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  • Aemisegger, F., et al. (författare)
  • Deuterium excess as a proxy for continental moisture recycling and plant transpiration
  • 2014
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7324 .- 1680-7316. ; 14:8, s. 4029-4054
  • Tidskriftsartikel (refereegranskat)abstract
    • Studying the evaporation process and its link to the atmospheric circulation is central for a better understanding of the feedbacks between the surface water components and the atmosphere. In this study, we use 5 months of deuterium excess (d) measurements at the hourly to daily timescale from a cavity ring-down laser spectrometer to characterise the evaporation source of low-level continental water vapour at the long-term hydrometeorological monitoring site Rietholzbach in northeastern Switzerland. To reconstruct the phase change history of the air masses in which we measure the d signature and to diagnose its area of surface evaporation we apply a Lagrangian moisture source diagnostic. With the help of a correlation analysis we investigate the strength of the relation between d measurements and the moisture source conditions. Temporal episodes with a duration of a few days of strong anticorrelation between d and relative humidity as well as temperature are identified. The role of plant transpiration, the large-scale advection of remotely evaporated moisture, the local boundary layer dynamics at the measurement site and recent precipitation at the site of evaporation are discussed as reasons for the existence of these modes of strong anticorrelation between d and moisture source conditions. We show that the importance of continental moisture recycling and the contribution of plant transpiration to the continental evaporation flux may be deduced from the d-relative humidity relation at the seasonal timescale as well as for individual events. The methodology and uncertainties associated with these estimates of the transpiration fraction of evapotranspiration are presented and the proposed novel framework is applied to individual events from our data set. Over the whole analysis period (August to December 2011) a transpiration fraction of the evapotranspiration flux over the continental part of the moisture source region of 62 % is found albeit with a large event-to-event variability (0 % to 89 %) for continental Europe. During days of strong local moisture recycling a higher overall transpiration fraction of 76 % (varying between 65 % and 86 %) is found. These estimates are affected by uncertainties in the assumptions involved in our method as well as by parameter uncertainties. An average uncertainty of 11 % results from the strong dependency of the transpiration estimates on the choice of the non-equilibrium fractionation factor. Other uncertainty sources like the influence of boundary layer dynamics are probably large but more difficult to quantify. Nevertheless, such Lagrangian estimates of the transpiration part of continental evaporation could potentially be useful for the verification of model estimates of this important land-atmosphere coupling parameter.
  • Andersson, Sandra, et al. (författare)
  • Composition and evolution of volcanic aerosol from eruptions of Kasatochi, Sarychev and Eyjafjallajokull in 2008-2010 based on CARIBIC observations
  • 2013
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7316 .- 1680-7324. ; 13:4, s. 1781-1796
  • Tidskriftsartikel (refereegranskat)abstract
    • Large volcanic eruptions impact significantly on climate and lead to ozone depletion due to injection of particles and gases into the stratosphere where their residence times are long. In this the composition of volcanic aerosol is an important but inadequately studied factor. Samples of volcanically influenced aerosol were collected following the Kasatochi (Alaska), Sarychev (Russia) and also during the Eyjafjallajokull (Iceland) eruptions in the period 2008-2010. Sampling was conducted by the CARIBIC platform during regular flights at an altitude of 10-12 km as well as during dedicated flights through the volcanic clouds from the eruption of Eyjafjallajokull in spring 2010. Elemental concentrations of the collected aerosol were obtained by accelerator-based analysis. Aerosol from the Eyjafjallajokull volcanic clouds was identified by high concentrations of sulphur and elements pointing to crustal origin, and confirmed by trajectory analysis. Signatures of volcanic influence were also used to detect volcanic aerosol in stratospheric samples collected following the Sarychev and Kasatochi eruptions. In total it was possible to identify 17 relevant samples collected between 1 and more than 100 days following the eruptions studied. The volcanically influenced aerosol mainly consisted of ash, sulphate and included a carbonaceous component. Samples collected in the volcanic cloud from Eyjafjallajokull were dominated by the ash and sulphate component (similar to 45% each) while samples collected in the tropopause region and LMS mainly consisted of sulphate (50-77%) and carbon (21-43%). These fractions were increasing/decreasing with the age of the aerosol. Because of the long observation period, it was possible to analyze the evolution of the relationship between the ash and sulphate components of the volcanic aerosol. From this analysis the residence time (1/e) of sulphur dioxide in the studied volcanic cloud was estimated to be 45 +/- 22 days.
