| 1. |
- Ahlm, Lars, et al.
(author)
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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
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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
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| 2. |
- Couvreux, Fleur, et al.
(author)
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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
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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.
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| 3. |
- Nikulin, Grigory, et al.
(author)
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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
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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.
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| 4. |
- Nilsson, Erik, 1983-, et al.
(author)
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Turbulence Kinetic Energy budget during the afternoon transition – Part 1 : Observed surface TKE budget and boundary layer description for 10 intensive observation period days
- 2016
-
In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375 .- 1680-7324. ; 16:14, s. 8849-8872
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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.
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| 5. |
- Nilsson, Erik, 1983-, et al.
(author)
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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
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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.
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| 6. |
- Bidleman, Terry F., et al.
(author)
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Biannual cycles of organochlorine pesticide enantiomers in arctic air suggest changing sources and pathways
- 2014
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375. ; 14:17, s. 25027-25050
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Journal article (peer-reviewed)abstract
- Air samples collected during 1994–2000 at the Canadian arctic air monitoring stationAlert (82300 N, 62200 W) were analyzed by enantiospecific gas chromatography –mass spectrometry for -hexachlorocyclohexane (-HCH), trans-chlordane (TC) and5 cis-chlordane (CC). Results were expressed as enantiomer fractions (EF = quantitiesof (+)/[(+)+(−)] enantiomers), where EFs=0.5, < 0.5 and > 0.5 indicate racemic composition,and preferential depletion of (+) and (−) enantiomers, respectively. Long-termaverage EFs were close to racemic values for -HCH (0.504±0.004, n =197) andCC (0.505±0.004, n =162), and deviated farther from racemic for TC (0.470±0.013,10 n =165). Digital filtration analysis revealed biannual cycles of lower -HCH EFs insummer-fall and higher EFs in winter-spring. These cycles suggest volatilization ofpartially degraded -HCH with EF < 0.5 from open water and advection to Alert duringthe warm season, and background transport of -HCH with EF> 0.5 during the coldseason. The contribution of sea-volatilized -HCH was only 11% at Alert, vs. 32%15 at Resolute Bay (74.68 N, 94.90W) in 1999. EFs of TC also followed biannual cyclesof lower and higher values in the warm and cold seasons. These were in phasewith low and high cycles of the TC/CC ratio (expressed as FTC =TC/(TC+CC)), whichsuggests greater contribution of microbially “weathered” TC in summer-fall vs. winterspring.CC was closer to racemic than TC and displayed seasonal cycles only in 1997–20 1998. EF profiles are likely to change with rising contribution of secondary emissionsources, weathering of residues in the environment, and loss of ice cover in the Arctic.Enantiomer-specific analysis could provide added forensic capability to air monitoringprograms.
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| 7. |
- Dalirian, Maryam, 1978-, et al.
(author)
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Cloud droplet activation of black carbon particles coated with organic compounds of varying solubility
- 2018
-
In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375. ; 18:16, s. 12477-12489
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Journal article (peer-reviewed)abstract
- Atmospheric black carbon (BC) particles are a concern due to their impact on air quality and climate. Their net climate effect 15 is, however, still uncertain. This uncertainty is partly related to the contribution of coated BC-particles to the global CCN budgets. In this study, laboratory measurements were performed to investigate cloud condensation nuclei (CCN) activity of BC (Regal black) particles, in pure state or coated through evaporating and subsequent condensation of glutaric acid, levoglucosan (both water-soluble organics) or oleic acid (an organic compound with low solubility). A combination of Soot Particle Aerosol Mass Spectrometer (SP-AMS) measurements and size distribution measurements with Scanning Mobility 20 Particle Sizer (SMPS) showed that the studied BC particles were nearly spherical agglomerates with a fractal dimension of 2.79 and that they were coated evenly by the organic species. The CCN activity of BC particles increased after coating with all the studied compounds and was governed by the fraction of organic material. The CCN activation of the BC particles coated by glutaric acid and levoglucosan were in good agreement with the theoretical calculations using shell-and-core model, which is based on a combination of the CCN activities of the pure compounds. The oleic acid coating enhanced the CCN 25 activity of the BC particles, even though the pure oleic acid particles were CCN inactive. The surprising effect of oleic acid might be related to the arrangement of the oleic acid molecules on the surface of the BC cores or other surface phenomena facilitating water condensation onto the coated particles. Our results show potential in accurately predicting the CCN activity of atmospheric BC coated with organic species by present theories, given that the identities and amount of the coating species are known. Furthermore, our results suggest that even relatively thin soluble coatings (around 2 nm for the compounds studied here) are enough to make the insoluble BC particles CCN active at typical atmospheric supersaturations and thus be efficiently taken up by cloud droplets. This highlights the need of an accurate description of the composition of atmospheric particles containing BC to unravel their net impact on climate.
