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1.	Ahlm, Lars, et al. (author) Particle number concentrations over Europe in 2030 : the role of emissions and new particle formation 2013 In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 13:20, s. 10271-10283 Journal article (peer-reviewed)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
2.	Couvreux, Fleur, et al. (author) Boundary-layer turbulent processes and mesoscale variability represented by Numerical Weather Prediction models during the BLLAST campaign 2016 In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16:14, s. 8983-9002 Journal article (peer-reviewed)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.
3.	Nikulin, Grigory, et al. (author) The mean meridional circulation and midlatitude ozone buildup 2005 In: Atmospheric Chemistry and Physics Discussions. - Katlenburg-Lindau : European Geosciences Union (EGU). - 1680-7367 .- 1680-7375 .- 1680-7324. ; 5, s. 3159-3172 Journal article (peer-reviewed)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.
4.	Nilsson, Erik, 1983-, et al. (author) 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 In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16:14, s. 8849-8872 Journal article (peer-reviewed)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.
5.	Nilsson, Erik, 1983-, et al. (author) Turbulence Kinetic Energy budget during the afternoon transition – Part 2 : A simple TKE model 2016 In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16, s. 8873-8898 Journal article (peer-reviewed)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.
6.	Aas, W., et al. (author) Lessons learnt from the first EMEP intensive measurement periods 2012 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:17, s. 8073-8094 Journal article (peer-reviewed)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.
7.	Abbatt, J. P. D., et al. (author) Halogen activation via interactions with environmental ice and snow in the polar lower troposphere and other regions 2012 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:14, s. 6237-6271 Journal article (peer-reviewed)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.
8.	Abdelkader, M., et al. (author) Dust-air pollution dynamics over the eastern Mediterranean 2015 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:16, s. 9173-9189 Journal article (peer-reviewed)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.
9.	Abdelkader, Mohamed, et al. (author) Sensitivity of transatlantic dust transport to chemical aging and related atmospheric processes 2017 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:6, s. 3799-3821 Journal article (peer-reviewed)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.
10.	Achtert, Peggy, 1982-, et al. (author) On the linkage between tropospheric and Polar Stratospheric clouds in the Arctic as observed by space-borne lidar 2012 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:8, s. 3791-3798 Journal article (peer-reviewed)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.
11.	Achtert, Peggy, et al. (author) Properties of Arctic liquid and mixed-phase clouds from shipborne Cloudnet observations during ACSE 2014 2020 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:23, s. 14983-15002 Journal article (peer-reviewed)abstract This study presents Cloudnet retrievals of Arctic clouds from measurements conducted during a 3-month research expedition along the Siberian shelf during summer and autumn 2014. During autumn, we find a strong reduction in the occurrence of liquid clouds and an increase for both mixed-phase and ice clouds at low levels compared to summer. About 80 % of all liquid clouds observed during the research cruise show a liquid water path below the infrared black body limit of approximately 50 g m(-2). The majority of mixed-phase and ice clouds had an ice water path below 20 g m(-2). Cloud properties are analysed with respect to cloud-top temperature and boundary layer structure. Changes in these parameters have little effect on the geometric thickness of liquid clouds while mixed-phase clouds during warm-air advection events are generally thinner than when such events were absent. Cloud-top temperatures are very similar for all mixed-phase clouds. However, more cases of lower cloudtop temperature were observed in the absence of warm-air advection. Profiles of liquid and ice water content are normalized with respect to cloud base and height. For liquid water clouds, the liquid water content profile reveals a strong increase with height with a maximum within the upper quarter of the clouds followed by a sharp decrease towards cloud top. Liquid water content is lowest for clouds observed below an inversion during warm-air advection events. Most mixedphase clouds show a liquid water content profile with a very similar shape to that of liquid clouds but with lower maximum values during events with warm air above the planetary boundary layer. The normalized ice water content profiles in mixed-phase clouds look different from those of liquid water content. They show a wider range in maximum values with the lowest ice water content for clouds below an inversion and the highest values for clouds above or extending through an inversion. The ice water content profile generally peaks at a height below the peak in the liquid water content profile - usually in the centre of the cloud, sometimes closer to cloud base, likely due to particle sublimation as the crystals fall through the cloud.