  • Arneth, Almut, et al. (författare)
  • Global terrestrial isoprene emission models: sensitivity to variability in climate and vegetation
  • 2011
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7316 .- 1680-7324. ; 11:15, s. 8037-8052
  • Tidskriftsartikel (refereegranskat)abstract
    • Due to its effects on the atmospheric lifetime of methane, the burdens of tropospheric ozone and growth of secondary organic aerosol, isoprene is central among the biogenic compounds that need to be taken into account for assessment of anthropogenic air pollution-climate change interactions. Lack of process-understanding regarding leaf isoprene production as well as of suitable observations to constrain and evaluate regional or global simulation results add large uncertainties to past, present and future emissions estimates. Focusing on contemporary climate conditions, we compare three global isoprene models that differ in their representation of vegetation and isoprene emission algorithm. We specifically aim to investigate the between-and within model variation that is introduced by varying some of the models' main features, and to determine which spatial and/or temporal features are robust between models and different experimental set-ups. In their individual standard configurations, the models broadly agree with respect to the chief isoprene sources and emission seasonality, with maximum monthly emission rates around 20-25 Tg C, when averaged by 30-degree latitudinal bands. They also indicate relatively small (approximately 5 to 10% around the mean) interannual variability of total global emissions. The models are sensitive to changes in one or more of their main model components and drivers (e. g., underlying vegetation fields, climate input) which can yield increases or decreases in total annual emissions of cumulatively by more than 30 %. Varying drivers also strongly alters the seasonal emission pattern. The variable response needs to be interpreted in view of the vegetation emission capacities, as well as diverging absolute and regional distribution of light, radiation and temperature, but the direction of the simulated emission changes was not as uniform as anticipated. Our results highlight the need for modellers to evaluate their implementations of isoprene emission models carefully when performing simulations that use nonstandard emission model configurations.
  • Arneth, Almut, et al. (författare)
  • Process-based estimates of terrestrial ecosystem isoprene emissions: incorporating the effects of a direct CO2-isoprene interaction
  • 2007
  • Ingår i: Atmospheric Chemistry and Physics. - European Geosciences Union. - 1680-7324 .- 1680-7316. ; 7, s. 31-53
  • Forskningsöversikt (refereegranskat)abstract
    • In recent years evidence has emerged that the amount of isoprene emitted from a leaf is affected by the CO2 growth environment. Many - though not all - laboratory experiments indicate that emissions increase significantly at below-ambient CO2 concentrations and decrease when concentrations are raised to above-ambient. A small number of process-based leaf isoprene emission models can reproduce this CO2 stimulation and inhibition. These models are briefly reviewed, and their performance in standard conditions compared with each other and to an empirical algorithm. One of the models was judged particularly useful for incorporation into a dynamic vegetation model framework, LPJ-GUESS, yielding a tool that allows the interactive effects of climate and increasing CO2 concentration on vegetation distribution, productivity, and leaf and ecosystem isoprene emissions to be explored. The coupled vegetation dynamics-isoprene model is described and used here in a mode particularly suited for the ecosystem scale, but it can be employed at the global level as well. Annual and/or daily isoprene emissions simulated by the model were evaluated against flux measurements ( or model estimates that had previously been evaluated with flux data) from a wide range of environments, and agreement between modelled and simulated values was generally good. By using a dynamic vegetation model, effects of canopy composition, disturbance history, or trends in CO2 concentration can be assessed. We show here for five model test sites that the suggested CO2-inhibition of leaf-isoprene metabolism can be large enough to offset increases in emissions due to CO2-stimulation of vegetation productivity and leaf area growth. When effects of climate change are considered atop the effects of atmospheric composition the interactions between the relevant processes will become even more complex. The CO2-isoprene inhibition may have the potential to significantly dampen the expected steep increase of ecosystem isoprene emission in a future, warmer atmosphere with higher CO2 levels; this effect raises important questions for projections of future atmospheric chemistry, and its connection to the terrestrial vegetation and carbon cycle.
