| 1. |
- Ahlm, Lars, et al.
(författare)
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Particle number concentrations over Europe in 2030 : the role of emissions and new particle formation
- 2013
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Ingår i: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 13:20, s. 10271-10283
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Tidskriftsartikel (refereegranskat)abstract
- The aerosol particle number concentration is a key parameter when estimating impacts of aerosol particles on climate and human health. We use a three-dimensional chemical transport model with detailed microphysics, PMCAMx-UF, to simulate particle number concentrations over Europe in the year 2030, by applying emission scenarios for trace gases and primary aerosols. The scenarios are based on expected changes in anthropogenic emissions of sulfur dioxide, ammonia, nitrogen oxides, and primary aerosol particles with a diameter less than 2.5 mu m (PM2.5) focusing on a photochemically active period, and the implications for other seasons are discussed. For the baseline scenario, which represents a best estimate of the evolution of anthropogenic emissions in Europe, PMCAMx-UF predicts that the total particle number concentration (N-tot) will decrease by 30-70% between 2008 and 2030. The number concentration of particles larger than 100 nm (N-100), a proxy for cloud condensation nuclei (CCN) concentration, is predicted to decrease by 40-70% during the same period. The predicted decrease in N-tot is mainly a result of reduced new particle formation due to the expected reduction in SO2 emissions, whereas the predicted decrease in N-100 is a result of both decreasing condensational growth and reduced primary aerosol emissions. For larger emission reductions, PMCAMx-UF predicts reductions of 60-80% in both N-tot and N-100 over Europe. Sensitivity tests reveal that a reduction in SO2 emissions is far more efficient than any other emission reduction investigated, in reducing N-tot. For N-100, emission reductions of both SO2 and PM2.5 contribute significantly to the reduced concentration, even though SO2 plays the dominant role once more. The impact of SO2 for both new particle formation and growth over Europe may be expected to be somewhat higher during the simulated period with high photochemical activity than during times of the year with less incoming solar radiation. The predicted reductions in both N-tot and N-100 between 2008 and 2030 in this study will likely reduce both the aerosol direct and indirect effects, and limit the damaging effects of aerosol particles on human health in Europe
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| 2. |
- Couvreux, Fleur, et al.
(författare)
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Boundary-layer turbulent processes and mesoscale variability represented by Numerical Weather Prediction models during the BLLAST campaign
- 2016
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Ingår i: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16:14, s. 8983-9002
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Tidskriftsartikel (refereegranskat)abstract
- This study evaluates the ability of three operational models, AROME, ARPEGE and ECMWF, to predict the boundary-layer turbulent processes and mesoscale variability observed during the Boundary Layer Late-Afternoon and Sunset Turbulence (BLLAST) field campaign. AROME is a 2.5 km limited area non-hydrostatic model operated over France, ARPEGE a global model with a 10 km grid-size over France and ECMWF a global model with a 16 km grid-size. We analyze the representation of the vertical profiles of temperature and humidity and the time evolution of near surface atmospheric variables as well as the radiative and turbulent fluxes for a total of 12 24h-long Intensive Observing Periods. Special attention is paid to the evolution of the turbulent kinetic energy that was sampled by a combination of independent instruments. For the first time, this variable, which is a central variable in the turbulence scheme used in AROME and ARPEGE, is evaluated with observations.
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| 3. |
- Nikulin, Grigory, et al.