12.	Adachi, Kouji, et al. (author) Composition and mixing state of Arctic aerosol and cloud residual particles from long-term sinale-particle observations at Zeppelin Observatory, Svalbard 2022 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:21, s. 14421-14439 Journal article (peer-reviewed)abstract The Arctic region is sensitive to climate change and is warming faster than the global average. Aerosol particles change cloud properties by acting as cloud condensation nuclei and ice-nucleating particles, thus influencing the Arctic climate system. Therefore, understanding the aerosol particle properties in the Arctic is needed to interpret and simulate their influences on climate. In this study, we collected ambient aerosol particles using whole-air and PM10 inlets and residual particles of cloud droplets and ice crystals from Arctic low-level clouds (typically, all-liquid or mixed-phase clouds) using a counterflow virtual impactor inlet at the Zeppelin Observatory near Ny-Ålesund, Svalbard, within a time frame of 4 years. We measured the composition and mixing state of individual fine-mode particles in 239 samples using transmission electron microscopy. On the basis of their composition, the aerosol and cloud residual particles were classified as mineral dust, sea salt, K-bearing, sulfate, and carbonaceous particles. The number fraction of aerosol particles showed seasonal changes, with sulfate dominating in summer and sea salt increasing in winter. There was no measurable difference in the fractions between ambient aerosol and cloud residual particles collected at ambient temperatures above 0 ∘C. On the other hand, cloud residual samples collected at ambient temperatures below 0 ∘C had several times more sea salt and mineral dust particles and fewer sulfates than ambient aerosol samples, suggesting that sea spray and mineral dust particles may influence the formation of cloud particles in Arctic mixed-phase clouds. We also found that 43 % of mineral dust particles from cloud residual samples were mixed with sea salt, whereas only 18 % of mineral dust particles in ambient aerosol samples were mixed with sea salt. This study highlights the variety in aerosol compositions and mixing states that influence or are influenced by aerosol–cloud interactions in Arctic low-level clouds.
13.	Agustí-Panareda, Anna, et al. (author) Modelling CO2 weather-why horizontal resolution matters 2019 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:11, s. 7347-7376 Journal article (peer-reviewed)abstract Climate change mitigation efforts require information on the current greenhouse gas atmospheric concentrations and their sources and sinks. Carbon dioxide (CO2) is the most abundant anthropogenic greenhouse gas. Its variability in the atmosphere is modulated by the synergy between weather and CO2 surface fluxes, often referred to as CO2 weather. It is interpreted with the help of global or regional numerical transport models, with horizontal resolutions ranging from a few hundreds of kilometres to a few kilometres. Changes in the model horizontal resolution affect not only atmospheric transport but also the representation of topography and surface CO2 fluxes. This paper assesses the impact of horizontal resolution on the simulated atmospheric CO2 variability with a numerical weather prediction model. The simulations are performed using the Copernicus Atmosphere Monitoring Service (CAMS) CO2 forecasting system at different resolutions from 9 to 80 km and are evaluated using in situ atmospheric surface measurements and atmospheric column-mean observations of CO2, as well as radiosonde and SYNOP observations of the winds. The results indicate that both diurnal and day-to-day variability of atmospheric CO2 are generally better represented at high resolution, as shown by a reduction in the errors in simulated wind and CO2. Mountain stations display the largest improvements at high resolution as they directly benefit from the more realistic orography. In addition, the CO2 spatial gradients are generally improved with increasing resolution for both stations near the surface and those observing the total column, as the overall inter-station error is also reduced in magnitude. However, close to emission hotspots, the high resolution can also lead to a deterioration of the simulation skill, highlighting uncertainties in the high-resolution fluxes that are more diffuse at lower resolutions. We conclude that increasing horizontal resolution matters for modelling CO2 weather because it has the potential to bring together improvements in the surface representation of both winds and CO2 fluxes, as well as an expected reduction in numerical errors of transport. Modelling applications like atmospheric inversion systems to estimate surface fluxes will only be able to benefit fully from upgrades in horizontal resolution if the topography, winds and prior flux distribution are also upgraded accordingly. It is clear from the results that an additional increase in resolution might reduce errors even further. However, the horizontal resolution sensitivity tests indicate that the change in the CO2 and wind modelling error with resolution is not linear, making it difficult to quantify the improvement beyond the tested resolutions. Finally, we show that the high-resolution simulations are useful for the assessment of the small-scale variability of CO2 which cannot be represented in coarser-resolution models. These representativeness errors need to be considered when assimilating in situ data and high-resolution satellite data such as Greenhouse gases Observing Satellite (GOSAT), Orbiting Carbon Observatory-2 (OCO-2), the Chinese Carbon Dioxide Observation Satellite Mission (TanSat) and future missions such as the Geostationary Carbon Observatory (GeoCarb) and the Sentinel satellite constellation for CO2. For these reasons, the high-resolution CO2 simulations provided by the CAMS in real time can be useful to estimate such small-scale variability in real time, as well as providing boundary conditions for regional modelling studies and supporting field experiments.
