| 31. |
- Barbaro, E., et al.
(author)
-
Measurement report: Spatial variations in ionic chemistry and water-stable isotopes in the snowpack on glaciers across Svalbard during the 2015-2016 snow accumulation season
- 2021
-
In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:4, s. 3163-3180
-
Journal article (peer-reviewed)abstract
- The Svalbard archipelago, located at the Arctic sea-ice edge between 74 and 81 degrees N, is similar to 60% covered by glaciers. The region experiences rapid variations in atmospheric flow during the snow season (from late September to May) and can be affected by air advected from both lower and higher latitudes, which likely impact the chemical composition of snowfall. While long-term changes in Svalbard snow chemistry have been documented in ice cores drilled from two high-elevation glaciers, the spatial variability of the snowpack composition across Svalbard is comparatively poorly understood. Here, we report the results of the most comprehensive seasonal snow chemistry survey to date, carried out in April 2016 across 22 sites on seven glaciers across the archipelago. At each glacier, three snowpits were sam- pled along the altitudinal profiles and the collected samples were analysed for major ions (Ca2+, K+, Na+, Mg2+, NH4+, SO42, Br-, Cl-, and NO3-) and stable water isotopes ( ffi18O, delta H-2). The main aims were to investigate the natural and anthropogenic processes influencing the snowpack and to better understand the influence of atmospheric aerosol transport and deposition patterns on the snow chemical composition. The snow deposited in the southern region of Svalbard is characterized by the highest total ionic loads, mainly attributed to sea-salt particles. Both NO3 and NH4+ in the seasonal snowpack reflect secondary aerosol formation and post-depositional changes, resulting in very different spatial deposition patterns: NO3 has its highest loading in northwestern Spitsbergen and NH4+ in the south-west. The Br enrichment in snow is highest in north-eastern glacier sites closest to areas of extensive sea-ice coverage. Spatial correlation patterns between Na+ and delta O-18 suggest that the influence of long-range transport of aerosols on snow chemistry is proportionally greater above 600-700ma.s.l.
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| 32. |
- Barlakas, Vasileios, 1986, et al.
(author)
-
The sub-adiabatic model as a concept for evaluating the representation and radiative effects of low-level clouds in a high-resolution atmospheric model
- 2020
-
In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:1, s. 303-322
-
Journal article (peer-reviewed)abstract
- The realistic representation of low-level clouds, including their radiative effects, in atmospheric models remains challenging. A sensitivity study is presented to establish a conceptual approach for the evaluation of low-level clouds and their radiative impact in a highly resolved atmospheric model. Considering simulations for six case days, the analysis supports the notion that the properties of clouds more closely match the assumptions of the sub-adiabatic rather than the vertically homogeneous cloud model, suggesting its use as the basis for evaluation. For the considered cases, 95.7% of the variance in cloud optical thickness is explained by the variance in the liquid water path, while the droplet number concentration and the sub-adiabatic fraction contribute only 3.5% and 0.2% to the total variance, respectively. A mean sub-adiabatic fraction of 0.45 is found, which exhibits strong inter-day variability. Applying a principal component analysis and subsequent varimax rotation to the considered set of nine properties, four dominating modes of variability are identified, which explain 97.7% of the total variance. The first and second components correspond to the cloud base and top height, and to liquid water path, optical thickness, and cloud geometrical extent, respectively, while the cloud droplet number concentration and the sub-adiabatic fraction are the strongest contributors to the third and fourth components. Using idealized offline radiative transfer calculations, it is confirmed that the shortwave and longwave cloud radiative effects exhibit little sensitivity to the vertical structure of clouds. This reconfirms, based on an unprecedented large set of highly resolved vertical cloud profiles, that the cloud optical thickness and the cloud top and bottom heights are the main factors dominating the shortwave and longwave radiative effect of clouds and should be evaluated together with radiative fluxes using observations to attribute model deficiencies in the radiative fluxes to deficiencies in the representation of clouds. Considering the different representations of cloud microphysical processes in atmospheric models, the analysis has been further extended and the deviations between the radiative impact of the single- and double-moment schemes are assessed. Contrasting the shortwave cloud radiative effect obtained from the double-moment scheme to that of a single-moment scheme, differences of about similar to 40 Wm(-2) and significant scatter are observed. The differences are attributable to a higher cloud albedo resulting from the high values of droplet number concentration in particular in the boundary layer predicted by the double-moment scheme, which reach median values of around similar to 600 cm(-3).