  • Arneth, Almut, et al. (författare)
  • Why are estimates of global terrestrial isoprene emissions so similar (and why is this not so for monoterpenes)?
  • 2008
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7324 .- 1680-7316. ; 8:16, s. 4605-4620
  • Tidskriftsartikel (refereegranskat)abstract
    • Emissions of biogenic volatile organic compounds (BVOC) are a chief uncertainty in calculating the burdens of important atmospheric compounds like tropospheric ozone or secondary organic aerosol, reflecting either imperfect chemical oxidation mechanisms or unreliable emission estimates, or both. To provide a starting point for a more systematic discussion we review here global isoprene and monoterpene emission estimates to-date. We note a surprisingly small variation in the predictions of global isoprene emission rate that is in stark contrast with our lack of process understanding and the small number of observations for model parameterisation and evaluation. Most of the models are based on similar emission algorithms, using fixed values for the emission capacity of various plant functional types. In some cases, these values are very similar but differ substantially in other models. The similarities with regard to the global isoprene emission rate would suggest that the dominant parameters driving the ultimate global estimate, and thus the dominant determinant of model sensitivity, are the specific emission algorithm and isoprene emission capacity. But the models also differ broadly with regard to their representation of net primary productivity, method of biome coverage determination and climate data. Contrary to isoprene, monoterpene estimates show significantly larger model-to-model variation although variation in terms of leaf algorithm, emission capacities, the way of model upscaling, vegetation cover or climatology used in terpene models are comparable to those used for isoprene. From our summary of published studies there appears to be no evidence that the terrestrial modelling community has been any more successful in 'resolving unknowns' in the mechanisms that control global isoprene emissions, compared to global monoterpene emissions. Rather, the proliferation of common parameterization schemes within a large variety of model platforms lends the illusion of convergence towards a common estimate of global isoprene emissions. This convergence might be used to provide optimism that the community has reached the 'relief phase', the phase when sufficient process understanding and data for evaluation allows models' projections to converge, when applying a recently proposed concept. We argue that there is no basis for this apparent relief phase. Rather, we urge modellers to be bolder in their analysis, and to draw attention to the fact that terrestrial emissions, particularly in the area of biome-specific emission capacities, are unknown rather than uncertain.
  • Asmi, A., et al. (författare)
  • Aerosol decadal trends - Part 2: In-situ aerosol particle number concentrations at GAW and ACTRIS stations
  • 2013
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7316 .- 1680-7324. ; 13:2, s. 895-916
  • Tidskriftsartikel (refereegranskat)abstract
    • We have analysed the trends of total aerosol particle number concentrations (N) measured at long-term measurement stations involved either in the Global Atmosphere Watch (GAW) and/or EU infrastructure project ACTRIS. The sites are located in Europe, North America, Antarctica, and on Pacific Ocean islands. The majority of the sites showed clear decreasing trends both in the full-length time series, and in the intra-site comparison period of 2001-2010, especially during the winter months. Several potential driving processes for the observed trends were studied, and even though there are some similarities between N trends and air temperature changes, the most likely cause of many northern hemisphere trends was found to be decreases in the anthropogenic emissions of primary particles, SO2 or some co-emitted species. We could not find a consistent agreement between the trends of N and particle optical properties in the few stations with long time series of all of these properties. The trends of N and the proxies for cloud condensation nuclei (CCN) were generally consistent in the few European stations where the measurements were available. This work provides a useful comparison analysis for modelling studies of trends in aerosol number concentrations.
  • Asmi, A., et al. (författare)
  • Number size distributions and seasonality of submicron particles in Europe 2008-2009
  • 2011
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7316 .- 1680-7324. ; 11:11, s. 5505-5538
  • Tidskriftsartikel (refereegranskat)abstract
    • Two years of harmonized aerosol number size distribution data from 24 European field monitoring sites have been analysed. The results give a comprehensive overview of the European near surface aerosol particle number concentrations and number size distributions between 30 and 500 nm of dry particle diameter. Spatial and temporal distribution of aerosols in the particle sizes most important for climate applications are presented. We also analyse the annual, weekly and diurnal cycles of the aerosol number concentrations, provide log-normal fitting parameters for median number size distributions, and give guidance notes for data users. Emphasis is placed on the usability of results within the aerosol modelling community.