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| 8. |
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| 9. |
- Eliasson, Salomon, et al.
(author)
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Assessing modelled spatial distributions of ice water path using satellite data
- 2010
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375. ; 10:5, s. 12185-12224
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Journal article (peer-reviewed)abstract
- The climate models used in the IPCC AR4 show large differences in monthly mean cloud ice. The most valuable source of information that can be used to potentially constrain the models is global satellite data. For this, the data sets must be long enough to capture the inter-annual variability of Ice Water Path (IWP). PATMOS-x was used together with ISCCP for the annual cycle evaluation in Fig. 7 while ECHAM-5 was used for the correlation with other models in Table 3. A clear distinction between ice categories in satellite retrievals, as desired from a model point of view, is currently impossible. However, long-term satellite data sets may still be used to indicate the climatology of IWP spatial distribution. We evaluated satellite data sets from CloudSat, PATMOS-x, ISCCP, MODIS and MSPPS in terms of monthly mean IWP, to determine which data sets can be used to evaluate the climate models. IWP data from CloudSat cloud profiling radar provides the most advanced data set on clouds. As CloudSat data are too short to evaluate the model data directly, it was mainly used here to evaluate IWP from the other satellite data sets. ISCCP and MSPPS were shown to have comparatively low IWP values. ISCCP shows particularly low values in the tropics, while MSPPS has particularly low values outside the tropics. MODIS and PATMOS-x were in closest agreement with CloudSat in terms of magnitude and spatial distribution, with MODIS being the best of the two. As PATMOS-x extends over more than 25 years and is in fairly close agreement with CloudSat, it was chosen as the reference data set for the model evaluation. In general there are large discrepancies between the individual climate models, and all of the models show problems in reproducing the observed spatial distribution of cloud-ice. Comparisons consistently showed that ECHAM-5 is the GCM from IPCC AR4 closest to satellite observations
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| 10. |
- Emanuelsson, Eva U., et al.
(author)
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Formation of anthropogenic secondary organic aerosol (SOA) and its influence on biogenic SOA properties
- 2012
-
In: Atmospheric Chemistry and Physics Discussions. - : Copernicus Publications. - 1680-7367 .- 1680-7375. ; 12:8, s. 20311-20350
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Journal article (peer-reviewed)abstract
- Secondary organic aerosol (SOA) formation from mixed anthropogenic and biogenic precursors has been studied exposing reaction mixtures to natural sunlight in the SAPHIR chamber in Jülich, Germany. Several experiments with exclusively anthro- 5 pogenic precursors were performed to establish a relationship between yield and organic aerosol mass loading for the atmospheric relevant range of aerosol loads of 0.01 to 10 μgm−3. The yields (0.5–9 %) were comparable to previous data and further used for the detailed evaluation of the mixed biogenic and anthropogenic experiments. For the mixed experiments a number of different oxidation schemes were addressed. The 10 reactivity, the sequence of addition, and the amount of the precursors influenced the SOA properties. Monoterpene oxidation products, including carboxylic acids and dimer esters were identified in the aged aerosol at levels comparable to ambient air. OH radicals were measured by Laser Induced Fluorescence, which allowed for establishing relations of aerosol properties and composition to the experimental OH dose. Further 15 more, the OH measurements in combination with the derived yields for anthropogenic SOA enabled application of a simplified model to calculate the chemical turnover of the anthropogenic precursor and corresponding anthropogenic contribution to the mixed aerosol. The estimated anthropogenic contributions were ranging from small (8 %) up to significant fraction (>50 %) providing a suitable range to study the effect of aerosol 20 composition on the aerosol volatility (volume fraction remaining at 343 K: 0.86–0.94). The anthropogenic aerosol had higher oxygen to carbon ratio O/C and was less volatile than the biogenic fraction. However, in order to produce significant amount of anthropogenic SOA the reaction mixtures needed a higher OH dose that also increased O/C and provided a less volatile aerosol. A strong positive correlation was found between 25 changes in volatility and O/C with the exception during dark hours where the SOA volatility decreased while O/C did not change significantly. This change in volatility under dark conditions is likely due to chemical or morphological changes not affecting O/C.