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| 33. |
- Baró Pérez, Alejandro, 1991, et al.
(author)
-
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
- 2024
-
In: Atmospheric Chemistry and Physics. - 1680-7316 .- 1680-7324. ; 24:8, s. 4591-4610
-
Journal article (peer-reviewed)abstract
- Biomass burning plumes are frequently transported over the southeast Atlantic (SEA) stratocumulus deck during the southern African fire season (June-October). The plumes bring large amounts of absorbing aerosols and enhanced moisture, which can trigger a rich set of aerosol-cloud-radiation interactions with climatic consequences that are still poorly understood. We use large-eddy simulation (LES) to explore and disentangle the individual impacts of aerosols and moisture on the underlying stratocumulus clouds, the marine boundary layer (MBL) evolution, and the stratocumulus-to-cumulus transition (SCT) for three different meteorological situations over the southeast Atlantic during August 2017. For all three cases, our LES shows that the SCT is driven by increased sea surface temperatures and cloud-top entrainment as the air is advected towards the Equator. In the LES model, aerosol indirect effects, including impacts on drizzle production, have a small influence on the modeled cloud evolution and SCT, even when aerosol concentrations are lowered to background concentrations. In contrast, local semi-direct effects, i.e., aerosol absorption of solar radiation in the MBL, cause a reduction in cloud cover that can lead to a speed-up of the SCT, in particular during the daytime and during broken cloud conditions, especially in highly polluted situations. The largest impact on the radiative budget comes from aerosol impacts on cloud albedo: the plume with absorbing aerosols produces a total average 3 d of simulations. We find that the moisture accompanying the aerosol plume produces an additional cooling effect that is about as large as the total aerosol radiative effect. Overall, there is still a large uncertainty associated with the radiative and cloud evolution effects of biomass burning aerosols. A comparison between different models in a common framework, combined with constraints from in situ observations, could help to reduce the uncertainty.
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| 34. |
- Baró Pérez, Alejandro, et al.
(author)
-
Comparing the simulated influence of biomass burning plumes on low-level clouds over the southeastern Atlantic under varying smoke conditions
- 2024
-
In: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 24:8, s. 4591-4610
-
Journal article (peer-reviewed)abstract
- Biomass burning plumes are frequently transported over the southeast Atlantic (SEA) stratocumulus deck during the southern African fire season (June-October). The plumes bring large amounts of absorbing aerosols and enhanced moisture, which can trigger a rich set of aerosol-cloud-radiation interactions with climatic consequences that are still poorly understood. We use large-eddy simulation (LES) to explore and disentangle the individual impacts of aerosols and moisture on the underlying stratocumulus clouds, the marine boundary layer (MBL) evolution, and the stratocumulus-to-cumulus transition (SCT) for three different meteorological situations over the southeast Atlantic during August 2017. For all three cases, our LES shows that the SCT is driven by increased sea surface temperatures and cloud-top entrainment as the air is advected towards the Equator. In the LES model, aerosol indirect effects, including impacts on drizzle production, have a small influence on the modeled cloud evolution and SCT, even when aerosol concentrations are lowered to background concentrations. In contrast, local semi-direct effects, i.e., aerosol absorption of solar radiation in the MBL, cause a reduction in cloud cover that can lead to a speed-up of the SCT, in particular during the daytime and during broken cloud conditions, especially in highly polluted situations. The largest impact on the radiative budget comes from aerosol impacts on cloud albedo: the plume with absorbing aerosols produces a total average 3 d of simulations. We find that the moisture accompanying the aerosol plume produces an additional cooling effect that is about as large as the total aerosol radiative effect. Overall, there is still a large uncertainty associated with the radiative and cloud evolution effects of biomass burning aerosols. A comparison between different models in a common framework, combined with constraints from in situ observations, could help to reduce the uncertainty.
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| 35. |
- Baró Pérez, Alejandro, et al.