(författare)
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The mean meridional circulation and midlatitude ozone buildup
- 2005
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Ingår i: Atmospheric Chemistry and Physics Discussions. - Katlenburg-Lindau : European Geosciences Union (EGU). - 1680-7367 .- 1680-7375 .- 1680-7324. ; 5, s. 3159-3172
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Tidskriftsartikel (refereegranskat)abstract
- The wintertime ozone buildup over the Northern Hemisphere (NH) midlatitudes and its connection with the mean meridional circulation in the stratosphere are examined statistically on a monthly basis from October to March ( 1980 - 2002). The ozone buildup begins locally in October with positive total ozone tendencies over the North Pacific, which spread eastward and westward in November and finally cover all midlatitudes in December. The local onset of the buildup in October is not evident in zonal mean ozone tendency, which is close to zero. From November to March, zonal mean total ozone tendency (50 degrees - 60 degrees N) shows a strong correlation (|r|= 0.7) with several zonal mean parameters associated to the mean meridional circulation, namely: eddy heat flux, temperature tendency, the vertical residual velocity and the residual streamfunction. At the same time, on the latitude-altitude cross section, correlation patterns between ozone tendency and widely used eddy heat flux are not uniform during winter. The strongest correlations are located equatorward ( almost throughout the stratosphere) or poleward ( only in the lower stratosphere) of the edge of the polar vortex. Such distribution may depend on the existence of the midlatitude and polar waveguides which defined refraction of upward propagating waves from the troposphere either to the midlatitude stratosphere or to the polar stratosphere. As a consequence of the nonuniform correlation patterns, heat flux averaged over the common region 45 degrees - 75 degrees N, 100 hPa is not always an optimum proxy for statistical models describing total ozone variability in midlatitudes. Other parameters approximating the strength of the mean meridional circulation have more uniform and stable correlation patterns with ozone tendency during winter. We show that the NH midlatitude ozone buildup has a stable statistical relationship with the mean meridional circulation in all months from October to March and half of the interannual variability in monthly ozone tendencies can be explained by applying different proxies of the mean meridional circulation.
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| 4. |
- Nilsson, Erik, 1983-, et al.
(författare)
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Turbulence Kinetic Energy budget during the afternoon transition – Part 1 : Observed surface TKE budget and boundary layer description for 10 intensive observation period days
- 2016
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Ingår i: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16:14, s. 8849-8872
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Tidskriftsartikel (refereegranskat)abstract
- The decay of turbulence kinetic energy (TKE) and its budget in the afternoon period from mid-day until zero buoyancy flux at the surface is studied in a two-part paper by means of measurements from the Boundary Layer Late Afternoon and Sunset Turbulence (BLLAST) field campaign for 10 Intensive Observation Period days. Here, in Part 1, near-surface measurements from a small tower are used to estimate a TKE budget. The overall boundary layer characteristics and meso-scale situation at the site are also described based upon taller tower measurements, radiosoundings and remote sensing instrumentation. Analysis of the TKE budget during the afternoon transition reveals a variety of different surface layer dynamics in terms of TKE and TKE decay. This is largely attributed to variations in the 8 m wind speed, which is responsible for different amounts of near-surface shear production on different afternoons and variations within some of the afternoon periods. The partitioning of near surface production into local dissipation and transport in neutral and unstably stratified conditions was investigated. Although variations exist both between and within afternoons, as a rule of thumb, our results suggest that about 50 % of the near surface production of TKE is compensated by local dissipation near the surface, leaving about 50 % available for transport. This result indicates that it is important to also consider TKE transport as a factor influencing the near-surface TKE decay rate, which in many earlier studies has mainly been linked with the production terms of TKE by buoyancy and wind shear. We also conclude that the TKE tendency is smaller than the other budget terms, indicating a quasi-stationary evolution of TKE in the afternoon transition. Even though the TKE tendency was observed to be small, a strong correlation to mean buoyancy production of −0.69 was found for the afternoon period. For comparison with previous results, the TKE budget terms are normalized with friction velocity and measurement height and discussed in the framework of Monin–Obukhov similarity theory. Empirically fitted expressions are presented. Alternatively, we also suggest a non-local parametrization of dissipation using a TKE-length scale model which takes into account the boundary layer depth in addition to distance above the ground. The non-local formulation is shown to give a better description of dissipation compared to a local parametrization.
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| 5. |
- Nilsson, Erik, 1983-, et al.
