and analyzed. The correlated optical and chemical detection allowed detailed examination of single particle collection and quantification within the LS-ToF-AMS. The single particle data enabled the mixing states of the ambient aerosol to be characterized within the context of the size-resolved ensemble chemical information. The particulate mixing states were examined as a function of sampling time and most of the particles were found to be internal mixtures containing many of the organic and inorganic species identified in the ensemble analysis. The single particle mass spectra were deconvolved, using techniques developed for ensemble AMS data analysis, into HOA, OOA, NH4NO3, (NH4)2SO4, and NH4Cl fractions. Average single particle mass and chemistry measurements are shown to be in agreement with ensemble MS and PTOF measurements. While a significant fraction of ambient particles were internal mixtures of varying degrees, single particle measurements of chemical composition allowed the identification of time periods during which the ambient ensemble was externally mixed. In some cases the chemical composition of the particles suggested a likely source. Throughout the full sampling period, the ambient ensemble was an external mixture of combustion-generated HOA particles from local sources (e.g. traffic), with number concentrations peaking during morning rush hour (04:00–08:00 LT) each day, and more processed particles of mixed composition from nonspecific sources. From 09:00–12:00 LT all particles within the ambient ensemble, including the locally produced HOA particles, became coated with NH4NO3 due to photochemical production of HNO3. The number concentration of externally mixed HOA particles remained low during daylight hours. Throughout the afternoon the OOA component dominated the organic fraction of the single particles, likely due to secondary organic aerosol formation and condensation. Single particle mass fractions of (NH4)2SO4 were lowest during the day and highest during the night. In one instance, gas-to-particle condensation of (NH4)2SO4 was observed on all measured particles within a strong SO2 plume arriving at T1 from the northwest. Particles with high NH4Cl mass fractions were identified during early morning periods. A limited number of particles (~5% of the total number) with mass spectral features characteristic of biomass burning were also identified.

Beschreibung: The seasonality of transport and mixing of air into the lowermost stratosphere (LMS) is studied using distributions of mean age of air and a~mass balance approach, based on in-situ observations of SF6 and CO2 during the SPURT (Spurenstofftransport in der Tropopausenregion, trace gas transport in the tropopause region) aircraft campaigns. Combining the information of the mean age of air and the water vapour distributions we demonstrate that the tropospheric air transported into the LMS above the extratropical tropopause layer (ExTL) originates predominantly from the tropical tropopause layer (TTL). The concept of our mass balance is based on simultaneous measurements of the two passive tracers and the assumption that transport into the LMS can be described by age spectra which are superposition of two different modes. Based on this concept we conclude that the stratospheric influence on LMS composition is strongest in April with tropospheric fractions (α1) below 20% and that the strongest tropospheric signatures are found in October with (α1 greater than 80%. Beyond the fractions, our mass balance concept allows to calculate the associated transit times for transport of tropospheric air from the tropics into the LMS. The shortest transit times (

Beschreibung: Field and lab measurements suggest that low-molecular weight (MW) organic acids and bases exist in accumulation and nucleation mode particles, despite their relatively high pure-liquid vapor pressures. The mechanism(s) by which such compounds contribute to the mass growth of existing aerosol particles and newly formed particles has not been thoroughly explored. One mechanism by which low-MW compounds may contribute to new particle growth is through the formation of organic salts. In this paper we use thermodynamic modeling to explore the potential for organic salt formation by atmospherically relevant organic acids and bases for two system types: one in which the relative contribution of ammonia vs. amines in forming organic salts was evaluated, the other in which the decrease in volatility of organic acids and bases due to organic salt formation was assessed. The modeling approach employed relied heavily on group contribution and other estimation methods for necessary physical and chemical parameters. The results of this work suggest that amines may be an important contributor to organic salt formation, and that experimental data are greatly needed to improve our understanding of organic salt formation in atmospherically relevant systems and to accurately predict the potential contribution of such salts to new particle growth.

Beschreibung: An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (elevation 2182 m-MSL), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ every 5 min. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m−3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed a~large accumulation mode peaking around 500–600 nm in Dva while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggest that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event occurred on 15 May 2006, during which ammonium sulfate contributed 〉90% of the total NR-PM1 mass. This event was followed by a~high OA episode likely associated with regional emissions. The trans-Pacific OA were more oxidized and aged than the regional OA.

Beschreibung: We examine the hygroscopic properties of secondary organic aerosol particles generated through the reaction of alpha-pinene and ozone using a continuous flow reaction chamber. The water activity versus composition relationship is calculated from measurements of growth factors at relative humidities up to 99.6% and from measurements of cloud condensation nuclei activity. The observed relationships are complex, suggesting highly non-ideal behavior for aerosol water contents at relative humidities less than 98%. We present two models that may explain the observed water activity-composition relationship equally well. The first model assumes that the aerosol is a pseudo binary mixture of infinitely water soluble compounds and sparingly soluble compounds that gradually enter the solution as dilution increases. The second model is used to compute the Gibbs free energy of the aerosol-water mixture and shows that the aerosol behaves similarly to what can be expected for single compounds that contain a certain fraction of oxygenated and non-polar functional groups.

Beschreibung: In spite of the strict EU regulations, concentrations of surface ozone and PM10 often exceed the pollution standards for The Netherlands and Europe. Their concentrations are controlled by (precursor) emissions, social and economic developments and a complex combination of meteorological actors. This study tackles the latter, and provides insight in the meteorological processes that play a role in O3 and PM10 levels in Cabauw (The Netherlands). The relations between meteorological actors and air quality are studied on a~local scale based on observations from Cabauw and are determined by a comprehensive correlation analysis and a multiple regression (MLR) analysis in 2 modes, with and without air quality variables as predictors. Furthermore, the objective Lamb Weather Type (WT) approach based on ECMWF (European Center for Medium-range Weather Forecasting) operational data is used to assess the influence of the large-scale circulation on air quality. Keeping in mind its future use in downscaling future climate scenarios for air quality purposes, special emphasis is given to an appropriate selection of the regressor variables readily available from operational meteorological forecasts or OAGCMs (Ocean-Atmosphere coupled General Circulation Models). The regression models perform satisfactory for both O3 and PM10, with an increased performance when including previous days air quality information. The lamb weather types show a seasonal distinct pattern for high (low) episodes of average O3 and PM10 concentrations, and these are clear related with the meteorology-air quality correlation analysis. Although using a circulation type approach can bring some interesting physical relations forward, our analysis reveals the circulation method is limited in terms of short-term air quality forecast for both O3 and PM10. In summary, it is concluded that the use of a regression model is more promising for short-term downscaling from climate scenarios than the use of a weather type classification approach.