(author)
-
Impact of smoke and non-smoke aerosols on radiation and low-level clouds over the southeast Atlantic from co-located satellite observations
- 2021
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:8, s. 6053-6077
-
Journal article (peer-reviewed)abstract
- Data derived from instruments on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) and CloudSat satellites as well as meteorological parameters from reanalysis are used to explore situations when moist aerosol layers overlie stratocumulus clouds over the southeast Atlantic during the biomass burning season (June to October). To separate and quantify the impacts of aerosol loading, aerosol type, and humidity on the radiative fluxes (including cloud top cooling), the data are split into different levels of aerosol and moisture loadings. The aerosol classification available from the CALIPSO products is used to compare and contrast situations with pristine air, with smoke, and with other (non-smoke) types of aerosols. A substantial number of cases with non-smoke aerosols above clouds are found to occur under similar meteorological conditions to the smoke cases. In contrast, the meteorology is substantially different for the pristine situations, making a direct comparison with the aerosol cases ambiguous. The moisture content is enhanced within the aerosol layers, but the relative humidity does not always increase monotonously with increasing optical depth. Shortwave (SW) heating rates within the moist aerosol plumes increase with increasing aerosol loading and are higher in the smoke cases compared to the non-smoke cases. However, there is no clear correlation between moisture changes and SW absorption. Cloud top cooling rates do not show a clear correlation with moisture within the overlying aerosol layers due to the strong variability of the cooling rates caused by other meteorological factors (most notably cloud top temperature). No clear influence of aerosol type or loading on cloud top cooling rates is detected. Further, there is no correlation between aerosol loading and the thermodynamic structure of the atmosphere nor the cloud top height.
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| 36. |
- Baron, P., et al.
(author)
-
Observation of horizontal winds in the middle-atmosphere between 30 degrees S and 55 degrees N during the northern winter 2009-2010
- 2013
-
In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:12, s. 6049-6064
-
Journal article (peer-reviewed)abstract
- Although the links between stratospheric dynamics, climate and weather have been demonstrated, direct observations of stratospheric winds are lacking, in particular at altitudes above 30 km. We report observations of winds between 8 and 0.01 hPa (similar to 35-80 km) from October 2009 to April 2010 by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station. The altitude range covers the region between 35-60 km where previous space-borne wind instruments show a lack of sensitivity. Both zonal and meridional wind components were obtained, though not simultaneously, in the latitude range from 30 degrees S to 55 degrees N and with a single profile precision of 7-9 ms(-1) between 8 and 0.6 hPa and better than 20 ms(-1) at altitudes above. The vertical resolution is 5-7 km except in the upper part of the retrieval range (10 km at 0.01 hPa). In the region between 1-0.05 hPa, an absolute value of the mean difference 5 ms(-1)). In the mesosphere, SMILES and ECMWF zonal winds exhibit large differences (>20 ms(-1)), especially in the tropics. We illustrate our results by showing daily and monthly zonal wind variations, namely the semi-annual oscillation in the tropics and reversals of the flow direction between 50-55 degrees N during sudden stratospheric warmings. The daily comparison with ECMWF winds reveals that in the beginning of February, a significantly stronger zonal westward flow is measured in the tropics at 2 hPa compared to the flow computed in the analysis (difference of similar to 20 ms(-1)). The results show that the comparison between SMILES and ECMWF winds is not only relevant for the quality assessment of the new SMILES winds, but it also provides insights on the quality of the ECMWF winds themselves. Although the instrument was not specifically designed for measuring winds, the results demonstrate that space-borne sub-mm wave radiometers have the potential to provide good quality data for improving the stratospheric winds in atmospheric models.
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| 37. |
- Baron, Phillippe, et al.