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| 11. |
- Hede, Thomas, et al.
(author)
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HULIS in Nanoaerosol Clusters; Investigations of Surface Tension and Aggregate Formation using Molecular Dynamics Simulations
- 2011
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367 .- 1680-7375.
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Journal article (other academic/artistic)abstract
- Cloud condensation nuclei act as cores for water vapor condensation, and their composition and chemical properties may enhance or depress the ability for droplet growth. In this study we use molecular dynamics simulations to show that humic-like substances of larger systems (8.6 nm in diameter) mimic experimental data well referring to reduction of surface tension. The structural properties examined show the ability for the humic-like substances to aggregate inside the nanoaerosol clusters.
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| 12. |
- Karlsson, Nélida Jocelyn Donají, 1980-
(author)
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Primary and secondary organics in tropical rainforest aerosols: Quantitative and qualitative analysis of 2-methyltetrols in the Amazon
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In: Atmospheric Chemistry and Physics Discussions. - 1680-7367 .- 1680-7375.
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Journal article (peer-reviewed)abstract
- Ambient aerosol samples from central Amazonia were analyzed for the presence of (2R,3S)- and (2S,3R)- methylerythritol and (2S,3S)- and (2R,3R)- methylthreitol, four stereoisomers that may have primary and secondary origins from the biosynthesis and oxidation processes of isoprene within plants and also in the atmosphere. The 2-methyltetrols were detected in aerosol samples collected at a measurement site near Manaus, Brazil in a remote tropical rainforest environment between June 2008 and June 2009. Average concentrations of 78.2 and 72.8 ng m-3 were observed for (2R,3S)- and (2S,3R)- methylerythritol and 3.1 and 3.3 ng m-3 for (2S,3S)- and (2R,3R)- methylthreitol during the dry season. In the wet season, the average concentrations were 7.1, 6.5, 2.0, and 2.2 ng m-3, respectively. The enantiomer fractions (Ef) were on average 0.52: 0.48 for (2R,3S)- and (2S,3R)- methylerythritol and 0.46: 0.54 for (2S,3S)- and (2R,3R)- methylthreitol. The concentration of these isoprene oxidation products attributed to primary origin ranged between 0.8 and 53.8 ng m-3 for the 2-methylerythritols and between 0.3 and 2.1 ng m-3 for the 2-methylthreitols. The 2-methylerythritols show no correlation with isoprene emission estimates whereas 2-methylthreitol displays a negative correlation. The present study reinforces the importance of the analysis of chiral organic compounds to correctly assess the relative contribution of primary biogenic emissions and isoprene oxidation products to biogenic secondary organic aerosol.
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| 13. |
- Khosrawi, F., et al.
(author)
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Sensitivity of polar stratospheric cloud formation to changes in water vapour and temperature
- 2015
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7375 .- 1680-7367. ; 15:13, s. 17743-17796
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Research review (peer-reviewed)abstract
- More than a decade ago it was suggested that a cooling of stratospheric temperatures by 1 K or an increase of 1 ppmv of stratospheric water vapour could promote denitrification, the permanent removal of nitrogen species from the stratosphere by solid polar stratospheric cloud (PSC) particles. In fact, during the two Arctic winters 2009/10 and 2010/11 the strongest denitrification in the recent decade was observed. Sensitivity studies along air parcel trajectories are performed to test how a future stratospheric water vapour (H 2 O) increase of 1 ppmv or a temperature decrease of 1 K would affect PSC formation. We perform our study based on measurements made during the Arctic winter 2010/11. Air parcel trajectories were calculated 6 days backward in time based on PSCs detected by CALIPSO (Cloud Aerosol Lidar and Infrared Pathfinder satellite observations). The sensitivity study was performed on single trajectories as well as on a trajectory ensemble. The sensitivity study shows a clear prolongation of the potential for PSC formation and PSC existence when the temperature in the stratosphere is decreased by 1 K and water vapour is increased by 1 ppmv. Based on 15 years of satellite measurements (2000-2014) from UARS/HALOE, Envisat/MIPAS, Odin/SMR, Aura/MLS, Envisat/SCIAMACHY and SCISAT/ACE-FTS it is further investigated if there is a decrease in temperature and/or increase of water vapour (H 2 O) observed in the polar regions similar to that observed at midlatitudes and in the tropics. Although in the polar regions no significant trend is found in the lower stratosphere, we found from the observations a correlation between cold winters and enhanced water vapour mixing ratios.