Beschreibung: We present global distributions of carbon monoxide (CO) from the upper troposphere to the mesosphere observed by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) on Envisat. Vertically resolved volume mixing ratio profiles have been retrieved from 4.7 μm limb emission spectra under consideration of non-local thermodynamic equilibrium. The precision of individual CO profiles is typically 5–30 ppbv (15–40%). Estimated systematic errors are in the order of 8–15%. Below 60 km, the vertical resolution is 4–7 km. The data set which covers 54 days from September 2003 to March 2004 has been derived with an improved retrieval version including (i) the retrieval of log(vmr), (ii) the consideration of illumination-dependent vibrational population gradients along the instrument's line of sight, and (iii) joint-fitted vmr horizontal gradients in latitudinal and longitudinal directions. A detailed analysis of spatially resolved CO distributions during the 2003/2004 Northern Hemisphere major warming event demonstrate the potential of MIPAS CO observations to obtain new information on transport processes during dynamical active episodes, particularly on those acting in the vertical. From the temporal evolution of zonally averaged CO abundances, we derived extraordinary polar winter descent velocities of 1200 m per day inside the recovered polar vortex in January 2004. Middle stratospheric CO abundances show a well established correlation with the chemical source CH4, particularly in the tropics. In the upper troposphere, a~moderate CO decrease from September 2003 to March 2004 was observed. Upper tropospheric CO observations provide a detailed picture of long-range transport of polluted air masses and uplift events. MIPAS observations taken on 9–11 September 2003 confirm the trapping of convective outflow of polluted CO-rich air from Southeast Asia into the Asian monsoon anticyclone, which has been described in previous studies. Upper tropospheric CO plumes, observed by MIPAS on this day, were predominantly located in the Northern Hemisphere. Most of these plumes could be related to Southeast Asian pollution by means of backward trajectory calculations. During 20–22 October, southern hemispheric biomass burning was the most likely source of the major CO plumes observed over the Southern Atlantic and Indian Ocean.

Beschreibung: We undertook three-dimensional numerical studies of a marine stratus deck under a strong inversion using an interactive shortwave- and longwave-radiation module. A suite of sensitivity tests were conducted to address the effects of model resolution on entrainment (inversion heights), cloud-radiation interactions, and cloud radiative-forcings by varying model horizontal resolution only, varying vertical resolution only, and varying horizontal- and vertical-resolution simultaneously but with a fixed aspect ratio of 2.5. Our results showed that entrainment (inversion height) is more sensitive to vertical- than to horizontal-resolution. A vertical resolution finer than 40 m can simulate spatial- and temporal-variations in the inversion height well. The inversion height decreases with increasing vertical resolution, but tends to increase with increasing horizontal resolution. Cloud liquid water path doubles after refining both the vertical- and horizontal-resolution by a factor of four. This doubling is associated with a positive feedback between cloud water and cloud top radiative cooling, which amplifies small differences initiated by changes in the model resolution. The magnitude of the cloud radiative-forcing tends to increase with increasing model resolution, mainly attributable to the increase in the cloud liquid water path. Shortwave radiative forcing is dominant, and more sensitive to model resolution than the longwave counterpart.

Beschreibung: Since aerosols act as cloud condensation nuclei (CCN) for cloud water droplets, changes in aerosol concentrations having significant impacts on the corresponding cloud properties. An increase in aerosol concentration leads to an increase in CCN, with an associated decrease in cloud droplet size for a given cloud liquid water content. Smaller droplet sizes may then lead to a reduction in precipitation efficiency and an increase in cloud lifetimes, which induces more reflection of solar radiation back into space, cooling the atmosphere below the cloud layer. In reality, this relationship is much more complex and is interrelated between aerosol, cloud, and atmospheric conditions present at any one time. MODIS aerosol and cloud properties are combined with NCEP Reanalysis data for eight different regions around the globe between March 2000 and December 2005 to study the effects of different aerosol, cloud, and atmospheric conditions on the aerosol indirect effect (AIE). The first AIE for both anthropogenic and dust aerosols is calculated so that the importance of each can be compared. The unique aspect of this research is that it combines multiple satellite data sets over a six year period to provide a comprehensive analysis of indirect effects for different aerosol regimes around the globe. Results show that in most regions, AIE has a distinct seasonal cycle, though the cycle varies in significance and period from region to region. In the Arabian Sea, the six-year mean anthropogenic + dust AIE is −0.4 Wm−2 and is greatest during the summer months (

Beschreibung: Mechanisms controlling surface ozone (O3) over East Asia are examined using the regional Community Multiscale Air Quality (CMAQ) model at two horizontal scales: 81 km and 27 km. Through sensitivity studies and comparison with recently available satellite data and surface measurements in China and Japan, we find that the O3 budget over East Asia shows complex interactions among photochemical production, regional transport, meteorological conditions, burning of agricultural residues, and global inflows. For example, wintertime surface O3 over northern domain is sensitive to boundary conditions derived from the MOZART (Model for Ozone and Related Tracers) global model, whereas summertime O3 budget is controlled by the competitive processes between photochemical production and monsoonal intrusion of low-O3 marine air masses from tropical Pacific. We find that simulated surface O3 for 2001 does not exhibit the same sharp drop in July and August concentrations that is observed at two mountaintop sites (Tai and Hua) for 2004 and Beijing for 1995–2005. CMAQ sensitivity tests with two widely used photochemical schemes demonstrate that over the industrial areas in East Asia north of 30° N, SAPRC99 produces higher values of mean summertime O3 than CBIV, amounting to a difference of 10 ppb. In addition, analysis of NCEP winds and geopotential heights suggests that southwesterly monsoonal intrusion in central east China is weakened in August 2001 as compared with the climatologically mean for 1980–2005. Further examination of the O3 diurnal cycle at nine Japanese sites shows that boundary layer evolution has an important effect on the vertical mixing of ground-level O3, and error in near surface meteorology might contribute to overprediction of nighttime O3 in urban and rural areas. In conclusion, the uncertainties in simulating cloud activities and convection mixing, Asian monsoon circulation, photochemical production, and nighttime cooling explain why CMAQ with 81 km horizontal scale overpredicts the observed surface O3 in July and August over central east China and central Japan by 5–15 ppb (CBIV) and 15–25 ppb (SAPRC99). The results suggest clear benefits in evaluating atmospheric chemistry over Asia with high resolution regional model.