(författare)
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Turbulence Kinetic Energy budget during the afternoon transition – Part 2 : A simple TKE model
- 2016
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Ingår i: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16, s. 8873-8898
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Tidskriftsartikel (refereegranskat)abstract
- A simple model for turbulence kinetic energy (TKE) and the TKE budget is presented for sheared convective atmospheric conditions based on observations from the Boundary Layer Late Afternoon and Sunset Turbulence (BLLAST) field campaign. It is based on an idealized mixed-layer approximation and a simplified near-surface TKE budget. In this model, the TKE is dependent on four budget terms (turbulent dissipation rate, buoyancy production, shear production and vertical transport of TKE) and only requires measurements of three input available (near-surface buoyancy flux, boundary layer depth and wind speed at one height in the surface layer). This simple model is shown to reproduce some of the observed variations between the different studied days in terms of near-surface TKE and its decay during the afternoon transition reasonably well. It is subsequently used to systematically study the effects of buoyancy and shear on TKE evolution using idealized constant and time-varying winds during the afternoon transition. From this, we conclude that many different TKE decay rates are possible under time-varying winds and that generalizing the decay with simple scaling laws for near-surface TKE of the form tαmay be questionable. The model's errors result from the exclusion of processes such as elevated shear production and horizontal advection. The model also produces an overly rapid decay of shear production with height. However, the most influential budget terms governing near-surface TKE in the observed sheared convective boundary layers are included, while only second order factors are neglected. Comparison between modeled and averaged observed estimates of dissipation rate illustrate that the overall behavior of the model is often quite reasonable. Therefore, we use the model to discuss the low turbulence conditions that form first in the upper parts of the boundary layer during the afternoon transition and are only apparent later near the surface. This occurs as a consequence of the continuous decrease of near-surface buoyancy flux during the afternoon transition. This region of weak afternoon turbulence is hypothesized to be a "pre-residual layer", which is important in determining the onset conditions for the weak sporadic turbulence that occur in the residual layer once near-surface stratification has become stable.
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| 6. |
- Aas, W., et al.
(författare)
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Lessons learnt from the first EMEP intensive measurement periods
- 2012
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:17, s. 8073-8094
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Tidskriftsartikel (refereegranskat)abstract
- The first EMEP intensive measurement periods were held in June 2006 and January 2007. The measurements aimed to characterize the aerosol chemical compositions, including the gas/aerosol partitioning of inorganic compounds. The measurement program during these periods included daily or hourly measurements of the secondary inorganic components, with additional measurements of elemental- and organic carbon (EC and OC) and mineral dust in PM1, PM2.5 and PM10. These measurements have provided extended knowledge regarding the composition of particulate matter and the temporal and spatial variability of PM, as well as an extended database for the assessment of chemical transport models. This paper summarise the first experiences of making use of measurements from the first EMEP intensive measurement periods along with EMEP model results from the updated model version to characterise aerosol composition. We investigated how the PM chemical composition varies between the summer and the winter month and geographically. The observation and model data are in general agreement regarding the main features of PM10 and PM2.5 composition and the relative contribution of different components, though the EMEP model tends to give slightly lower estimates of PM10 and PM2.5 compared to measurements. The intensive measurement data has identified areas where improvements are needed. Hourly concurrent measurements of gaseous and particulate components for the first time facilitated testing of modelled diurnal variability of the gas/aerosol partitioning of nitrogen species. In general, the modelled diurnal cycles of nitrate and ammonium aerosols are in fair agreement with the measurements, but the diurnal variability of ammonia is not well captured. The largest differences between model and observations of aerosol mass are seen in Italy during winter, which to a large extent may be explained by an underestimation of residential wood burning sources. It should be noted that both primary and secondary OC has been included in the calculations for the first time, showing promising results. Mineral dust is important, especially in southern Europe, and the model seems to capture the dust episodes well. The lack of measurements of mineral dust hampers the possibility for model evaluation for this highly uncertain PM component. There are also lessons learnt regarding improved measurements for future intensive periods. There is a need for increased comparability between the measurements at different sites. For the nitrogen compounds it is clear that more measurements using artefact free methods based on continuous measurement methods and/or denuders are needed. For EC/OC, a reference methodology (both in field and laboratory) was lacking during these periods giving problems with comparability, though measurement protocols have recently been established and these should be followed by the Parties to the EMEP Protocol. For measurements with no defined protocols, it might be a good solution to use centralised laboratories to ensure comparability across the network. To cope with the introduction of these new measurements, new reporting guidelines have been developed to ensure that all proper information about the methodologies and data quality is given.
