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1.	Abdelkader, M., et al. (författare) Dust-air pollution dynamics over the eastern Mediterranean 2015 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:16, s. 9173-9189 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.
2.	Abdelkader, Mohamed, et al. (författare) Sensitivity of transatlantic dust transport to chemical aging and related atmospheric processes 2017 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:6, s. 3799-3821 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.
3.	Agustí-Panareda, Anna, et al. (författare) Modelling CO2 weather-why horizontal resolution matters 2019 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:11, s. 7347-7376 Tidskriftsartikel (refereegranskat)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.
4.	Ahlberg, Erik, et al. (författare) Effect of salt seed particle surface area, composition and phase on secondary organic aerosol mass yields in oxidation flow reactors 2019 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:4, s. 2701-2712 Tidskriftsartikel (refereegranskat)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.
5.	Ahlm, Lars, et al. (författare) Marine cloud brightening - as effective without clouds 2017 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:21, s. 13071-13087 Tidskriftsartikel (refereegranskat)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.
6.	Alastuey, Andres, et al. (författare) Geochemistry of PM10 over Europe during the EMEP intensive measurement periods in summer 2012 and winter 2013 2016 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:10, s. 6107-6129 Tidskriftsartikel (refereegranskat)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.
7.	Angot, H., et al. (författare) Chemical cycling and deposition of atmospheric mercury in polar regions: review of recent measurements and comparison with models 2016 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:16, s. 10735-10763 Tidskriftsartikel (refereegranskat)abstract Mercury (Hg) is a worldwide contaminant that can cause adverse health effects to wildlife and humans. While atmospheric modeling traces the link from emissions to deposition of Hg onto environmental surfaces, large uncertainties arise from our incomplete understanding of atmospheric processes (oxidation pathways, deposition, and re-emission). Atmospheric Hg reactivity is exacerbated in high latitudes and there is still much to be learned from polar regions in terms of atmospheric processes. This paper provides a synthesis of the atmospheric Hg monitoring data available in recent years (2011-2015) in the Arctic and in Antarctica along with a comparison of these observations with numerical simulations using four cutting-edge global models. The cycle of atmospheric Hg in the Arctic and in Antarctica presents both similarities and differences. Coastal sites in the two regions are both influenced by springtime atmospheric Hg depletion events and by summertime snowpack re-emission and oceanic evasion of Hg. The cycle of atmospheric Hg differs between the two regions primarily because of their different geography. While Arctic sites are significantly influenced by northern hemispheric Hg emissions especially in winter, coastal Antarctic sites are significantly influenced by the reactivity observed on the East Antarctic ice sheet due to katabatic winds. Based on the comparison of multi-model simulations with observations, this paper discusses whether the processes that affect atmospheric Hg seasonality and inter-annual variability are appropriately represented in the models and identifies research gaps in our understanding of the atmospheric Hg cycling in high latitudes.
8.	Baars, Holger, et al. (författare) An overview of the first decade of Polly(NET) : an emerging network of automated Raman-polarization lidars for continuous aerosol profiling 2016 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:8, s. 5111-5137 Tidskriftsartikel (refereegranskat)abstract A global vertically resolved aerosol data set covering more than 10 years of observations at more than 20 measurement sites distributed from 63 degrees N to 52 degrees S and 72 degrees W to 124 degrees E has been achieved within the Raman and polarization lidar network Polly(NET). This network consists of portable, remote-controlled multiwavelength-polarization-Raman lidars (Polly) for automated and continuous 24/7 observations of clouds and aerosols. Polly(NET) is an independent, voluntary, and scientific network. All Polly lidars feature a standardized instrument design with different capabilities ranging from single wavelength to multiwavelength systems, and now apply unified calibration, quality control, and data analysis. The observations are processed in near-real time without manual intervention, and are presented online at polly.tropos.de. The paper gives an overview of the observations on four continents and two research vessels obtained with eight Polly systems. The specific aerosol types at these locations (mineral dust, smoke, dust-smoke and other dusty mixtures, urban haze, and volcanic ash) are identified by their Angstrom exponent, lidar ratio, and depolarization ratio. The vertical aerosol distribution at the Polly(NET) locations is discussed on the basis of more than 55 000 automatically retrieved 30 min particle backscatter coefficient profiles at 532 nm as this operating wavelength is available for all Polly lidar systems. A seasonal analysis of measurements at selected sites revealed typical and extraordinary aerosol conditions as well as seasonal differences. These studies show the potential of Polly(NET) to support the establishment of a global aerosol climatology that covers the entire troposphere.