Beschreibung: A new technique is described for the analysis of cloud-resolving model simulations, which allows one to investigate the statistics of the lifecycles of cumulus clouds. Clouds are tracked from timestep-to-timestep within the model run. This allows for a very simple method of tracking, but one which is both comprehensive and robust. An approach for handling cloud splits and mergers is described which allows clouds with simple and complicated time histories to be compared within a single framework. This is found to be important for the analysis of an idealized simulation of radiative-convective equilibrium, in which the moist, buoyant, updrafts (i.e., the convective cores) were tracked. Around half of all such cores were subject to splits and mergers during their lifecycles. For cores without any such events, the average lifetime is 30 min, but events can lengthen the typical lifetime considerably.

Beschreibung: We measured the size distribution of atmospheric neutral and charged clusters and particles down to mobility diameter around 1.5 nm by applying pulse-height CPC technique at SMEAR II station in Hyytiälä, southern Finland during spring 2007 and May 2008. The concentration of molecular clusters smaller than 3 nm seems to be highly variable in boreal forest environment. The concentration varied typically between 500–50 000 cm−3, the medians being 8060 cm−3 in year 2007 and 3380 cm−3 in 2008. By comparing to concentrations measured with ion spectrometers, we conclude that ion clusters and neutral clusters produced by ion-ion recombination are usually not sufficient to explain all of the observed clusters; the median fraction of recombination products from all neutral clusters was 4.9%. Before and during most new particle formation events the cluster formation rate rose only slightly, or remained close to stable. Nocturnal formation of clusters was also frequently observed.

Beschreibung: Simulations of future tropospheric composition often include substantial increases in biogenic isoprene emissions arising from the Arrhenius-like leaf emission response and warmer surface temperatures, and from enhanced vegetation productivity in response to temperature and atmospheric CO2 concentration. However, a number of recent laboratory and field data have suggested a direct inhibition of leaf isoprene production by increasing atmospheric CO2 concentration, notwithstanding isoprene being produced from precursor molecules that include some of the primary products of carbon assimilation. The cellular mechanism that underlies the decoupling of leaf photosynthesis and isoprene production still awaits a full explanation but accounting for this observation in a dynamic vegetation model that contains a semi-mechanistic treatment of isoprene emissions has been shown to change future global isoprene emission estimates notably. Here we use these estimates in conjunction with a chemistry-climate model to compare the effects of isoprene simulations without and with a direct CO2-inhibition on late 21st century O3 and OH levels. The impact on surface O3 was significant. Including the CO2-inhibition of isoprene resulted in opposing responses in polluted (O3 decreases of up to 10 ppbv) vs. less polluted (O3 increases of up to 10 ppbv) source regions, due to isoprene nitrate and peroxy acetyl nitrate (PAN) chemistry. OH concentration increased with relatively lower future isoprene emissions, decreasing methane lifetime by ~7 months. Our simulations underline the large uncertainties in future chemistry and climate studies due to biogenic emission patterns and emphasize the problems of using globally averaged climate metrics to quantify the atmospheric impact of reactive, heterogeneously distributed substances.

Beschreibung: The first measurements of stratospheric bromine nitrate (BrONO2) are reported. Bromine nitrate has been clearly identified in atmospheric infrared emission spectra recorded with the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) aboard the European Envisat satellite, and stratospheric concentration profiles have been determined for different conditions (day and night, different latitudes). The BrONO2 concentrations show strong day/night variations, with much lower concentrations during the day. Maximum volume mixing ratios observed during night are 20 to 25 pptv. The observed concentration profiles are in agreement with estimations from photochemical models and show that the current understanding of stratospheric bromine chemistry is generally correct.

Beschreibung: Boreal spring climate is uniquely susceptible to solar warming mechanisms because it has expansive snow cover and receives relatively strong insolation. Carbonaceous particles can influence snow coverage by warming the atmosphere, reducing surface-incident solar energy (dimming), and reducing snow reflectance after deposition (darkening). We apply a range of models and observations to explore impacts of these processes on springtime climate, drawing several conclusions: 1) Nearly all atmospheric particles (those with visible-band single-scatter albedo less than 0.999), including all mixtures of black carbon (BC) and organic matter (OM), increase net solar heating of the atmosphere-snow column. 2) Darkening caused by small concentrations of particles within snow exceeds the loss of absorbed energy from concurrent dimming, thus increasing solar heating of snowpack as well (positive net surface forcing). Over global snow, we estimate 6-fold greater surface forcing from darkening than dimming, caused by BC+OM. 3) Equilibrium climate experiments suggest that fossil fuel and biofuel emissions of BC+OM induce 95% as much springtime snow cover loss over Eurasia as anthropogenic carbon dioxide, a consequence of strong snow-albedo feedback and large BC+OM emissions from Asia. 4) Of 22 climate models contributing to the IPCC Fourth Assessment Report, 21 underpredict the rapid warming (0.64°C decade−1) observed over springtime Eurasia since 1979. Darkening from natural and anthropogenic sources of BC and mineral dust exerts 3-fold greater forcing on springtime snow over Eurasia (3.9 W m−2) than North America (1.2 W m−2). Inclusion of this forcing significantly improves simulated continental warming trends, but does not reconcile the low bias in rate of Eurasian spring snow cover decline exhibited by all models.

Beschreibung: We have developed an ensemble Kalman Filter (EnKF) to estimate 8-day regional surface fluxes of CO2 from space-borne CO2 dry-air mole fraction observations (XCO2

Beschreibung: There is currently a need of reliable experimental procedure to follow the heterogeneous processing simulating the atmospheric conditions. This work offers a new experimental approach to study the reactivity and the behaviour of SVOC associated with atmospheric particles. The heterogeneous ozonolysis of naphthalene adsorbed on silica and XAD-4 particles is investigated in specially designed flow tube reactors. The experimental procedure consists in adsorbing gaseous naphthalene on particles before exposing it to ozone. By this novel approach the kinetics is determined following the consumption of naphthalene. Using this procedure, the rate constant kO3 of naphthalene is equal to (2.26±0.09)×10−17cm3.molec−1.s−1 and (4.31±1.07)×10−19cm3.molec−1.s−1 at 25°C for silica and XAD-4, respectively. The results show both that nature of the particles significantly affects the kinetics and that heterogeneous ozonolysis of naphthalene is faster than in the gaseous phase.