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| 14. |
- Nordin, E. Z., et al.
(author)
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Secondary organic aerosol formation from gasoline passenger vehicle emissions investigated in a smog chamber
- 2012
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus Publications. - 1680-7367 .- 1680-7375. ; 12:12, s. 31725-31765
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Journal article (peer-reviewed)abstract
- Gasoline vehicles have elevated emissions of volatile organic compounds during cold starts and idling and have recently been pointed out as potentially the main source of anthropogenic secondary organic aerosol (SOA) in megacities. However, there is a lack of laboratory studies to systematically investigate SOA formation in real-world exhaust. In this study, SOA formation from pure aromatic precursors, idling and cold start gasoline exhaust from one Euro II, one Euro III and one Euro IV passenger vehicles were investigated using photo-oxidation experiments in a 6 m3 smog chamber. The experiments were carried out at atmospherically relevant organic aerosol mass concentrations. The characterization methods included a high resolution aerosol mass spectrometer and a proton transfer mass spectrometer. It was found that gasoline exhaust readily forms SOA with a signature aerosol mass spectrum similar to the oxidized organic aerosol that commonly dominates the organic aerosol mass spectra downwind urban areas. After 4 h aging the formed SOA was 1–2 orders of magnitude higher than the Primary OA emissions. The SOA mass spectrum from a relevant mixture of traditional light aromatic precursors gave f43 (mass fraction at m/z = 4 3) approximately two times higher than to the gasoline SOA. However O : C and H : C ratios were similar for the two cases. Classical C6–C9 light aromatic precursors were responsible for up to 60% of the formed SOA, which is significantly higher than for diesel exhaust. Important candidates for additional precursors are higher order aromatic compounds such as C10, C11 light aromatics, naphthalene and methyl-naphthalenes.
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| 15. |
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| 16. |
- Ekström, Sanna, et al.
(author)
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The Cloud Condensation Nuclei (CCN) properties of 2-methyltetrols and C3–C6 polyols from osmolality and surface tension measurements (Discussion paper)
- 2008
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In: Atmospheric Chemistry and Physics Discussion. - : Copernicus GmbH. - 1680-7367. ; 8:5, s. 17237-17256
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Journal article (peer-reviewed)abstract
- A significant fraction of the organic material in aerosols is made of highly soluble compounds such as sugars (mono- and polysaccharides) and polyols, including the 2-methyltetrols, methylerythritol and methyltreitol. The high solubility of these compounds has brought the question of their potentially high CCN efficiency. For the 2-methyltetrols, this would have important implications for cloud formation at global scale because they are thought to be produced by the atmospheric oxidation of isoprene. To investigate this question, the complete Köhler curves for C3–C6 polyols and the 2-methyltetrols have been determined experimentally from osmolality and surface tension measurements. Contrary to what expected, none of these compounds displayed a critical supersaturation lower than those of inorganic salts or organic acids. Their Raoult terms show that this limited CCN efficiency is due to their absence of dissociation in water, this in spite of slight surface-tension effects for the 2-methyltetrols. Thus, compounds such as sugars and polyols would not contribute more to cloud formation in the atmosphere than any other organic compounds studied so far. In particular, the presence of 2-methyltetrols in aerosols would not particularly enhance cloud formation in the atmosphere, contrary to what has been suggested.
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| 17. |
- Friberg, Johan, et al.
(author)
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Volcanic impact on the climate – the stratospheric aerosol load in the period 2006–2015
- 2018
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7375.