  • Bartels-Rausch, T., et al. (författare)
  • A review of air-ice chemical and physical interactions (AICI): Liquids, quasi-liquids, and solids in snow
  • 2014
  • Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 14:3, s. 1587-1633
  • Tidskriftsartikel (refereegranskat)abstract
    • Snow in the environment acts as a host to rich chemistry and provides a matrix for physical exchange of contaminants within the ecosystem. The goal of this review is to summarise the current state of knowledge of physical processes and chemical reactivity in surface snow with relevance to polar regions. It focuses on a description of impurities in distinct compartments present in surface snow, such as snow crystals, grain boundaries, crystal surfaces, and liquid parts. It emphasises the microscopic description of the ice surface and its link with the environment. Distinct differences between the disordered air-ice interface, often termed quasi-liquid layer, and a liquid phase are highlighted. The reactivity in these different compartments of surface snow is discussed using many experimental studies, simulations, and selected snow models from the molecular to the macro-scale. Although new experimental techniques have extended our knowledge of the surface properties of ice and their impact on some single reactions and processes, others occurring on, at or within snow grains remain unquantified. The presence of liquid or liquid-like compartments either due to the formation of brine or disorder at surfaces of snow crystals below the freezing point may strongly modify reaction rates. Therefore, future experiments should include a detailed characterisation of the surface properties of the ice matrices. A further point that remains largely unresolved is the distribution of impurities between the different domains of the condensed phase inside the snowpack, i.e. in the bulk solid, in liquid at the surface or trapped in confined pockets within or between grains, or at the surface. While surface-sensitive laboratory techniques may in the future help to resolve this point for equilibrium conditions, additional uncertainty for the environmental snowpack may be caused by the highly dynamic nature of the snowpack due to the fast metamorphism occurring under certain environmental conditions. Due to these gaps in knowledge the first snow chemistry models have attempted to reproduce certain processes like the long-term incorporation of volatile compounds in snow and firn or the release of reactive species from the snowpack. Although so far none of the models offers a coupled approach of physical and chemical processes or a detailed representation of the different compartments, they have successfully been used to reproduce some field experiments. A fully coupled snow chemistry and physics model remains to be developed. © Author(s) 2014.
  • Beddows, D. C. S., et al. (författare)
  • Variations in tropospheric submicron particle size distributions across the European continent 2008-2009
  • 2014
  • Ingår i: Atmospheric Chemistry and Physics. - Copernicus Gesellschaft Mbh. - 1680-7324 .- 1680-7316. ; 14:8, s. 4327-4348
  • Tidskriftsartikel (refereegranskat)abstract
    • Cluster analysis of particle number size distributions from background sites across Europe is presented. This generated a total of nine clusters of particle size distributions which could be further combined into two main groups, namely: a south-to-north category (four clusters) and a west-to-east category (five clusters). The first group was identified as most frequently being detected inside and around northern Germany and neighbouring countries, showing clear evidence of local afternoon nucleation and growth events that could be linked to movement of air masses from south to north arriving ultimately at the Arctic contributing to Arctic haze. The second group of particle size spectra proved to have narrower size distributions and collectively showed a dependence of modal diameter upon the longitude of the site (west to east) at which they were most frequently detected. These clusters indicated regional nucleation (at the coastal sites) growing to larger modes further inland. The apparent growth rate of the modal diameter was around 0.6-0.9 nm h(-1). Four specific air mass back-trajectories were successively taken as case studies to examine in real time the evolution of aerosol size distributions across Europe. While aerosol growth processes can be observed as aerosol traverses Europe, the processes are often obscured by the addition of aerosol by emissions en route. This study revealed that some of the 24 stations exhibit more complex behaviour than others, especially when impacted by local sources or a variety of different air masses. Overall, the aerosol size distribution clustering analysis greatly simplifies the complex data set and allows a description of aerosol aging processes, which reflects the longer-term average development of particle number size distributions as air masses advect across Europe.
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