Beschreibung: Formaldehyde (HCHO) is an important intermediate compound in the degradation of volatile organic compounds (VOCs) in the troposphere. Sources of HCHO are largely dominated by its secondary production from VOC oxidation, methane and isoprene being the main precursors in unpolluted areas. As a result of the moderate lifetime of HCHO, its spatial distribution is determined by reactive hydrocarbon emissions. We focus here on Europe, never studied before, and investigate the influence of the different emissions on HCHO tropospheric columns with the CHIMERE chemical transport model in order to interpret the comparisons between SCIAMACHY and simulated HCHO columns. Observed columns present a bias less than 20% on average. The differences are discussed according to the errors on the model and the observations and the remaining discrepancies are attributed to a misrepresentation of biogenic emissions. This study requires the characterisation of: (1) the model errors and performances concerning formaldehyde. The errors on the HCHO columns, mainly related to chemistry and mixed emission types, are evaluated to 2×1015 molecule/cm2 and the model performances evaluated using surface measurements are satisfactory (~13%); (2) the observation errors that define the needs in spatial and temporal averaging for meaningful comparisons. Perspectives of using SCIAMACHY observations as constraint for biogenic isoprene emissions with an adapted averaging are approached: this new constraint should help to reduce their uncertainties more than 50% in region of intense emissions.

Beschreibung: For a comprehensive understanding of the global carbon cycle precise knowledge of all processes is necessary. Stable isotope (13C and 18O) abundances provide information for the qualification and the quantification of the diverse source and sink processes. This study focuses on the δ18O signature of CO2 from combustion processes, which are widely present both naturally (wild fires), and human induced (fossil fuel combustion, biomass burning) in the carbon cycle. All these combustion processes use atmospheric oxygen, of which the isotopic signature is assumed to be constant with time throughout the whole atmosphere. The combustion is generally presumed to take place at high temperatures, thus minimizing isotopic fractionation. Therefore it is generally supposed that the 18O signature of the produced CO2 is equal to that of the atmospheric oxygen. This study, however, reveals that the situation is much more complicated and that important fractionation effects do occur. From laboratory studies fractionation effects in the order of about 26‰ became obvious, a clear differentiation of about 7‰ was also found in car exhausts which were sampled directly under ambient atmospheric conditions. We investigated a wide range of materials (both different raw materials and similar materials with different inherent 18O signature), sample geometries (e.g. texture and surface-volume ratios) and combustion circumstances. We found that the main factor influencing the specific isotopic signatures of the combustion-derived CO2 and of the concomitantly released oxygen-containing side products, is the case-specific rate of combustion. This points firmly into the direction of (diffusive) transport of oxygen to the reaction zone as the cause of the isotope fractionation. The original 18O signature of the material appeared to have little or no influence.

Beschreibung: We present vertical profiles of the aerosol extinction coefficient retrieved from ground-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements at Tsukuba, Japan (36.1° N, 140.1° E), from November 2006 to March 2007. Retrievals utilizing absorption by the oxygen collision complex O4 are first made at two wavelengths, 354 and 476 nm. A robust assessment of the MAX-DOAS aerosol data is made using coincident lidar measurements throughout the period. Agreement between aerosol extinction coefficients measured by MAX-DOAS and the lidar tends to be better at the longer wavelength and at lower altitudes. At 476 nm, the best agreement, to within 30%, is found at altitudes of 0–1 km, confirming results from a literature assessment for a two-month measurement period. These findings are supported by comparisons of the aerosol optical depth by MAX-DOAS and sky radiometer measurements and are further explained by differences in the O4 absorption and the air mass factor profile between 354 and 476 nm. Thus, uncertainty in MAX-DOAS aerosol measurements is well quantified and characterized, providing a basis for quantitative studies using MAX-DOAS measurements.

Beschreibung: The pre-industrial and present day distributions and burdens of Secondary Organic Aerosol (SOA) have been calculated using the off-line aerosol chemistry transport model Oslo CTM2. The production of SOA was found to have increased from about 43 Tg yr−1 to 69 Tg yr−1 since pre-industrial times, leading to an increase in the global annual mean SOA burden from 0.44 Tg to 0.70 Tg, or about 59%. The increases are greatest over industrialised areas, as well as over regions with high biogenic precursor emissions. The contribution of emissions from different sources to the larger SOA burdens has been calculated. The results suggest that the majority of the increase is caused by emissions of primary organic aerosols (POA), from fossil fuel and bio fuel combustion. When SOA partitioning to ammonium sulphate aerosol was not accounted for, the increase in SOA burden between pre-industrial times and the present was found to be lower (51%), with a production increase of 55%. As yet, very few radiative forcing estimates of SOA exist, and no such estimates were provided in the latest IPCC report. In this study, we find that the change in SOA burden caused a radiative forcing of −0.09 W m−2, when SOA was allowed to partition to both organic and sulphate aerosols, and −0.06 W m−2 when only partitioning to organic aerosols was assumed. Therefore, the radiative forcing of SOA is found to be substantially stronger than the best estimate for POA in the latest IPCC assessment.

Beschreibung: An inverse model using atmospheric CO2 observations from a European network of stations to reconstruct daily CO2 fluxes and their uncertainties over Europe at 50 km resolution has been developed within a Bayesian framework. We use the pseudo-data or identical twin approach in which we try to recover known fluxes using a range of perturbations to the input. In this second part, the focus is put on the sensitivity of flux accuracy to the inverse setup, varying the prior flux errors, the pseudo-data errors and the network of stations. We show that, under a range of assumptions about prior error and data error we can recover fluxes reliably at the scale of 1000 km and 10 days. At smaller scales the performance is highly sensitive to details of the inverse set-up. The use of temporal correlations in the flux domain appears to be of the same importance as the spatial correlations. We also note that the use of simple, isotropic correlations on the prior flux errors is more reliable than the use of apparently physically-based errors. Finally, increasing the European atmospheric network density improves the area with significant error reduction in the flux retrieval.

Beschreibung: A mineral dust module is developed and implemented into the global aerosol microphysics model, GISS-TOMAS. The model is evaluated against long-term measurements of dust surface mass concentrations and deposition fluxes. Predicted mass concentrations and deposition fluxes are in error on average by a factor of 3 and 5, respectively. The comparison shows that the model performs better near the dust source regions but underestimates surface concentrations and deposition fluxes in more remote regions. For example, including only sites with measured dust concentrations of at least 0.5 μg m−3, the model prediction agrees with observations to within a factor of 2. It was hypothesized that the lifetime of dust, 2.6 days in our base case, is too short and causes the underestimation in remote areas. However, a sensitivity simulation with smaller dust particles and increased lifetime, 3.7 days, does not significantly improve the comparison. We conclude that the underestimation of mineral dust in remote areas results from local factors and sources not well described by the dust source function and/or the GCM meteorology. The effect of dust aerosols on CCN(0.2%) concentrations is negligible in most regions of the globe; however, CCN(0.2%) concentrations decrease by 10–20% in dusty regions as a result of coagulational scavenging of CCN particles by dust and a decrease in H2SO4 condensation to CCN particles due to the additional surface area of dust.