9.	Babkovskaia, Natalia, et al. (författare) A DNS study of aerosol and small-scale cloud turbulence interaction 2016 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:12, s. 7889-7898 Tidskriftsartikel (refereegranskat)abstract The purpose of this study is to investigate the interaction between small-scale turbulence and aerosol and cloud microphysical properties using direct numerical simulations (DNS). We consider the domain located at the height of about 2000 m from the sea level, experiencing transient high supersaturation due to atmospheric fluctuations of temperature and humidity. To study the effect of total number of particles (Ntot) on air temperature, activation and supersaturation, we vary Ntot. To investigate the effect of aerosol dynamics on small-scale turbulence and vertical air motion, we vary the intensity of turbulent fluctuations and the buoyant force. We find that even a small number of aerosol particles (55.5 cm-3), and therefore a small droplet number concentration, strongly affects the air temperature due to release of latent heat. The system comes to an equilibrium faster and the relative number of activated particles appears to be smaller for larger Ntot. We conclude that aerosol particles strongly affect the air motion. In a case of updraught coursed by buoyant force, the presence of aerosol particles results in acceleration of air motion in vertical direction and increase of turbulent fluctuations.
10.	Ball, William T., et al. (författare) Evidence for a continuous decline in lower stratospheric ozone offsetting ozone layer recovery 2018 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:2, s. 1379-1394 Tidskriftsartikel (refereegranskat)abstract Ozone forms in the Earth's atmosphere from the photodissociation of molecular oxygen, primarily in the tropical stratosphere. It is then transported to the extratropics by the Brewer-Dobson circulation (BDC), forming a protective ozone layer around the globe. Human emissions of halogen-containing ozone-depleting substances (hODSs) led to a decline in stratospheric ozone until they were banned by the Montreal Protocol, and since 1998 ozone in the upper stratosphere is rising again, likely the recovery from halogen-induced losses. Total column measurements of ozone between the Earth's surface and the top of the atmosphere indicate that the ozone layer has stopped declining across the globe, but no clear increase has been observed at latitudes between 60 degrees S and 60 degrees N outside the polar regions (60-90 degrees). Here we report evidence from multiple satellite measurements that ozone in the lower stratosphere between 60 degrees S and 60 degrees N has indeed continued to decline since 1998. We find that, even though upper stratospheric ozone is recovering, the continuing downward trend in the lower stratosphere prevails, resulting in a downward trend in stratospheric column ozone between 60 degrees S and 60 degrees N. We find that total column ozone between 60 degrees S and 60 degrees N appears not to have decreased only because of increases in tropospheric column ozone that compensate for the stratospheric decreases. The reasons for the continued reduction of lower stratospheric ozone are not clear; models do not reproduce these trends, and thus the causes now urgently need to be established.