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| 7. |
- Abbatt, J. P. D., et al.
(författare)
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Halogen activation via interactions with environmental ice and snow in the polar lower troposphere and other regions
- 2012
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:14, s. 6237-6271
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Tidskriftsartikel (refereegranskat)abstract
- The role of ice in the formation of chemically active halogens in the environment requires a full understanding because of its role in atmospheric chemistry, including controlling the regional atmospheric oxidizing capacity in specific situations. In particular, ice and snow are important for facilitating multiphase oxidative chemistry and as media upon which marine algae live. This paper reviews the nature of environmental ice substrates that participate in halogen chemistry, describes the reactions that occur on such substrates, presents the field evidence for ice-mediated halogen activation, summarizes our best understanding of ice-halogen activation mechanisms, and describes the current state of modeling these processes at different scales. Given the rapid pace of developments in the field, this paper largely addresses advances made in the past five years, with emphasis given to the polar boundary layer. The integrative nature of this field is highlighted in the presentation of work from the molecular to the regional scale, with a focus on understanding fundamental processes. This is essential for developing realistic parameterizations and descriptions of these processes for inclusion in larger scale models that are used to determine their regional and global impacts.
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| 8. |
- Abdelkader, M., et al.
(författare)
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Dust-air pollution dynamics over the eastern Mediterranean
- 2015
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:16, s. 9173-9189
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Tidskriftsartikel (refereegranskat)abstract
- Interactions of desert dust and air pollution over the eastern Mediterranean (EM) have been studied, focusing on two distinct dust transport events on 22 and 28 September 2011. The atmospheric chemistry-climate model EMAC has been used at about 50 km grid spacing, applying an on-line dust emission scheme and calcium as a proxy for dust reactivity. EMAC includes a detailed tropospheric chemistry mechanism, aerosol microphysics and thermodynamics schemes to describe dust aging. The model is evaluated using ground-based observations for aerosol concentrations and aerosol optical depth (AOD) as well as satellite observations. Simulation results and back trajectory analysis show that the development of synoptic disturbances over the EM can enhance dust transport from the Sahara and Arabian deserts in frontal systems that also carry air pollution to the EM. The frontal systems are associated with precipitation that controls the dust removal. Our results show the importance of chemical aging of dust, which increases particle size, dust deposition and scavenging efficiency during transport, overall reducing the lifetime relative to non-aged dust particles. The relatively long travel periods of Saharan dust result in more sustained aging compared to Arabian dust. Sensitivity simulations indicate 3 times more dust deposition of aged relative to pristine dust, which significantly decreases the dust lifetime and loading.
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| 9. |
- Abdelkader, Mohamed, et al.