Beschreibung: Multi-platform and multi-sensor observations are employed to investigate the impact of mineral dust on cloud microphysical and precipitation processes in mesoscale convective systems. It is clearly evident that for a given convection strength,small hydrometeors were more prevalent in the stratiform rain regions with dust than in those regions that were dust free. Evidence of abundant cloud ice particles in the dust sector, particularly at altitudes where heterogeneous nucleation process of mineral dust prevails, further supports the observed changes of precipitation. The consequences of the microphysical effects of the dust aerosols were to shift the precipitation size spectrum from heavy precipitation to light precipitation and ultimately suppressing precipitation.

Beschreibung: Night-time ozone deposition for a Scots pine forest in Southern Finland was studied at the SMEAR II measurement station by evaluating the turbulent eddy covariance (EC), storage change and vertical advection fluxes. Similarly to night-time carbon dioxide flux, the eddy-covariance flux of ozone was decreasing with turbulence intensity (friction velocity), and storage change of the compound did not compensate the reduction (well-known night-time measurement problem). Accounting for vertical advection resulted in invariance of ozone deposition rate on turbulence intensity. This was also demonstrated for carbon dioxide, verified by independent measurements of NEE by chamber systems. The result highlights the importance of advection when considering the exchange measurements of any scalar. Analysis of aerodynamic and laminar boundary layer resistances by the model approach indicated that the surface resistance and/or chemical sink strength was limiting ozone deposition. The possible aerial ozone sink by known fast chemical reactions with sesquiterpenes and NO explain only a minor fraction of ozone sink. Thus the deposition is controlled either by stomatal uptake or surface reactions or both of them, the mechanisms not affected by turbulence intensity. Therefore invariance of deposition flux on turbulence intensity is expected also from resistance and chemical sink analysis.

Beschreibung: To estimate the impact of emissions by road, aircraft and ship traffic on ozone and OH of the present-day atmosphere seven different atmospheric chemistry models simulated the atmospheric composition of the year 2003. Based on newly developed global emission inventories for road, maritime and aircraft emission data sets each model performed a series of five simulations: A base scenario using the full set of emissions, three sensitivity studies with each individual sector of transport reduced by 5% and one simulation with all traffic related emissions reduced by 5%. The approach minimizes non-linearities in atmospheric chemical effects and are later scaled to 100%. The global annual mean impact of ship emissions on ozone in the boundary layer leads to an increase of ozone of 1.2%, followed by road (0.87%) and aircraft emissions (0.3%). In the upper troposphere between 200–300 hPa both road and ship traffic affect ozone by 1.1%, whereas aircraft emissions contribute 0.9%. However, the sensitivity of ozone formation per NOx molecule emitted is highest for aircraft exhausts. The local maximum effect of the summed traffic emissions on the ozone column predicted by the models is 4.0 DU and occurs over the northern subtropical Atlantic. The impact of traffic emissions on total ozone in the Southern Hemisphere is approximately half of the northern hemispheric perturbation. Below 800 hPa both ozone and OH respond most sensitively to ship emissions in the marine boundary layer over the Atlantic, where the effect can exceed 10% (zonal mean) which is 80% of the total traffic induced ozone perturbation. In the Southern Hemisphere ship emissions contribute relatively strongly to the total ozone perturbation by 60%–80% throughout the year (equivalent to 1–1.5 ppbv). Road emissions have the strongest impact on ozone in the continental boundary layer and the free troposphere in summer. They also affect the upper troposphere particularly during northern summer associated with strong convection in mid latitudes. Ozone perturbations due to road traffic show the strongest seasonal cycle in the northern troposphere, and can even change sign in the continental boundary layer during winter. The OH concentration in the boundary layer is most strongly affected by ship emissions, which has a significant influence on the lifetime of many trace gases including methane. Methane lifetime changes due to ship emissions amount to 4.1%, followed by road (1.6%) and air traffic (1.0%).

Beschreibung: An inverse model using atmospheric CO2 observations from a European network of stations to reconstruct daily CO2 fluxes and their uncertainties over Europe at 50 km resolution has been developed within a Bayesian framework. In this first part, a pseudo-data experiment is performed to assess the potential of continuous measurements over Europe using a network of 10 stations such as in 2001. Under the assumptions of a small observation noise and a perfect atmospheric transport model, the reconstruction of daily CO2 fluxes and in particular of their synoptic variability is best over Western Europe where the network is the densest. At least a 10 days temporal and a 1000 km spatial averaging of the inverted daily/50 km fluxes is required in order to obtain a good agreement between the estimated and the "true" fluxes in terms of correlation and variability. The performances of the inversion system rapidly degrade when fluxes are sought for a smaller temporal or spatial averaging.

Beschreibung: Binary heterogeneous nucleation of water-succinic/glutaric/malonic/adipic acid on nanometer-sized particles is investigated within the frame of classical heterogeneous nucleation theory. Homogeneous nucleation is also included for comparison. It is found that the nucleation probabilities depend on the contact angle and on the size of the seed particles. New thermodynamical properties, such as saturation vapor pressure, density and surface tension for all the dicarboxylic acid aqueous solutions are included in the calculations. While the new surface tension and density formulations do not bring any significant difference in the computed nucleation rate for homogeneous nucleation for succinic and glutaric acids, the use of the newly derived equations for the vapor pressure decrease the acid concentrations in gas phase with 3 orders of magnitude. According to our calculations, the binary heterogeneous nucleation of succinic acid-water and glutaric acid-water – although it requires a 3–4 orders of magnitude lower vapor concentrations than the homogeneous nucleation – cannot take place in atmospheric conditions. On the other hand binary homogeneous nucleation of adipic acid-water systems might be possible in conditions occuring in upper boundary layer. However, a more detailed characterization of the interaction between the surface and the molecules of the nucleating vapor should be considered in the future.

Beschreibung: Detrended fluctuation analysis is applied to the time series of the global tropopause height derived from the 1980–2004 daily radiosonde data, in order to detect long-range correlations in its time evolution. Global tropopause height fluctuations in small time-intervals are found to be positively correlated to those in larger time intervals in a power-law fashion. The exponent of this dependence is larger in the tropics than in the middle and high latitudes in both hemispheres. Greater persistence is observed in the tropopause of the Northern than in the Southern Hemisphere. This finding for the tropopause height variability should reduce the existing uncertainties in assessing the climatic characteristics.