14.	Ahlberg, Erik, et al. (author) Effect of salt seed particle surface area, composition and phase on secondary organic aerosol mass yields in oxidation flow reactors 2019 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:4, s. 2701-2712 Journal article (peer-reviewed)abstract Atmospheric particulate water is ubiquitous, affecting particle transport and uptake of gases. Yet, research on the effect of water on secondary organic aerosol (SOA) mass yields is not consistent. In this study, the SOA mass yields of an α-pinene and m-xylene mixture, at a concentration of 60 μgm-3, were examined using an oxidation flow reactor operated at a relative humidity (RH) of 60% and a residence time of 160 s. Wet or dried ammonium sulfate and ammonium nitrate seed particles were used. By varying the amount of seed particle surface area, the underestimation of SOA formation induced by the short residence time in flow reactors was confirmed. Starting at a SOA mass concentration of 5 μgm-3, the maximum yield increased by a factor of 2 with dry seed particles and on average a factor of 3.2 with wet seed particles. Hence, wet particles increased the SOA mass yield by 60% compared to the dry experiment. Maximum yield in the reactor was achieved using a surface area concentration of 1600 μm2 cm-3. This corresponded to a condensational lifetime of 20 s for low-volatility organics. The O V C ratio of SOA on wet ammonium sulfate was significantly higher than when using ammonium nitrate or dry ammonium sulfate seed particles, probably due to differences in heterogeneous chemistry.
15.	Ahlberg, Erik, et al. (author) Measurement report : Black carbon properties and concentrations in southern Sweden urban and rural air-the importance of long-range transport 2023 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 23:5, s. 3051-3064 Journal article (peer-reviewed)abstract Soot, or black carbon (BC), aerosol is a major climate forcer with severe health effects. The impacts depend strongly on particle number concentration, size and mixing state. This work reports on two field campaigns at nearby urban and rural sites, 65gkm apart, in southern Sweden during late summer 2018. BC was measured using a single-particle soot photometer (SP2) and Aethalometers (AE33). Differences in BC concentrations between the sites are driven primarily by local traffic emissions. Equivalent and refractory BC mass concentrations at the urban site were on average a factor 2.2 and 2.5, with peaks during rush hour up to a factor g1/44, higher than the rural background levels. The number fraction of particles containing a soot core was significantly higher in the city. BC particles at the urban site were on average smaller by mass and had less coating owing to fresh traffic emissions. The organic components of the fresh traffic plumes were similar in mass spectral signature to hydrocarbon-like organic aerosol (HOA), commonly associated with traffic. Despite the intense local traffic (g1/4g30g000 vehicles passing per day), PM1, including organic aerosol, was dominated by aged continental air masses even at the curbside site. The fraction of thickly coated particles at the urban site was highly correlated with the mass concentrations of all measured chemical species of PM1, consistent with aged, internally mixed aerosol. Trajectory analysis for the whole year showed that air masses arriving at the rural site from eastern Europe contained approximately double the amount of BC compared to air masses from western Europe. Furthermore, the largest regional emissions of BC transported to the rural site, from the Malmö-Copenhagen urban area, are discernible above background levels only when precipitation events are excluded. We show that continental Europe and not the Malmö-Copenhagen region is the major contributor to the background BC mass concentrations in southern Sweden.