11.	Ball, William T., et al. (författare) Reconciling differences in stratospheric ozone composites 2017 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:20, s. 12269-12302 Tidskriftsartikel (refereegranskat)abstract Observations of stratospheric ozone from multiple instruments now span three decades; combining these into composite datasets allows long-term ozone trends to be estimated. Recently, several ozone composites have been published, but trends disagree by latitude and altitude, even between composites built upon the same instrument data. We confirm that the main causes of differences in decadal trend estimates lie in (i) steps in the composite time series when the instrument source data changes and (ii) artificial sub-decadal trends in the underlying instrument data. These artefacts introduce features that can alias with regressors in multiple linear regression (MLR) analysis; both can lead to inaccurate trend estimates. Here, we aim to remove these artefacts using Bayesian methods to infer the underlying ozone time series from a set of composites by building a joint-likelihood function using a Gaussian-mixture density to model outliers introduced by data artefacts, together with a data-driven prior on ozone variability that incorporates knowledge of problems during instrument operation. We apply this Bayesian self-calibration approach to stratospheric ozone in 10 degrees bands from 60 degrees S to 60 degrees N and from 46 to 1 hPa (similar to 21-48 km) for 1985-2012. There are two main outcomes: (i) we independently identify and confirm many of the data problems previously identified, but which remain unaccounted for in existing composites; (ii) we construct an ozone composite, with uncertainties, that is free from most of these problems - we call this the BAyeSian Integrated and Consolidated (BASIC) composite. To analyse the new BASIC composite, we use dynamical linear modelling (DLM), which provides a more robust estimate of long-term changes through Bayesian inference than MLR. BASIC and DLM, together, provide a step forward in improving estimates of decadal trends. Our results indicate a significant recovery of ozone since 1998 in the upper stratosphere, of both northern and southern midlatitudes, in all four composites analysed, and particularly in the BASIC composite. The BASIC results also show no hemispheric difference in the recovery at midlatitudes, in contrast to an apparent feature that is present, but not consistent, in the four composites. Our overall conclusion is that it is possible to effectively combine different ozone composites and account for artefacts and drifts, and that this leads to a clear and significant result that upper stratospheric ozone levels have increased since 1998, following an earlier decline.
12.	Ball, William T., et al. (författare) Stratospheric ozone trends for 1985-2018 : sensitivity to recent large variability 2019 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:19, s. 12731-12748 Tidskriftsartikel (refereegranskat)abstract The Montreal Protocol, and its subsequent amendments, has successfully prevented catastrophic losses of stratospheric ozone, and signs of recovery are now evident. Nevertheless, recent work has suggested that ozone in the lower stratosphere (< 24 km) continued to decline over the 1998-2016 period, offsetting recovery at higher altitudes and preventing a statistically significant increase in quasi-global (60 degrees S-60 degrees N) total column ozone. In 2017, a large lower stratospheric ozone resurgence over less than 12 months was estimated (using a chemistry transport model; CTM) to have offset the long-term decline in the quasi-global integrated lower stratospheric ozone column. Here, we extend the analysis of space-based ozone observations to December 2018 using the BASIC(SG) ozone composite. We find that the observed 2017 resurgence was only around half that modelled by the CTM, was of comparable magnitude to other strong interannual changes in the past, and was restricted to Southern Hemisphere (SH) midlatitudes (60-30 degrees S). In the SH midlatitude lower stratosphere, the data suggest that by the end of 2018 ozone is still likely lower than in 1998 (probability similar to 80 %). In contrast, tropical and Northern Hemisphere (NH) ozone continue to display ongoing decreases, exceeding 90 % probability. Robust tropical (> 95 %, 30 degrees S-30 degrees N) decreases dominate the quasi-global integrated decrease (99 % probability); the integrated tropical stratospheric column (1-100 hPa, 30 degrees S-30 degrees N) displays a significant overall ozone decrease, with 95 % probability. These decreases do not reveal an inefficacy of the Montreal Protocol; rather, they suggest that other effects are at work, mainly dynamical variability on long or short timescales, counteracting the positive effects of the Montreal Protocol on stratospheric ozone recovery. We demonstrate that large interannual midlatitude (30-60 degrees) variations, such as the 2017 resurgence, are driven by non-linear quasi-biennial oscillation (QBO) phase-dependent seasonal variability. However, this variability is not represented in current regression analyses. To understand if observed lower stratospheric ozone decreases are a transient or long-term phenomenon, progress needs to be made in accounting for this dynamically driven variability.
13.	Beecken, Jörg, 1982, et al. (författare) Emission factors of SO2, NOx and particles from ships in Neva Bay from ground-based and helicopter-borne measurements and AIS-based modeling 2015 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:9, s. 5229-5241 Tidskriftsartikel (refereegranskat)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.