Beschreibung: We conducted measurements of Hg° and RGM at two inland sites, Thompson Farm (TF) and Pac Monadnock (PM), and a marine site (Appledore Island – AI) from the UNH AIRMAP observing network in New Hampshire in 2007. Measurements of other important trace gases and meteorological variables were used to help understand influences on the atmospheric Hg budget in New England. Seasonal variation in both species observed at TF and PM is attributable to such factors as seasonal variation in deposition strength, meteorological conditions and biogenic emissions. Hg° and RGM varied diurnally at TF, particularly in spring, following the trend in air temperature and jNO2 and suggesting photochemical production of RGM. The diurnal patterns of Hg° and RGM at AI during summer were nearly opposite in phase, with Hg° decreasing through late afternoon, suggesting more significant photochemical oxidation of Hg° to RGM in the marine environment, likely due to the presence of marine halogen compounds. A strong relationship of RGM with SO2 at TF suggests a strong contribution of RGM from anthropogenic sources. Significant levels of halogen compounds measured at TF in previous studies, as well as similar Hg° levels and Hg°-CO ratios at TF and AI may suggest that similar air masses are prevalent at these sites.

Beschreibung: In this study, we analyse the sensitivity of nadir viewing satellite observations in the visible range to freshly produced lightning NOx, i.e. for meteorological and (photo-) chemical conditions found in and around cumulonimbus clouds. For the first time, such a study is performed accounting for photo-chemistry, dynamics, and radiative transfer in a consistent way: A one week episode in the TOGA COARE/CEPEX region (Pacific) in December 1992 is simulated with a 3-D cloud resolving chemistry model. The simulated hydrometeor mixing ratios are fed into a Monte Carlo radiative transfer model to calculate box-Air Mass Factors (box-AMFs) for NO2. From these box-AMFs, together with model NOx profiles, slant columns of NO2 (SNO2), i.e. synthetic satellite measurements, are calculated and set in relation to the actual model NOx vertical column (VNOx), yielding the "sensitivity" SNO2/VNOx. From this study, we find a mean sensitivity of 0.46. NOx below the cloud bottom is mostly present as NO2, but shielded from the satellites' view, whereas NOx at the cloud top or above is shifted to NO due to high photolysis and low temperature, and hence not detectable from space. But a significant fraction of the lightning produced NOx in the middle part of the cloud is present as NO2 and has a good visibility from space. Due to the resulting total sensitivity being quite high, nadir viewing satellites provide a valuable additional platform to quantify NOx production by lightning; strong lightning events over "clean" regions should be clearly detectable in satellite observations. Since the observed enhancement of NO2 column densities over mesoscale convective systems are lower than expected for current estimates of NOx production per flash, satellite measurements can in particular constrain the upper bound of lightning NOx production estimates.

Beschreibung: The yields of organic nitrates and of secondary organic aerosol (SOA) particle formation were measured for the reaction NO3+β-pinene under dry and humid conditions in the atmosphere simulation chamber SAPHIR at Research Center Jülich. These experiments were conducted at low concentrations of NO3 (NO3+N2O5

Beschreibung: Ice crystals, also known as diamond dust, are suspended in the boundary layer air under clear sky conditions during most of the Arctic winter in Northern Canada. Occasionally ice crystal events can produce significantly thick layers with optical depths in excess of 2.0 even in the absence of liquid water clouds. Four case studies of high optical depth ice crystal events at Eureka in the Nunavut Territory of Canada during the winter of 2006–2007 are presented. They show that the measured ice crystal surface infrared downward radiative forcing ranged from 8 to 36 W m−2 in the wavelength band from 5.6 to 20 μm for visible optical depths ranging from 0.2 to 1.7. MODIS infrared and visible images and the operational radiosonde wind profile were used to show that these high optical depth events were caused by surface snow being blown off 600 to 800 m high mountain ridges about 20 to 30 km North-West of Eureka and advected by the winds towards Eureka as they settled towards the ground within the highly stable boundary layer. This work presents the first study that demonstrates the important role that surrounding topography plays in determining the occurrence of high optical depth ice crystal events and points to a new source of boundary layer ice crystal events distinct from the classical diamond dust phenomenon.

Beschreibung: Recently it was discovered that over the Middle East during summer ozone mixing ratios can reach a pronounced maximum in the middle troposphere. Here we extend the analysis to the surface and show that especially in the Persian Gulf region conditions are highly favorable for ozone air pollution. Model results indicate that the region is a hot spot of photo-smog where air quality standards are violated throughout the year. Long-distance transports of air pollution from Europe, the Middle East, natural emissions and stratospheric ozone conspire to bring about high background ozone mixing ratios. This provides a hotbed to indigenous air pollution in the dry local weather conditions, which are likely to get worse in future.

Beschreibung: This study examined the estimation accuracy of NOx emissions over East Asia with particular focus on North China and South Korea due to their strong source (North China)-receptor (South Korea) relationship. In order to determine contributions of North China emissions to South Korean air quality accurately, it is important to examine the accuracy of the emission inventories of both regions. In this study, NO2 columns from the US EPA Models-3/CMAQ model simulations carried out using the 2001 ACE-ASIA (Asia Pacific Regional Aerosol Characterization Experiment) emission inventory over East Asia were compared with the GOME-derived NO2 columns. There were large discrepancies between the CMAQ-predicted and GOME-derived NO2 columns in the fall and winter seasons. In particular, while the CMAQ-predicted NO2 columns produced larger values than the GOME-derived NO2 columns over South Korea (receptor region) for all four seasons, the CMAQ-predicted NO2 columns produced smaller values than the GOME-derived NO2 columns over North China (source region) for all seasons with the exception of summer. It is believed that there might be some estimation error in the NOx emissions as well as large uncertainty in NOx loss rates over North China and South Korea. Regarding the latter, this study further focused on the biogenic VOC emissions that were strongly coupled with NOx chemistry in East Asia. It was found that the rates of NOx loss determined by CMAQ modeling studies might be significantly low due to the possible overestimation of biogenic isoprene emissions during summer, particularly in China. In addition, due to the possible overestimation of isoprene emissions, the CMAQ-modeled NO2/NOx ratios might show an incorrectly high level, compared with the actual NO2/NOx ratios. In addition to the retarded NOx chemical loss rates and overestimated NO2/NOx ratios, the omission of soil NOx emissions over North China during summer can lead to an underestimation of NOx emissions over North China during summer. Overall, it is estimated that the NOx emissions in North China are underestimated possibly by ~50% over an entire year. In order to confirm the uncertainty in NOx emissions, the NOx emission over South Korea was further investigated using the ACE-ASIA inventory, REAS (Regional Emission inventory in ASia) and CAPSS (Clean Air Policy Support System) by NIER (National Institute of Environmental Research) in Korea. The NOx emissions from ACE-ASIA and the REAS inventories appear to be approximately 2 times larger for mega-cities in Korea than that from the CAPSS inventory. In contrast, the NOx emissions of ACE-ASIA and REAS inventories are only 10% smaller for North China than the recently-estimated "date-back" ANL (Argonne National Laboratory) inventory. A comparison between the CMAQ-predicted and GOME-derived NO2 columns indicated that both the ACE-ASIA and REAS inventories have some uncertainty in NOx emissions over North China (A) and South Korea (C), which can lead to some error in modeling the formation of ozone and secondary aerosols in South Korea and North China.