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Journal article (peer-reviewed)abstract
- Abstract. We present a study on the stratospheric aerosol load during 2006–2015, discuss the influence from volcanism and other sources, and reconstruct an AOD data-set in a resolution of 1° latitudinally and 8 days timewise. Our attempt is to include the entire stratosphere, from the tropopause to the almost particle free altitudes of the mid-stratosphere. A dynamic tropopause of 1.5 PVU was found to be the best suited one, enclosing almost all of the volcanic signals in the CALIOP data-set. New methods were developed to handle bias in the data. The data were successfully cleaned from polar stratospheric clouds using a temperature threshold of 195 K. Furthermore, a method was developed to correct data when the CALIPSO laser beam was strongly attenuated by volcanic aerosol, preventing a negative bias in the AOD data-set. Tropospheric influence, likely from upwelling dust, was found in the extratropical transition layer in spring. Eruptions of both extratropical and tropical volcanoes that injected aerosol into the stratosphere impacted the stratospheric aerosol load for up to a year if their clouds reached lower than 20 km altitudes, whereas deeper reaching tropical injections rose in the tropical pipe and impacted it for several years. Over the years 2006–2015, volcanic eruptions increased the stratospheric AOD on average by ~ 40 %. In absolute numbers the stratospheric AOD and radiative forcing amounted to 0.008 and −0.2 Wm−2, respectively.
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| 18. |
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| 19. |
- Tunved, Peter, et al.
(author)
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A pseudo-Lagrangian model study of the size distribution properties over Scandinavia : Transport from Aspvreten to Värriö
- 2004
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In: Atmospheric Chemistry and Physics Discussions. - : Copernicus GmbH. - 1680-7367. ; :4, s. 7757-7794
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Journal article (peer-reviewed)abstract
- The evolution of the aerosol size distribution during transport between Aspvreten (58.8° N, 17.4° E) and Värriö (67.46° N, 29.35° E) was studied using a pseudo-Lagrangian approach. Aerosol dynamic processes were studied and interpreted utilizing a state-of-the-art aerosol dynamic box model UHMA (University of Helsinki Multicomponent Aerosol model) complemented with OH, NO3, O3 and terpene chemistry. In the model simulations, the growth and formation of aerosol particles was controlled by sulphuric acid, ammonia, water and an unidentified low volatile organic compound. This organic compound was assumed to be a product of terpene oxidation with a yield of 13% in the base case conditions. Changes of aerosol size distribution properties during transport between the stations were examined in twelve clear sky cases. On average, the modelled number agreed fairly well with observations. Mass concentration was overestimated by 10%. Apart from dilution, the only removal mechanism for aerosol mass is dry deposition. A series of sensitivity tests performed revealed that the absolute magnitude of dry deposition effects on the aerosol size distribution is slow overall. Furthermore, nucleation does not leave a significant contribution to aerosol number in the selected cases. The sensitivity of the modelled size distribution to concentration of precursor gases and oxidants is, however, obvious. In order to explain observed mass increase during transport we conclude that a yield of low volatile products from oxidation of terpenes of 10–15% is required to explain observed growth rates. Coagulation is acknowledged to be highly important in modelled cases.
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| 20. |
- Tunved, Peter, et al.
(author)
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An investigation of processes controlling the evolution of the boundary layer aerosol size distribution properties at the Swedish background station Aspvreten
- 2004
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In: Atmospheric Chemistry and Physics Discussions. - : the Copernicus GmbH (Copernicus Publications). - 1680-7367. ; 4:4, s. 4507-4543
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Journal article (peer-reviewed)abstract
- Aerosol size distributions have been measured at the Swedish background station Aspvreten (58.8° N, 17.4° E). Different states of the aerosol were determined using a novel application of cluster analysis. The analysis resulted in eight different clusters capturing the different stages of the aerosol lifecycle. The aerosol was interpreted as belonging to fresh, intermediate and aged type of size distribution and different magnitudes thereof. With aid of back trajectory analysis we present statistics concerning the relation of source area and different meteorological parameters using a non-lagrangian approach. Source area is argued to be important although not sufficient to describe the observed aerosol properties. Especially processing by clouds and precipitation is shown to be crucial for the evolution of the aerosol size distribution. As much as 60% of the observed size distributions present features likely related to cloud processes or wet deposition. The lifetime properties of different sized aerosols are discussed by means of measured variability. Processing by non-precipitating clouds most obviously affect aerosols in the size range 100 nm and larger. This indicates an approximate limit for activation in clouds to 100 nm in this type of environment. The aerosol lifecycle is discussed. Size distributions bearing signs of recent new particle formation (~30% of the observed size distributions) represent the first stage in the lifecycle. Aging may proceed in two directions: either growth by condensation and coagulation or processing by non-precipitating clouds. In both cases mass is accumulated. Wet removal is the main process capable of removing aerosol mass. Wet deposition is argued to be an important mechanism in reaching a state where nucleation may occur (i.e. sufficiently low aerosol surface area) in environments similar to the one studied
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