14.	Berthet, Gwenaël, et al. (författare) Impact of a moderate volcanic eruption on chemistry in the lower stratosphere : balloon-borne observations and model calculations 2017 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:3, s. 2229-2253 Tidskriftsartikel (refereegranskat)abstract The major volcanic eruption of Mount Pinatubo in 1991 has been shown to have significant effects on stratospheric chemistry and ozone depletion even at midlatitudes. Since then, only moderate but recurrent volcanic eruptions have modulated the stratospheric aerosol loading and are assumed to be one cause for the reported increase in the global aerosol content over the past 15 years. This particularly enhanced aerosol context raises questions about the effects on stratospheric chemistry which depend on the latitude, altitude and season of injection. In this study, we focus on the midlatitude Sarychev volcano eruption in June 2009, which injected 0.9 Tg of sulfur dioxide (about 20 times less than Pinatubo) into a lower stratosphere mainly governed by high-stratospheric temperatures. Together with in situ measurements of aerosol amounts, we analyse high-resolution in situ and/or remote-sensing observations of NO2, HNO3 and BrO from balloon-borne infrared and UV-visible spectrometers launched in Sweden in August-September 2009. It is shown that differences between observations and three-dimensional (3-D) chemistry-transport model (CTM) outputs are not due to transport calculation issues but rather reflect the chemical impact of the volcanic plume below 19 km altitude. Good measurement-model agreement is obtained when the CTM is driven by volcanic aerosol loadings derived from in situ or space-borne data. As a result of enhanced N2O5 hydrolysis in the Sarychev volcanic aerosol conditions, the model calculates reductions of similar to 45% and increases of similar to 11% in NO2 and HNO3 amounts respectively over the August-September 2009 period. The decrease in NOx abundances is limited due to the expected saturation effect for high aerosol loadings. The links between the various chemical catalytic cycles involving chlorine, bromine, nitrogen and HOx compounds in the lower stratosphere are discussed. The increased BrO amounts (similar to 22 %) compare rather well with the balloon-borne observations when volcanic aerosol levels are accounted for in the CTM and appear to be mainly controlled by the coupling with nitrogen chemistry rather than by enhanced BrONO2 hydrolysis. We show that the chlorine partitioning is significantly controlled by enhanced BrONO2 hydrolysis. However, simulated effects of the Sarychev eruption on chlorine activation are very limited in the high-temperature conditions in the stratosphere in the period considered, inhibiting the effect of ClONO2 hydrolysis. As a consequence, the simulated chemical ozone loss due to the Sarychev aerosols is low with a reduction of -22 ppbv (-1.5 %) of the ozone budget around 16 km. This is at least 10 times lower than the maximum ozone depletion from chemical processes (up to -20 %) reported in the Northern Hemisphere lower stratosphere over the first year following the Pinatubo eruption. This study suggests that moderate volcanic eruptions have limited chemical effects when occurring at midlatitudes (restricted residence times) and outside winter periods (high-temperature conditions). However, it would be of interest to investigate longer-lasting tropical volcanic plumes or sulfur injections in the wintertime low-temperature conditions.
15.	Bidleman, Terry Frank, et al. (författare) Annual cycles of organochlorine pesticide enantiomers in Arctic air suggest changing sources and pathways 2015 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:3, s. 1411-1420 Tidskriftsartikel (refereegranskat)abstract Air samples collected during 1994-2000 at the Canadian Arctic air monitoring station Alert (82 degrees 30'N, 62 degrees 20'W) were analysed by enantiospecific gas chromatography-mass spectrometry for alpha-hexachlorocyclohexane (alpha-HCH), trans-chlordane (TC) and cis-chlordane (CC). Results were expressed as enantiomer fractions (EF = peak areas of (+)/[(+) + (-)] enantiomers), where EFs = 0.5, <0.5 and >0.5 indicate racemic composition, and preferential depletion of (+) and (-) enantiomers, respectively. Long-term average EFs were close to racemic values for alpha-HCH (0.504 +/- 0.004, n = 197) and CC (0.505 +/- 0.004, n = 162), and deviated farther from racemic for TC (0.470 +/- 0.013, n = 165). Digital filtration analysis revealed annual cycles of lower alpha-HCH EFs in summer-fall and higher EFs in winter-spring. These cycles suggest volatilization of partially degraded alpha-HCH with EF < 0.5 from open water and advection to Alert during the warm season, and background transport of alpha-HCH with EF > 0.5 during the cold season. The contribution of sea-volatilized alpha-HCH was only 11% at Alert, vs. 32% at Resolute Bay (74.68 degrees N, 94.90 degrees W) in 1999. EFs of TC also followed annual cycles of lower and higher values in the warm and cold seasons. These were in phase with low and high cycles of the TC / CC ratio (expressed as F-TC = TC/(TC + CC)), which suggests greater contribution of microbially "weathered" TC in summer-fall versus winter-spring. CC was closer to racemic than TC and displayed seasonal cycles only in 1997-1998. EF profiles are likely to change with rising contribution of secondary emission sources, weathering of residues in the environment, and loss of ice cover in the Arctic. Enantiomer-specific analysis could provide added forensic capability to air monitoring programs.