(author)
-
Observation of horizontal winds in the middle-atmosphere between 30° S and 55° N during the northern winter 2009–2010
- 2012
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13, s. 6049-6064
-
Journal article (peer-reviewed)abstract
- Although the links between stratospheric dynamics, climate and weather have been demonstrated, direct observations of stratospheric winds are lacking. We report observations of winds between 8 and 0.01 hPa (~35–80 km) from October 2009 to April 2010 by the Superconducting Submillimeter-Wave Limb-Emission Sounder (SMILES) on the International Space Station. The altitude range covers the region between 35–60 km where previous space-borne wind instruments show a lack of sensitivity. Both zonal and meridional wind components were obtained, though not simultaneously, in the latitude range from 30° S to 55° N and with a single profile precision of 7–9 m s−1 between 8 and 0.6 hPa and better than 20 m s−1 at altitudes above. The vertical resolution is 5–7 km except in the upper part of the retrieval range (10 km at 0.01 hPa). In the region between 1–0.05 hPa, a mean difference <2 m s−1 is found between SMILES profiles retrieved from different spectroscopic lines and instrumental settings. Good agreement (mean difference of ~2 m s−1) is also found with the European Centre for Medium-Range Weather Forecasts (ECMWF) analysis in most of the stratosphere except for the zonal winds over the equator (mean difference of 5–10 m s−1). In the mesosphere, SMILES and ECMWF zonal winds exhibit large differences (> 20 m s−1), especially in the tropics. We illustrate our results by showing daily and monthly zonal wind variations, namely the semi-annual oscillation in the tropics and reversals of the flow direction between 50° N–55° N during sudden stratospheric warmings in the stratosphere. The daily comparison with ECMWF winds reveals that in the beginning of February, a significantly stronger zonal westward flow is measured in the tropics at 2 hPa compared to the flow computed in the analysis (difference of ~20 m s−1). The results show that the comparison between SMILES and ECMWF winds is not only relevant for the quality assessment of the new SMILES winds but it also provides insights on the quality of the ECMWF winds themselves. Although the instrument was not specifically designed for measuring winds, the results demonstrate that space-borne sub-mm wave radiometers have the potential to provide good quality data for improving the stratospheric winds in atmospheric models.
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| 38. |
- Bartels-Rausch, T., et al.
(author)
-
A review of air-ice chemical and physical interactions (AICI): Liquids, quasi-liquids, and solids in snow
- 2014
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:3, s. 1587-1633
-
Journal article (peer-reviewed)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.
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| 39. |
- Beddows, D. C. S., et al.
(author)
-
Variations in tropospheric submicron particle size distributions across the European continent 2008-2009
- 2014
-
In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:8, s. 4327-4348
-
Journal article (peer-reviewed)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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| 40. |
- Beecken, Jörg, 1982, et al.
(author)
-
Emission factors of SO2, NOx and particles from ships in Neva Bay from ground-based and helicopter-borne measurements and AIS-based modeling
- 2015
-
In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:9, s. 5229-5241
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Journal article (peer-reviewed)abstract
- Emission factors of SO2, NOx and size-distributed particle numbers were measured for approximately 300 different ships in the Gulf of Finland and Neva Bay area during two campaigns in August/September 2011 and June/July 2012. The measurements were carried out from a harbor vessel and from an Mi-8 helicopter downwind of passing ships. Other measurements were carried out from shore sites near the island of Kronstadt and along the Neva River in the urban area of Saint Petersburg. Most ships were running at reduced speed (10 kn), i.e., not at their optimal load. Vessels for domestic and international shipping were monitored. It was seen that the distribution of the SO2 emission factors is bi-modal, with averages of 4.6 and 18.2 gSO(2) kg(fuel)(-1) for the lower and the higher mode, respectively. The emission factors show compliance with the 1% fuel sulfur content Sulfur Emission Control Areas (SECA) limit for 90% of the vessels in 2011 and 97% in 2012. The distribution of the NOx emission factor is mono-modal, with an average of 58 gNO(x) kg(fuel)(-1). The corresponding emission related to the generated power yields an average of 12.1 gNO(x) kWh(-1). The distribution of the emission factors for particulate number shows that nearly 90% of all particles in the 5.6 nm to 10 mu m size range were below 70 nm in diameter. The distribution of the corresponding emission factors for the mass indicates two separated main modes, one for particles between 30 and 300 nm and the other for above 2 mu m. The average particle emission factors were found to be in the range from 0.7 to 2.7 x 10(16) particles kg(fuel)(-1) and 0.2 to 3.4 gPM kg(fuel)(-1), respectively. The NOx and particulate emissions are comparable with other studies. The measured emission factors were compared, for individual ships, to modeled ones using the Ship Traffic Emission Assessment Model (STEAM) of the Finnish Meteorological Institute. A reasonably good agreement for gaseous sulfur and nitrogen emissions can be seen for ships in international traffic, but significant deviations are found for inland vessels. Regarding particulate mass, the values of the modeled data are about 2-3 times higher than the measured results, which probably reflects the assumptions made in the modeled fuel sulfur content. The sulfur contents in the fuel retrieved from the measurements were lower than the previously used assumptions by the City of Saint Petersburg when carrying out atmospheric modeling, and using these measurements it was possible to better assess the impact of shipping on air quality.
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