16.	Ahlm, Lars, 1976-, et al. (author) A comparison of dry and wet season aerosol number fluxes over the Amazon rain forest 2010 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:6, s. 3063-3079 Journal article (peer-reviewed)abstract Vertical number fluxes of aerosol particles and vertical fluxes of CO2 were measured with the eddy covariance method at the top of a 53m high tower in the Amazon rain forest as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) experiment. The observed aerosol number fluxes included particles with sizes down to 10 nm in diameter. The measurements were carried out during the wet and dry season in 2008. In this study focus is on the dry season aerosol fluxes, with significant influence from biomass burning, and these are compared with aerosol fluxes measured during the wet season. Net particle deposition fluxes dominated in daytime in both seasons and the deposition flux was considerably larger in the dry season due to the much higher dry season particle concentration. The particle transfer velocity increased linearly with increasing friction velocity in both seasons. The difference in transfer velocity between the two seasons was small, indicating that the seasonal change in aerosol number size distribution is not enough for causing any significant change in deposition velocity. In general, particle transfer velocities in this study are low compared to studies over boreal forests. The reasons are probably the high percentage of accumulation mode particles and the low percentage of nucleation mode particles in the Amazon boundary layer, both in the dry and wet season, and low wind speeds in the tropics compared to the midlatitudes. In the dry season, nocturnal particle fluxes behaved very similar to the nocturnal CO2 fluxes. Throughout the night, the measured particle flux at the top of the tower was close to zero, but early in the morning there was an upward particle flux peak that is not likely a result of entrainment or local pollution. It is possible that these morning upward particle fluxes are associated with emission of primary biogenic particles from the rain forest. Emitted particles may be stored within the canopy during stable conditions at nighttime, similarly to CO2, and being released from the canopy when conditions become more turbulent in the morning.
17.	Ahlm, Lars, 1976-, et al. (author) Aerosol number fluxes over the Amazon rain forest during the wet season 2009 In: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 9:24, s. 9381-9400 Journal article (peer-reviewed)abstract Number fluxes of particles with diameter larger than 10 nm were measured with the eddy covariance method over the Amazon rain forest during the wet season as part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) campaign 2008. The primary goal was to investigate whether sources or sinks dominate the aerosol number flux in the tropical rain forest-atmosphere system. During the measurement campaign, from 12 March to 18 May, 60% of the particle fluxes pointed downward, which is a similar fraction to what has been observed over boreal forests. The net deposition flux prevailed even in the absolute cleanest atmospheric conditions during the campaign and therefore cannot be explained only by deposition of anthropogenic particles. The particle transfer velocity vt increased with increasing friction velocity and the relation is described by the equation vt=2.4×10−3×u* where u* is the friction velocity. Upward particle fluxes often appeared in the morning hours and seem to a large extent to be an effect of entrainment fluxes into a growing mixed layer rather than primary aerosol emission. In general, the number source of primary aerosol particles within the footprint area of the measurements was small, possibly because the measured particle number fluxes reflect mostly particles less than approximately 200 nm. This is an indication that the contribution of primary biogenic aerosol particles to the aerosol population in the Amazon boundary layer may be low in terms of number concentrations. However, the possibility of horizontal variations in primary aerosol emission over the Amazon rain forest cannot be ruled out.
18.	Ahlm, Lars, et al. (author) Emission and dry deposition of accumulation mode particles in the Amazon Basin 2010 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 10:21, s. 10237-10253 Journal article (peer-reviewed)abstract Size-resolved vertical aerosol number fluxes of particles in the diameter range 0.25–2.5 μm were measured with the eddy covariance method from a 53 m high tower over the Amazon rain forest, 60 km NNW of Manaus, Brazil. This study focuses on data measured during the relatively clean wet season, but a shorter measurement period from the more polluted dry season is used as a comparison. Size-resolved net particle fluxes of the five lowest size bins, representing 0.25–0.45 μm in diameter, pointed downward in more or less all wind sectors in the wet season. This is an indication that the source of primary biogenic aerosol particles may be small in this particle size range. In the diameter range 0.5–2.5 μm, vertical particle fluxes were highly dependent on wind direction. In wind sectors where anthropogenic influence was low, net emission fluxes dominated. However, in wind sectors associated with higher anthropogenic influence, net deposition fluxes dominated. The net emission fluxes were interpreted as primary biogenic aerosol emission, but deposition of anthropogenic particles seems to have masked this emission in wind sectors with higher anthropogenic influence. The emission fluxes were at maximum in the afternoon when the mixed layer is well developed, and these emissions were best correlated with horizontal wind speed by the equation log10F=0.47·U+2.26 where F is the emission number flux of 0.5–2.5 μm particles [m−2s−1] and U is the horizontal wind speed [ms−1] at the top of the tower.