16.	Bolinius, Damien Johann, et al. (författare) Comparison of eddy covariance and modified Bowen ratio methods for measuring gas fluxes and implications for measuring fluxes of persistent organic pollutants 2016 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:8, s. 5315-5322 Tidskriftsartikel (refereegranskat)abstract Semi-volatile persistent organic pollutants (POPs) cycle between the atmosphere and terrestrial surfaces; however measuring fluxes of POPs between the atmosphere and other media is challenging. Sampling times of hours to days are required to accurately measure trace concentrations of POPs in the atmosphere, which rules out the use of eddy covariance techniques that are used to measure gas fluxes of major air pollutants. An alternative, the modified Bowen ratio (MBR) method, has been used instead. In this study we used data from FLUXNET for CO2 and water vapor (H2O) to compare fluxes measured by eddy covariance to fluxes measured with the MBR method using vertical concentration gradients in air derived from averaged data that simulate the long sampling times typically required to measure POPs. When concentration gradients are strong and fluxes are unidirectional, the MBR method and the eddy covariance method agree within a factor of 3 for CO2, and within a factor of 10 for H2O. To remain within the range of applicability of the MBR method, field studies should be carried out under conditions such that the direction of net flux does not change during the sampling period. If that condition is met, then the performance of the MBR method is neither strongly affected by the length of sample duration nor the use of a fixed value for the transfer coefficient.
17.	Bourgeois, Quentin, et al. (författare) How much of the global aerosol optical depth is found in the boundary layer and free troposphere? 2018 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:10, s. 7709-7720 Tidskriftsartikel (refereegranskat)abstract The global aerosol extinction from the CALIOP space lidar was used to compute aerosol optical depth (AOD) over a 9-year period (2007-2015) and partitioned between the boundary layer (BL) and the free troposphere (FT) using BL heights obtained from the ERA-Interim archive. The results show that the vertical distribution of AOD does not follow the diurnal cycle of the BL but remains similar between day and night highlighting the presence of a residual layer during night. The BL and FT contribute 69 and 31 %, respectively, to the global tropospheric AOD during daytime in line with observations obtained in Aire sur l'Adour (France) using the Light Optical Aerosol Counter (LOAC) instrument. The FT AOD contribution is larger in the tropics than at mid-latitudes which indicates that convective transport largely controls the vertical profile of aerosols. Over oceans, the FT AOD contribution is mainly governed by long-range transport of aerosols from emission sources located within neighboring continents. According to the CALIOP aerosol classification, dust and smoke particles are the main aerosol types transported into the FT. Overall, the study shows that the fraction of AOD in the FT - and thus potentially located above low-level clouds - is substantial and deserves more attention when evaluating the radiative effect of aerosols in climate models. More generally, the results have implications for processes determining the overall budgets, sources, sinks and transport of aerosol particles and their description in atmospheric models.
18.	Boy, M., et al. (författare) Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes 2019 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:3, s. 2015-2061 Tidskriftsartikel (refereegranskat)abstract The Nordic Centre of Excellence CRAICC (Cryosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change-cryosphere interactions that affect Arctic amplification.