Beschreibung: A new one-decade dataset of formaldehyde (HCHO) columns retrieved from GOME and SCIAMACHY is compared with HCHO columns simulated by an updated version of the IMAGES global chemical transport model. This model version includes an optimized chemical scheme with respect to HCHO production, where the short-term and final HCHO yields from pyrogenically emitted non-methane volatile organic compounds (NMVOCs) are estimated from the Master Chemical Mechanism (MCM) and an explicit speciation profile of pyrogenic emissions. The model is driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, whereas biogenic emissions are provided either by the Global Emissions Inventory Activity (GEIA), or by a newly developed inventory based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) algorithms driven by meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). The comparisons focus on tropical ecosystems, North America and China, which experience strong biogenic and biomass burning NMVOC emissions reflected in the enhanced measured HCHO columns. These comparisons aim at testing the ability of the model to reproduce the observed features of the HCHO distribution on the global scale and at providing a first assessment of the performance of the current emission inventories. The high correlation coefficients (r〉0.8) between the observed and simulated columns over most regions indicate a very good consistency between the model, the implemented inventories and the HCHO dataset. The use of the MEGAN-ECMWF inventory improves the model/data agreement in almost all regions, but biases persist over parts of Africa and the Northern Australia. Although neither GFED version is consistent with the data over all regions, a better match is achieved over Indonesia and Southern Africa when GFEDv2 is used, but GFEDv1 succeeds better in getting the correct seasonal patterns and intensities of the fire episodes over the Amazon basin, as reflected by the higher correlations calculated in this region.

Beschreibung: A photoacoustic spectrometer, a nephelometer, an aetholemeter, and an aerosol mass spectrometer were used to measure at ground level real-time aerosol light absorption, scattering, and chemistry at an urban site located in north east Mexico City (Instituto Mexicano del Petroleo, Mexican Petroleum Institute, denoted by IMP), as part of the Megacity Impact on Regional and Global Environments field experiment, MILAGRO, in March 2006. Photoacoustic and reciprocal nephelometer measurements at 532 nm accomplished with a single instrument compare favorably with conventional measurements made with an aethelometer and a TSI nephelometer. The diurnally averaged single scattering albedo at 532 nm was found to vary from 0.60 to 0.85 with the peak value at midday and the minimum value at 7 a.m. local time, indicating that the Mexico City plume is likely to have a net warming effect on local climate. The peak value is associated with strong photochemical generation of secondary aerosol. It is estimated that the same-day photochemical production of secondary aerosol (inorganic and organic) is approximately 40 percent of the aerosol mass concentration and light scattering in association with the peak single scattering albedo. A strong correlation of aerosol scattering at 532 nm and total aerosol mass concentration was found, and an average mass scattering efficiency factor of 3.8 m2/g was determined. Comparisons of photoacoustic and aethalometer light absorption with oxygenated organic aerosol concentration (OOA) indicate a very small systematic bias of the filter based measurement associated with OOA and the peak aerosol single scattering albedo.

Beschreibung: We report on satellite observations of atmospheric Sulfur Dioxide (SO2) emitted from metal smelting industries in Peru, South America and Siberia, Russia. Most of the non-ferrous metal ores are sulfidic and during the smelting process the sulfur is emitted as SO2. In addition to Norilsk, Russia, Peruvian copper smelters are among the most polluting point sources in the world. We retrieve SO2 column amounts from spectra of the Global Ozone Monitoring Experiment (GOME) on the Earth Research Satellite 2 (ERS-2) for the years 1996 to 2002 using an algorithm based on differential Optical Absorption Spectroscopy (DOAS). Areas of enhanced SO2 column amounts are clearly identified on a 7-years mean map of GOME observations over the regions with La Oroya and Ilo copper smelters of Peru and Norilsk smelters of Russia. Since the instrument sensitivity is highly dependent on surface albedo, SO2 vertical profile, solar zenith angle (SZA), wavelength, clouds, and aerosol, radiative transfer modelling is used to convert the analysed slant column densities into vertical column densities. In this study, the full spherical Monte-Carlo radiative transport model TRACY-II is used for SO2 AMF calculation. GOME data is analysed in further detail by calculating time series over these regions. For the different locations, the results demonstrate both, increasing and decreasing trends in the SO2 column amounts over the time period of 1996–2002. The decreasing trend for the Ilo copper smelter is in good agreement with implemented measures for emission reductions. However, even for the cases with decreasing trends, these point sources are still a dominant source of anthropogenic SO2 emissions in their region. For the smelters in Peru, the potential influence due to SO2 emission by the nearby volcanoes is investigated and found to be negligible.

Beschreibung: Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA) in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit mass resolution quadrupole Aerosol Mass Spectrometer (AMS). The results highlight how photochemical processing can lead to considerable evolution of the mass, the volatility and the level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the primary contribution after a few hours of aging under typical summertime conditions. Aging decreased the OA volatility of the total OA as measured with a thermodenuder; it also made the OA progressively more oxygenated in every experiment. With explicit knowledge of the condensed-phase mass spectrum (MS) of the primary emissions from each fire, each MS can be decomposed into primary and residual spectra throughout the experiment. The residual spectra provide an estimate of the composition of the photochemically produced OA. These spectra are also very similar to those of the oxygenated OA that dominates ambient AMS datasets. In addition, aged wood smoke spectra are shown to be similar to those from OA created by photo-oxidized dilute diesel exhaust and aged biomass-burning OA measured in urban and remote locations. This demonstrates that the oxygenated OA observed in the atmosphere can be produced by photochemical aging of dilute emissions from combustion of fuels containing both modern and fossil carbon.

Beschreibung: In this paper we demonstrate the potential of the infrared Fourier transform spectrometer IASI in analysing volcanic eruptions, using the September 2007 eruption at Jebel at Tair as an illustrative example. Detailed radiative transfer calculations are presented, simulating IASI-like transmittance spectra for a variety of volcanic plumes. We analyse the sensitivity of IASI to SO2 at different altitudes and demonstrate that IASI is in principle capable of sensing SO2 down to the surface. Using the brightness temperature difference of well chosen SO2 channels as a filter, we are able to track the plume of the Jebel at Tair eruption for 12 days, on a par with state of the art UV sounders. A method is presented for quickly estimating the altitude of a volcanic plume based on the relative intensities of the SO2 absorption lines. Despite recent advances, it is still very challenging to retrieve vertical profiles of SO2 from nadir viewing satellites. Currently the most accurate profiles in nadir are retrieved using backtracking of the plume with atmospheric transport models. Via full inverse retrievals using the optimal estimation method, we show the possibility of extracting medium coarse vertical profiles from IASI data. The retrieval allows us to present an evolution of the total mass of SO2 in the plume for the Jebel at Tair eruption. An analytical relation is derived between brightness temperature differences and concentrations, which fits the experimental data very well. The spectral range of IASI also allows retrieval of volcanic aerosols. In the initial plume of the Jebel at Tair eruption, volcanic aerosols were found in the form of ice particles, for which we derived particle sizes.