19.	Ahlm, Lars, et al. (author) Marine cloud brightening - as effective without clouds 2017 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:21, s. 13071-13087 Journal article (peer-reviewed)abstract Marine cloud brightening through sea spray injection has been proposed as a climate engineering method for avoiding the most severe consequences of global warming. A limitation of most of the previous modelling studies on marine cloud brightening is that they have either considered individual models or only investigated the effects of a specific increase in the number of cloud droplets. Here we present results from coordinated simulations with three Earth system models (ESMs) participating in the Geoengineering Model Intercomparison Project (GeoMIP) G4sea-salt experiment. Injection rates of accumulation-mode sea spray aerosol particles over ocean between 30 degrees N and 30 degrees S are set in each model to generate a global-mean effective radiative forcing (ERF) of -2.0 W m(-2) at the top of the atmosphere. We find that the injection increases the cloud droplet number concentration in lower layers, reduces the cloud-top effective droplet radius, and increases the cloud optical depth over the injection area. We also find, however, that the global-mean clear-sky ERF by the injected particles is as large as the corresponding total ERF in all three ESMs, indicating a large potential of the aerosol direct effect in regions of low cloudiness. The largest enhancement in ERF due to the presence of clouds occur as expected in the subtropical stratocumulus regions off the west coasts of the American and African continents. However, outside these regions, the ERF is in general equally large in cloudy and clear-sky conditions. These findings suggest a more important role of the aerosol direct effect in sea spray climate engineering than previously thought.
20.	Alastuey, Andres, et al. (author) Geochemistry of PM10 over Europe during the EMEP intensive measurement periods in summer 2012 and winter 2013 2016 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:10, s. 6107-6129 Journal article (peer-reviewed)abstract The third intensive measurement period (IMP) organised by the European Monitoring and Evaluation Programme (EMEP) under the UNECE CLTRAP took place in summer 2012 and winter 2013, with PM10 filter samples concurrently collected at 20 (16 EMEP) regional background sites across Europe for subsequent analysis of their mineral dust content. All samples were analysed by the same or a comparable methodology. Higher PM10 mineral dust loadings were observed at most sites in summer (0.5-10aEuro-A mu gaEuro-m(-3)) compared to winter (0.2-2aEuro-A mu gaEuro-m(-3)), with the most elevated concentrations in the southern- and easternmost countries, accounting for 20-40aEuro-% of PM10. Saharan dust outbreaks were responsible for the high summer dust loadings at western and central European sites, whereas regional or local sources explained the elevated concentrations observed at eastern sites. The eastern Mediterranean sites experienced elevated levels due to African dust outbreaks during both summer and winter. The mineral dust composition varied more in winter than in summer, with a higher relative contribution of anthropogenic dust during the former period. A relatively high contribution of K from non-mineral and non-sea-salt sources, such as biomass burning, was evident in winter at some of the central and eastern European sites. The spatial distribution of some components and metals reveals the influence of specific anthropogenic sources on a regional scale: shipping emissions (V, Ni, and SO42-) in the Mediterranean region, metallurgy (Cr, Ni, and Mn) in central and eastern Europe, high temperature processes (As, Pb, and SO42-) in eastern countries, and traffic (Cu) at sites affected by emissions from nearby cities.
21.	Aliaga, Diego, et al. (author) Identifying source regions of air masses sampled at the tropical high-altitude site of Chacaltaya using WRF-FLEXPART and cluster analysis 2021 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:21, s. 16453-16477 Journal article (peer-reviewed)abstract Observations of aerosol and trace gases in the remote troposphere are vital to quantify background concentrations and identify long-term trends in atmospheric composition on large spatial scales. Measurements made at high altitude are often used to study free-tropospheric air; however such high-altitude sites can be influenced by boundary layer air masses. Thus, accurate information on air mass origin and transport pathways to high-altitude sites is required. Here we present a new method, based on the source-receptor relationship (SRR) obtained from backwards WRF-FLEXPART simulations and a k-means clustering approach, to identify source regions of air masses arriving at measurement sites. Our method is tailored to areas of complex terrain and to stations influenced by both local and long-range sources. We have applied this method to the Chacaltaya (CHC) GAW station (5240 m a.s.l.; 16.35 degrees S, 68.13 degrees W) for the 6-month duration of the Southern Hemisphere high-altitude experiment on particle nucleation and growth (SALILNA) to identify where sampled air masses originate and to quantify the influence of the surface and the free troposphere. A key aspect of our method is that it is probabilistic, and for each observation time, more than one air mass (cluster) can influence the station, and the percentage influence of each air mass can be quantified. This is in contrast to binary methods, which label each observation time as influenced by either boundary layer or free-troposphere air masses. Air sampled at CHC is a mix of different provenance. We find that on average 9 % of the air, at any given observation time, has been in contact with the surface within 4 d prior to arriving at CHC. Furthermore, 24 % of the air has been located within the first 1.5 km above ground level (surface included). Consequently, 76 % of the air sampled at CHC originates from the free troposphere. However, pure free-tropospheric influences are rare, and often samples are concurrently influenced by both boundary layer and free-tropospheric air masses. A clear diurnal cycle is present, with very few air masses that have been in contact with the surface being detected at night. The 6-month analysis also shows that the most dominant air mass (cluster) originates in the Amazon and is responsible for 29 % of the sampled air. Furthermore, short-range clusters (origins within 100 km of CHC) have high temporal frequency modulated by local meteorology driven by the diurnal cycle, whereas the mid- and long-range clusters' (> 200 km) variability occurs on timescales governed by synoptic-scale dynamics. To verify the reliability of our method, in situ sulfate observations from CHC are combined with the SRR clusters to correctly identify the (pre-known) source of the sulfate: the Sabancaya volcano located 400 km north-west from the station.