19.	Broman, Lina, et al. (författare) Common volume satellite studies of polar mesospheric clouds with Odin/OSIRIS tomography and AIM/CIPS nadir imaging 2019 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:19, s. 12455-12475 Tidskriftsartikel (refereegranskat)abstract Two important approaches for satellite studies of polar mesospheric clouds (PMCs) are nadir measurements adapting phase function analysis and limb measurements adapting spectroscopic analysis. Combining both approaches enables new studies of cloud structures and microphysical processes but is complicated by differences in scattering conditions, observation geometry and sensitivity. In this study, we compare common volume PMC observations from the nadir-viewing Cloud Imaging and Particle Size (CIPS) instrument on the Aeronomy of Ice in the Mesosphere (AIM) satellite and a special set of tomographic limb observations from the Optical Spectrograph and InfraRed Imager System (OSIRIS) on the Odin satellite performed over 18 d for the years 2010 and 2011 and the latitude range 78 to 80 degrees N. While CIPS provides preeminent horizontal resolution, the OSIRIS tomographic analysis provides combined horizontal and vertical PMC information. This first direct comparison is an important step towards co-analysing CIPS and OSIRIS data, aiming at unprecedented insights into horizontal and vertical cloud processes. Important scientific questions on how the PMC life cycle is affected by changes in humidity and temperature due to atmospheric gravity waves, planetary waves and tides can be addressed by combining PMC observations in multiple dimensions. Two- and three-dimensional cloud structures simultaneously observed by CIPS and tomographic OSIRIS provide a useful tool for studies of cloud growth and sublimation Moreover, the combined CIPS/tomographic OSIRIS dataset can be used for studies of even more fundamental character, such as the question of the assumption of the PMC particle size distribution. We perform the first thorough error characterization of OSIRIS tomographic cloud brightness and cloud ice water content (IWC). We establish a consistent method for comparing cloud properties from limb tomography and nadir observations, accounting for differences in scattering conditions, resolution and sensitivity. Based on an extensive common volume and a temporal coincidence criterion of only 5 min, our method enables a detailed comparison of PMC regions of varying brightness and IWC. However, since the dataset is limited to 18 d of observations this study does not include a comparison of cloud frequency. The cloud properties of the OSIRIS tomographic dataset are vertically resolved, while the cloud properties of the CIPS dataset is vertically integrated. To make these different quantities comparable, the OSIRIS tomographic cloud properties cloud scattering coefficient and ice mass density (IMD) have been integrated over the vertical extent of the cloud to form cloud albedo and IWC of the same quantity as CIPS cloud products. We find that the OSIRIS albedo (obtained from the vertical integration of the primary OSIRIS tomography product, cloud scattering coefficient) shows very good agreement with the primary CIPS product, cloud albedo, with a correlation coefficient of 0.96. However, OSIRIS systematically reports brighter clouds than CIPS and the bias between the instruments (OSIRIS -CIPS) is 3.4 x 10(-6) sr(-1) (+/- 2.9x 10(-6) sr(-1)) on average. The OSIRIS tomography IWC (obtained from the vertical integration of IMD) agrees well with the CIPS IWC, with a correlation coefficient of 0.91. However, the IWC reported by OSIRIS is lower than CIPS, and we quantify the bias to -22 g km(-2) (+/- 14 g km(-2)) on average.
20.	Buchholz, Angela, et al. (författare) Insights into the O : C-dependent mechanisms controlling the evaporation of alpha-pinene secondary organic aerosol particles 2019 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:6, s. 4061-4073 Tidskriftsartikel (refereegranskat)abstract The volatility of oxidation products of volatile organic compounds (VOCs) in the atmosphere is a key factor to determine if they partition into the particle phase contributing to secondary organic aerosol (SOA) mass. Thus, linking volatility and measured particle composition will provide insights into SOA formation and its fate in the atmosphere. We produced alpha-pinene SOA with three different oxidation levels (characterized by average oxygen-to-carbon ratio; (O:C) over bar = 0.53, 0.69, and 0.96) in an oxidation flow reactor. We investigated the particle volatility by isothermal evaporation in clean air as a function of relative humidity (RH < 2 %, 40 %, and 80 %) and used a filter-based thermal desorption method to gain volatility and chemical composition information. We observed reduced particle evaporation for particles with increasing <(O:C )over bar> ratio, indicating that particles become more resilient to evaporation with oxidative aging. Particle evaporation was increased in the presence of water vapour and presumably particulate water; at the same time the resistance of the residual particles to thermal desorption was increased as well. For SOA with (O:C ) over bar = 0.96, the unexpectedly large increase in mean thermal desorption temperature and changes in the thermogram shapes under wet conditions (80 % RH) were an indication of aqueous phase chemistry. For the lower (O:C ) over bar cases, some water-induced composition changes were observed. However, the enhanced evaporation under wet conditions could be explained by the reduction in particle viscosity from the semi-solid to liquid-like range, and the observed higher desorption temperature of the residual particles is a direct consequence of the increased removal of high-volatility and the continued presence of low-volatility compounds.
