| 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.
|
|