22.	Allen, G., et al. (author) South East Pacific atmospheric composition and variability sampled = ong 20 degrees S during VOCALS-REx 2011 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:11, s. 5237-5262 Journal article (peer-reviewed)abstract The VAMOS Ocean-Cloud-Atmosphere-Land Regional Experiment (VOCALS-REx) was conducted from 15 October to 15 November 2008 in the South East Pacific (SEP) region to investigate interactions between land, sea and atmosphere in this unique tropical eastern ocean environment and to improve the skill of global and regional models in = presenting the region. This study synthesises selected aircraft, ship = d surface site observations from VOCALS-REx to statistically summarise = d characterise the atmospheric composition and variability of the = rine Boundary Layer (MBL) and Free Troposphere (FT) along the 20 = grees S parallel between 70 degrees W and 85 degrees W. Significant = nal gradients in mean MBL sub-micron aerosol particle size and = mposition, carbon monoxide, sulphur dioxide and ozone were seen over = e campaign, with a generally more variable and polluted coastal = vironment and a less variable, more pristine remote maritime regime. = adients in aerosol and trace gas concentrations were observed to be = sociated with strong gradients in cloud droplet number. The FT was = ten more polluted in terms of trace gases than the MBL in the mean; = wever increased variability in the FT composition suggests an episodic = ture to elevated concentrations. This is consistent with a complex = rtical interleaving of airmasses with diverse sources and hence = llutant concentrations as seen by generalised back trajectory = alysis, which suggests contributions from both local and long-range = urces. Furthermore, back trajectory analysis demonstrates that the = served zonal gradients both in the boundary layer and the free = oposphere are characteristic of marked changes in airmass history with = stance offshore - coastal boundary layer airmasses having been in = cent contact with the local land surface and remote maritime airmasses = ving resided over ocean for in excess of ten days. Boundary layer = mposition to the east of 75 degrees W was observed to be dominated by = astal emissions from sources to the west of the Andes, with evidence = r diurnal pumping of the Andean boundary layer above the height of the = rine capping inversion. Analysis of intra-campaign variability in = mospheric composition was not found to be significantly correlated = th observed low-frequency variability in the large scale flow pattern; = mpaign-average interquartile ranges of CO, SO(2) and O(3) = ncentrations at all longitudes were observed to dominate over much = aller differences in median concentrations calculated between periods = different flow regimes. The campaign climatology presented here aims = provide a valuable dataset to inform model simulation and future = ocess studies, particularly in the context of aerosol-cloud = teraction and further evaluation of dynamical processes in the SEP = gion for conditions analogous to those during VOCALS-REx. To this end, = r results are discussed in terms of coastal, transitional and remote = atial regimes in the MBL and FT and a gridded dataset are provided as = resource.
23.	Andersson, August, et al. (author) Seasonal source variability of carbonaceous aerosols at the Rwanda Climate Observatory 2020 In: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:8, s. 4561-4573 Journal article (peer-reviewed)abstract Sub-Saharan Africa (SSA) is a global hot spot for aerosol emissions, which affect the regional climate and air quality. In this paper, we use ground-based observations to address the large uncertainties in the source-resolved emission estimation of carbonaceous aerosols. Ambient fine fraction aerosol was collected on filters at the high-altitude (2590 m a.s.1.) Rwanda Climate Observatory (RCO), a SSA background site, during the dry and wet seasons in 2014 and 2015. The concentrations of both the carbonaceous and inorganic ion components show a strong seasonal cycle, with highly elevated concentrations during the dry season. Source marker ratios, including carbon isotopes, show that the wet and dry seasons have distinct aerosol compositions. The dry season is characterized by elevated amounts of biomass burning products, which approach similar to 95 % for carbonaceous aerosols. An isotopic mass-balance estimate shows that the amount of the carbonaceous aerosol stemming from savanna fires may increase from 0.2 mu g m(-3) in the wet season up to 10 mu g m(-3) during the dry season. Based on these results, we quantitatively show that savanna fire is the key modulator of the seasonal aerosol composition variability at the RCO.