21.	Burton, S. P., et al. (författare) Observations of the spectral dependence of linear particle depolarization ratio of aerosols using NASA Langley airborne High Spectral Resolution Lidar 2015 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:23, s. 13453-13473 Tidskriftsartikel (refereegranskat)abstract Linear particle depolarization ratio is presented for three case studies from the NASA Langley airborne High Spectral Resolution Lidar-2 (HSRL-2). Particle depolarization ratio from lidar is an indicator of non-spherical particles and is sensitive to the fraction of non-spherical particles and their size. The HSRL-2 instrument measures depolarization at three wavelengths: 355, 532, and 1064 nm. The three measurement cases presented here include two cases of dust-dominated aerosol and one case of smoke aerosol. These cases have partial analogs in earlier HSRL-1 depolarization measurements at 532 and 1064 nm and in literature, but the availability of three wavelengths gives additional insight into different scenarios for non-spherical particles in the atmosphere. A case of transported Saharan dust has a spectral dependence with a peak of 0.30 at 532 nm with smaller particle depolarization ratios of 0.27 and 0.25 at 1064 and 355 nm, respectively. A case of aerosol containing locally generated wind-blown North American dust has a maximum of 0.38 at 1064 nm, decreasing to 0.37 and 0.24 at 532 and 355 nm, respectively. The cause of the maximum at 1064 nm is inferred to be very large particles that have not settled out of the dust layer. The smoke layer has the opposite spectral dependence, with the peak of 0.24 at 355 nm, decreasing to 0.09 and 0.02 at 532 and 1064 nm, respectively. The depolarization in the smoke case may be explained by the presence of coated soot aggregates. We note that in these specific case studies, the linear particle depolarization ratio for smoke and dust-dominated aerosol are more similar at 355 nm than at 532 nm, having possible implications for using the particle depolarization ratio at a single wavelength for aerosol typing.
22.	Castarède, Dimitri, et al. (författare) A thermodynamic description for the hygroscopic growth of atmospheric aerosol particles 2018 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:20, s. 14939-14948 Tidskriftsartikel (refereegranskat)abstract The phase state of atmospheric particulate is important to atmospheric processes, and aerosol radiative forcing remains a large uncertainty in climate predictions. That said, precise atmospheric phase behavior is difficult to quantify and observations have shown that "precondensation" of water below predicted saturation values can occur. We propose a revised approach to understanding the transition from solid soluble particles to liquid droplets, typically described as cloud condensation nucleation - a process that is traditionally captured by Kohler theory, which describes a modified equilibrium saturation vapor pressure due to (i) mixing entropy (Raoult's law) and (ii) droplet geometry (Kelvin effect). Given that observations of precondensation are not predicted by Kohler theory, we devise a more complete model that includes interfacial forces giving rise to predeliquescence, i.e., the formation of a brine layer wetting a salt particle at relative humidities well below the deliquescence point.