Beschreibung: The second generation Collection 005 (C005) MODIS operational algorithm for retrieval of aerosol properties was evaluated and validated for the greater Mediterranean basin (29.5° N–46.5° N and 10.5° W–38.5° E), a region with an atmosphere under siege by air pollution and diminishing water resources that are exacerbated by high aerosol loads and climatic change. The present study aims to quantify the differences between the C005 and the previous (C004) MODIS collections, and re-assess the results of previous studies that have been performed for the region using MODIS C004 aerosol optical depth (AOD) products. Daily data of AOD from EOS-Terra covering the 6-year period 2000–2006 were taken from both C005 and C004 Level-3 datasets, and were inter-compared and validated against ground-based measurements from 29 AERONET stations. The C005 data were found to significantly better agree with the AERONET data than those of C004. The correlation coefficient between MODIS and AERONET was found to increase from 0.66 to 0.76 and the slope of linear regression MODIS/AERONET from 0.79 to 0.85. The MODIS C005 data still overestimate/underestimate the AERONET AOD values smaller/larger than 0.25, but to a much smaller extent than C004 data. The better agreement of C005 with AERONET data arises from the generally lower C005 values, with regional mean AOD values equal to 0.27 and 0.22 for C004 and C005, respectively. This decrease, however, is not uniform over the region and involves a significant decrease over land and a small increase over the ocean for AOD values greater than 0.1 (opposite changes were found under aerosol-clean conditions). Both data sets indicate a decrease in the regional mean AOD over the period 2000–2006, equal to 20% based on C005 and 17% based on C004 datasets, though the intra-annual and inter-annual variation did not change significantly, thus indicating a systematic correction to C004 values.

Beschreibung: 10Be concentrations measured in ice cores exhibit larger temporal variability than expected based on theoretical production calculations. To investigate whether this is due to atmospheric transport a general circulation model study is performed with the 10Be production divided into stratospheric, tropospheric tropical, tropospheric subtropical and tropospheric polar sources. A control run with present day 10Be production rate is compared with a run during a geomagnetic minimum. The present 10Be production rate is 4–5 times higher at high latitudes than in the tropics whereas during a period of no geomagnetic dipole field it is constant at all latitudes. The 10Be deposition fluxes, however, show a very similar latitudinal distribution in both the present day and the geomagnetic minimum run indicating that 10Be is well mixed in the atmosphere before its deposition. This is also confirmed by the fact that the contribution of 10Be produced in the stratosphere is dominant (55%–70%) and relatively constant at all latitudes. The contribution of stratospheric 10Be is approximately 70% in Greenland and 60% in Antarctica reflecting the weaker stratosphere-troposphere air exchange in the Southern Hemisphere.

Beschreibung: Dust and black carbon aerosol have long been known to have potentially important and diverse impacts on cloud droplet formation. Most studies to date focus on the soluble fraction of such particles, and ignore interactions of the insoluble fraction with water vapor (even if known to be hydrophilic). To address this gap, we develop a new parameterization framework that considers cloud droplet formation within an ascending air parcel containing insoluble (but wettable) particles mixed with aerosol containing an appreciable soluble fraction. Activation of particles with a soluble fraction is described through well-established Köhler Theory, while the activation of hydrophilic insoluble particles is treated by "adsorption-activation" theory. In the latter, water vapor is adsorbed onto insoluble particles, the activity of which is described by a multilayer Frankel-Halsey-Hill (FHH) adsorption isotherm modified to account for particle curvature. We further develop FHH activation theory, and i) find combinations of the adsorption parameters AFHH, BFHH for which activation into cloud droplets is not possible, and, ii) express activation properties (critical supersaturation) that follow a simple power law with respect to dry particle diameter. Parameterization formulations are developed for sectional and lognormal aerosol size distribution functions. The new parameterization is tested by comparing the parameterized cloud droplet number concentration against predictions with a detailed numerical cloud model, considering a wide range of particle populations, cloud updraft conditions, water vapor condensation coefficient and FHH adsorption isotherm characteristics. The agreement between parameterization and parcel model is excellent, with an average error of 10% and R2 ~0.98.

Beschreibung: Zenith-sky scattered sunlight observations using differential optical absorption spectroscopy (DOAS) technique were carried out in Shanghai, China (31.3° N, 121.5° E) since December 2006. At this polluted urban site, the measurement provided NO2 total columns in the daytime. Here, we present a new method to extract time series of tropospheric vertical column densities (VCD) of NO2 from these observations. The derived tropospheric NO2 VCD is an important quantity for the estimation of emissions and for the validation of satellite observations. Our method makes use of assumptions on the relative NO2 height profiles and on the diurnal variation of the stratospheric NO2 VCD. The influence of these parameters on the retrieved tropospheric NO2 VCD is discussed; for a polluted site like Shanghai, the accuracy of our method is estimated to be

Beschreibung: In this study, we present carbonyl sulfide (COS) measurements from an ice core drilled near South Pole, East Antarctica (SPRESSO). The samples are from 135–291 m, with estimated mean COS ages ranging from 278 to 2155 years before present (defined as 2000 C.E.). When combined with the previous records of COS from Antarctic ice cores and firn air, the current data provide a continuous record of COS extending beyond the last two millennia. The general agreement between ice cores, firn air, and modern air measurements supports the idea that polar ice is a valid archive for paleoatmospheric COS. The average COS mixing ratio of the SPRESSO data set is (331±18) ppt (parts per trillion as mol/mol, ±1σ, n=100), excluding 6 outliers. These data confirm earlier firn air and ice core measurements indicating that the late 20th century COS levels of 500 ppt are greatly increased over preindustrial levels and represent the highest atmospheric levels over the past 2000 years. The data also provide evidence of climate-related variability on centennial time-scales, with relative maxima at the peaks of Medieval Climate Anomaly and Little Ice Age. There is evidence for a long-term increasing trend in COS of 1.8 ppt per 100 years. Further ice core studies will be needed to determine whether this trend reflects secular variability in atmospheric COS, or a slow post-depositional chemical loss of COS in the ice core.