(författare)
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Sensitivity of transatlantic dust transport to chemical aging and related atmospheric processes
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:6, s. 3799-3821
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Tidskriftsartikel (refereegranskat)abstract
- We present a sensitivity study on transatlantic dust transport, a process which has many implications for the atmosphere, the ocean and the climate. We investigate the impact of key processes that control the dust outflow, i.e., the emission flux, convection schemes and the chemical aging of mineral dust, by using the EMAC model following Abdelkader et al. (2015). To characterize the dust outflow over the Atlantic Ocean, we distinguish two geographic zones: (i) dust interactions within the Intertropical Convergence Zone (ITCZ), or the dust-ITCZ interaction zone (DIZ), and (ii) the adjacent dust transport over the Atlantic Ocean (DTA) zone. In the latter zone, the dust loading shows a steep and linear gradient westward over the Atlantic Ocean since particle sedimentation is the dominant removal process, whereas in the DIZ zone aerosol-cloud interactions, wet deposition and scavenging processes determine the extent of the dust outflow. Generally, the EMAC simulated dust compares well with CALIPSO observations; however, our reference model configuration tends to overestimate the dust extinction at a lower elevation and underestimates it at a higher elevation. The aerosol optical depth (AOD) over the Caribbean responds to the dust emission flux only when the emitted dust mass is significantly increased over the source region in Africa by a factor of 10. These findings point to the dominant role of dust removal (especially wet deposition) in transatlantic dust transport. Experiments with different convection schemes have indeed revealed that the transatlantic dust transport is more sensitive to the convection scheme than to the dust emission flux parameterization. To study the impact of dust chemical aging, we focus on a major dust outflow in July 2009. We use the calcium cation as a proxy for the overall chemical reactive dust fraction and consider the uptake of major inorganic acids (i.e., H2SO4, HNO3 and HCl) and their anions, i.e., sulfate (SO42-), bisulfate (HSO4-), nitrate (NO 3) and chloride (Cl), on the surface of mineral particles. The subsequent neutralization reactions with the calcium cation form various salt compounds that cause the uptake of water vapor from the atmosphere, i.e., through the chemical aging of dust particles leading to an increase of 0.15 in the AOD under subsaturated conditions (July 2009 monthly mean). As a result of the radiative feedback on surface winds, dust emissions increased regionally. On the other hand, the aged dust particles, compared to the non-aged particles, are more efficiently removed by both wet and dry deposition due to the increased hygroscopicity and particle size (mainly due to water uptake). The enhanced removal of aged particles decreases the dust burden and lifetime, which indirectly reduces the dust AOD by 0.05 (monthly mean). Both processes can be significant (major dust outflow, July 2009), but the net effect depends on the region and level of dust chemical aging.
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| 10. |
- Achtert, Peggy, 1982-, et al.
(författare)
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On the linkage between tropospheric and Polar Stratospheric clouds in the Arctic as observed by space-borne lidar
- 2012
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:8, s. 3791-3798
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Tidskriftsartikel (refereegranskat)abstract
- The type of Polar stratospheric clouds (PSCs) as well as their temporal and spatial extent are important for the occurrence of heterogeneous reactions in the polar stratosphere. The formation of PSCs depends strongly on temperature. However, the mechanisms of the formation of solid PSCs are still poorly understood. Recent satellite studies of Antarctic PSCs have shown that their formation can be associated with deep-tropospheric clouds which have the ability to cool the lower stratosphere radiatively and/or adiabatically. In the present study, lidar measurements aboard the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite were used to investigate whether the formation of Arctic PSCs can be associated with deep-tropospheric clouds as well. Deep-tropospheric cloud systems have a vertical extent of more than 6.5 km with a cloud top height above 7 km altitude. PSCs observed by CALIPSO during the Arctic winter 2007/2008 were classified according to their type (STS, NAT, or ice) and to the kind of underlying tropospheric clouds. Our analysis reveals that 172 out of 211 observed PSCs occurred in connection with tropospheric clouds. 72% of these 172 observed PSCs occurred above deep-tropospheric clouds. We also find that the type of PSC seems to be connected to the characteristics of the underlying tropospheric cloud system. During the Arctic winter 2007/2008 PSCs consisting of ice were mainly observed in connection with deep-tropospheric cloud systems while no ice PSC was detected above cirrus. Furthermore, we find no correlation between the occurrence of PSCs and the top temperature of tropospheric clouds. Thus, our findings suggest that Arctic PSC formation is connected to adiabatice cooling, i.e. dynamic effects rather than radiative cooling.
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