23.	Chauvigné, Aurélien, et al. (författare) Biomass burning and urban emission impacts in the Andes Cordillera region based on in situ measurements from the Chacaltaya observatory, Bolivia (5240 m a.s.l.) 2019 Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:23, s. 14805-14824 Tidskriftsartikel (refereegranskat)abstract This study documents and analyses a 4-year continuous record of aerosol optical properties measured at the Global Atmosphere Watch (GAW) station of Chacaltaya (CHC; 5240 m a.s.l.), in Bolivia. Records of particle light scattering and particle light absorption coefficients are used to investigate how the high Andean Cordillera is affected by both long-range transport and by the fast-growing agglomeration of La Paz-El Alto, located approximately 20 km away and 1.5 km below the sampling site. The extended multiyear record allows us to study the properties of aerosol particles for different air mass types, during wet and dry seasons, also covering periods when the site was affected by biomass burning in the Bolivian lowlands and the Amazon Basin. The absorption, scattering, and extinction coefficients (median annual values of 0.74, 12.14, and 12.96 Mm(-1) respectively) show a clear seasonal variation with low values during the wet season (0.57, 7.94, and 8.68 Mm(-1) respectively) and higher values during the dry season (0.80, 11.23, and 14.51 Mm(-1) respectively). The record is driven by variability at both seasonal and diurnal scales. At a diurnal scale, all records of intensive and extensive aerosol properties show a pronounced variation (daytime maximum, night-time minimum), as a result of the dynamic and convective effects. The particle light absorption, scattering, and extinction coefficients are on average 1.94, 1.49, and 1.55 times higher respectively in the turbulent thermally driven conditions than the more stable conditions, due to more efficient transport from the boundary layer. Retrieved intensive optical properties are significantly different from one season to the other, reflecting the changing aerosol emission sources of aerosol at a larger scale. Using the wavelength dependence of aerosol particle optical properties, we discriminated between contributions from natural (mainly mineral dust) and anthropogenic (mainly biomass burning and urban transport or industries) emissions according to seasons and local circulation. The main sources influencing measurements at CHC are from the urban area of La Paz-El Alto in the Altiplano and from regional biomass burning in the Amazon Basin. Results show a 28 % to 80 % increase in the extinction coefficients during the biomass burning season with respect to the dry season, which is observed in both tropospheric dynamic conditions. From this analysis, long-term observations at CHC provide the first direct evidence of the impact of biomass burning emissions of the Amazon Basin and urban emissions from the La Paz area on atmospheric optical properties at a remote site all the way to the free troposphere.
24.	Chen, J., et al. (författare) Ice-nucleating particle concentrations unaffected by urban air pollution in Beijing, China 2018 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 18:5, s. 3523-3539 Tidskriftsartikel (refereegranskat)abstract Exceedingly high levels of PM2.5 with complex chemical composition occur frequently in China. It has been speculated whether anthropogenic PM2.5 may significantly contribute to ice-nucleating particles (INP). However, few studies have focused on the ice-nucleating properties of urban particles. In this work, two ice-nucleating droplet arrays have been used to determine the atmospheric number concentration of INP (N-INP) in the range from 6 to 25 degrees C in Beijing. No correlations between N-INP and either PM2.5 or black carbon mass concentrations were found, although both varied by more than a factor of 30 during the sampling period. Similarly, there were no correlations between N-INP and either total particle number concentration or number concentrations for particles with diameters > 500 nm. Furthermore, there was no clear difference between day and night samples. All these results indicate that Beijing air pollution did not increase or decrease INP concentrations in the examined temperature range above values observed in nonurban areas; hence, the background INP concentrations might not be anthropogenically influenced as far as urban air pollution is concerned, at least in the examined temperature range.
25.	Christensen, Ole Martin, 1984, et al. (författare) The relationship between polar mesospheric clouds and their background atmosphere as observed by Odin-SMR and Odin-OSIRIS 2016 Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:19, s. 12587-12600 Tidskriftsartikel (refereegranskat)abstract In this study the properties of polar mesospheric clouds (PMCs) and the background atmosphere in which they exist are studied using measurements from two instruments, OSIRIS and SMR, on board the Odin satellite. The data comes from a set of tomographic measurements conducted by the satellite during 2010 and 2011. The expected ice mass density and cloud frequency for conditions of thermodynamic equilibrium, calculated using the temperature and water vapour as measured by SMR, are compared to the ice mass density and cloud frequency as measured by OSIRIS. We find that assuming thermodynamic equilibrium reproduces the seasonal, latitudinal and vertical variations in ice mass density and cloud frequency, but with a high bias of a factor of 2 in ice mass density. To investigate this bias, we use a simple ice particle growth model to estimate the time it would take for the observed clouds to sublimate completely and the time it takes for these clouds to reform. We find a difference in the median sublimation time (1.8 h) and the reformation time (3.2 h) at peak cloud altitudes (82-84 km). This difference implies that temperature variations on these timescales have a tendency to reduce the ice content of the clouds, possibly explaining the high bias of the equilibrium model. Finally, we detect and are, for the first time, able to positively identify cloud features with horizontal scales of 100 to 300 km extending far below the region of supersaturation (>2 km). Using the growth model, we conclude these features cannot be explained by sedimentation alone and suggest that these events may be an indication of strong vertical transport.

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