24.	Angelbratt, Jon, 1981, et al. (author) A new method to detect long term trends of methane (CH4) and nitrous oxide (N2O) total columns measured within the NDACC ground-based high resolution solar FTIR network 2011 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:13, s. 6167-6183 Journal article (peer-reviewed)abstract Total columns measured with the ground-based solar FTIR technique are highly variable in time due to atmospheric chemistry and dynamics in the atmosphere above the measurement station. In this paper, a multiple regression model with anomalies of air pressure, total columns of hydrogen fluoride (HF) and carbon monoxide (CO) and tropopause height are used to reduce the variability in the methane (CH(4)) and nitrous oxide (N(2)O) total columns to estimate reliable linear trends with as small uncertainties as possible. The method is developed at the Harestua station (60 degrees N, 11 degrees E, 600 ma.s.l.) and used on three other European FTIR stations, i.e. Jungfraujoch (47 degrees N, 8 degrees E, 3600 ma.s.l.), Zugspitze (47 degrees N, 11 degrees E, 3000 ma.s.l.), and Kiruna (68 degrees N, 20 degrees E, 400 ma.s.l.). Linear CH(4) trends between 0.13 +/- 0.01-0.25 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2009 period. A piecewise model with three separate linear trends, connected at change points, was used to estimate the short term fluctuations in the CH(4) total columns. This model shows a growth in 1996-1999 followed by a period of steady state until 2007. From 2007 until 2009 the atmospheric CH(4) amount increases between 0.57 +/- 0.22-1.15 +/- 0.17% yr(-1). Linear N(2)O trends between 0.19 +/- 0.01-0.40 +/- 0.02% yr(-1) were estimated for all stations in the 1996-2007 period, here with the strongest trend at Harestua and Kiruna and the lowest at the Alp stations. From the N(2)O total columns crude tropospheric and stratospheric partial columns were derived, indicating that the observed difference in the N(2)O trends between the FTIR sites is of stratospheric origin. This agrees well with the N(2)O measurements by the SMR instrument onboard the Odin satellite showing the highest trends at Harestua, 0.98 +/- 0.28% yr(-1), and considerably smaller trends at lower latitudes, 0.27 +/- 0.25% yr(-1). The multiple regression model was compared with two other trend methods, the ordinary linear regression and a Bootstrap algorithm. The multiple regression model estimated CH(4) and N(2)O trends that differed up to 31% compared to the other two methods and had uncertainties that were up to 300% lower. Since the multiple regression method were carefully validated this stresses the importance to account for variability in the total columns when estimating trend from solar FTIR data.
25.	Angelbratt, Jon, 1981, et al. (author) Carbon monoxide (CO) and ethane (C2H6) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model 2011 In: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:17, s. 9253-9269 Journal article (peer-reviewed)abstract Trends in the CO and C(2)H(6) partial columns (similar to 0-15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996-2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to -0.45 +/- 0.16%yr(-1), -1.00 +/- 0.24%yr(-1), -0.62 +/- 0.19%yr(-1) and -0.61 +/- 0.16%yr(-1), respectively. The corresponding trends for C(2)H(6) are -1.51 +/- 0.23%yr(-1), -2.11 +/- 0.30%yr(-1), -1.09 +/- 0.25%yr(-1) and -1.14 +/- 0.18%yr(-1). All trends are presented with their 2-sigma confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996-2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH(4) and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C(2)H(6) partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Alesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10-22% deviation for CO and 14-31% deviation for C(2)H(6). Their seasonal amplitude is captured within 6-35% and 9-124% for CO and C(2)H(6), respectively. However, 61-98% of the CO and C(2)H(6) partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1-9% and 37-50% of the measurements for CO and C(2)H(6), respectively. The global model sensitivity for assumptions made in this paper is also analyzed.

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