| 1. |
- Birch, C. E., et al.
(författare)
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Modelling atmospheric structure, cloud and their response to CCN in the central Arctic : ASCOS case studies
- 2012
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 12:7, s. 3419-3435
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Tidskriftsartikel (refereegranskat)abstract
- Observations made during late summer in the central Arctic Ocean, as part of the Arctic Summer Cloud Ocean Study (ASCOS), are used to evaluate cloud and vertical temperature structure in the Met Office Unified Model (MetUM). The observation period can be split into 5 regimes; the first two regimes had a large number of frontal systems, which were associated with deep cloud. During the remainder of the campaign a layer of low-level cloud occurred, typical of central Arctic summer conditions, along with two periods of greatly reduced cloud cover. The short-range operational NWP forecasts could not accurately reproduce the observed variations in near-surface temperature. A major source of this error was found to be the temperature-dependant surface albedo parameterisation scheme. The model reproduced the low-level cloud layer, though it was too thin, too shallow, and in a boundary-layer that was too frequently well-mixed. The model was also unable to reproduce the observed periods of reduced cloud cover, which were associated with very low cloud condensation nuclei (CCN) concentrations (< 1 cm(-3)). As with most global NWP models, the MetUM does not have a prognostic aerosol/cloud scheme but uses a constant CCN concentration of 100 cm(-3) over all marine environments. It is therefore unable to represent the low CCN number concentrations and the rapid variations in concentration frequently observed in the central Arctic during late summer. Experiments with a single-column model configuration of the MetUM show that reducing model CCN number concentrations to observed values reduces the amount of cloud, increases the near-surface stability, and improves the representation of both the surface radiation fluxes and the surface temperature. The model is shown to be sensitive to CCN only when number concentrations are less than 10-20 cm(-3).
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| 2. |
- Browse, J., et al.
(författare)
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The complex response of Arctic aerosol to sea-ice retreat
- 2014
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 14:14, s. 7543-7557
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Tidskriftsartikel (refereegranskat)abstract
- Loss of summertime Arctic sea ice will lead to a large increase in the emission of aerosols and precursor gases from the ocean surface. It has been suggested that these enhanced emissions will exert substantial aerosol radiative forcings, dominated by the indirect effect of aerosol on clouds. Here, we investigate the potential for these indirect forcings using a global aerosol microphysics model evaluated against aerosol observations from the Arctic Summer Cloud Ocean Study (ASCOS) campaign to examine the response of Arctic cloud condensation nuclei (CCN) to sea-ice retreat. In response to a complete loss of summer ice, we find that north of 70 degrees N emission fluxes of sea salt, marine primary organic aerosol (OA) and dimethyl sulfide increase by a factor of similar to 10, similar to 4 and similar to 15 respectively. However, the CCN response is weak, with negative changes over the central Arctic Ocean. The weak response is due to the efficient scavenging of aerosol by extensive drizzling stratocumulus clouds. In the scavenging-dominated Arctic environment, the production of condensable vapour from oxidation of dimethyl sulfide grows particles to sizes where they can be scavenged. This loss is not sufficiently compensated by new particle formation, due to the suppression of nucleation by the large condensation sink resulting from sea-salt and primary OA emissions. Thus, our results suggest that increased aerosol emissions will not cause a climate feedback through changes in cloud microphysical and radiative properties.
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| 3. |
- Bulatovic, Ines, 1991-, et al.
(författare)
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Large-eddy simulation of a two-layer boundary-layer cloud system from the Arctic Ocean 2018 expedition
- 2023
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324. ; 23:12, s. 7033-7055
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Tidskriftsartikel (refereegranskat)abstract
- Climate change is particularly noticeable in the Arctic. The most common type of cloud at these latitudes is mixed-phase stratocumulus. These clouds occur frequently and persistently during all seasons and play a critical role in the Arctic energy budget. Previous observations in the central (north of 80∘ N) Arctic have shown a high occurrence of prolonged periods of a shallow, single-layer mixed-phase stratocumulus at the top of the boundary layer (BL; altitudes ∼ 300 to 400 m). However, recent observations from the summer of 2018 instead showed a prevalence of a two-layer boundary-layer cloud system. Here we use large-eddy simulation to examine the maintenance of one of the cloud systems observed in the summer of 2018 and the sensitivity of the cloud layers to different micro- and macro-scale parameters. We find that the model generally reproduces the observed thermodynamic structure well, with two near-neutrally stratified layers in the BL caused by a low cloud (located within the first few hundred meters) capped by a lower-altitude temperature inversion and an upper cloud layer (based around one kilometer or slightly higher) capped by the main temperature inversion of the BL. The simulated cloud structure is persistent unless there are low aerosol number concentrations (≤ 5 cm−3), which cause the upper cloud layer to dissipate, or high large-scale wind speeds (≥ 8.5 m s−1), which erode the lower inversion and the related cloud layer. The changes in cloud structure alter both the short- and longwave cloud radiative effect at the surface. This results in changes in the net radiative effect of the modeled cloud system, which can impact the surface melting or freezing. The findings highlight the importance of better understanding and representing aerosol sources and sinks over the central Arctic Ocean. Furthermore, they underline the significance of meteorological parameters, such as the large-scale wind speed, for maintaining the two-layer boundary-layer cloud structure encountered in the lower atmosphere of the central Arctic.
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| 4. |
- Bulatovic, Ines, et al.
(författare)
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The importance of Aitken mode aerosol particles for cloud sustenance in the summertime high Arctic - a simulation study supported by observational data
- 2021
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:5, s. 3871-3897
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Tidskriftsartikel (refereegranskat)abstract
- The potential importance of Aitken mode particles (diameters similar to 25-80 nm) for stratiform mixed-phase clouds in the summertime high Arctic (> 80 degrees N) has been investigated using two large-eddy simulation models. We find that, in both models, Aitken mode particles significantly affect the simulated microphysical and radiative properties of the cloud and can help sustain the cloud when accumulation mode concentrations are low (< 10-20 cm(-3)), even when the particles have low hygroscopicity (hygroscopicity parameter - kappa = 0.1). However, the influence of the Aitken mode decreases if the overall liquid water content of the cloud is low, either due to a higher ice fraction or due to low radiative cooling rates. An analysis of the simulated supersaturation (ss) statistics shows that the ss frequently reaches 0.5 % and sometimes even exceeds 1 %, which confirms that Aitken mode particles can be activated. The modelling results are in qualitative agreement with observations of the Hoppel minimum obtained from four different expeditions in the high Arctic. Our findings highlight the importance of better understanding Aitken mode particle formation, chemical properties and emissions, particularly in clean environments such as the high Arctic.
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| 5. |
- Chang, R. Y. -W, et al.
(författare)
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Aerosol composition and sources in the central Arctic Ocean during ASCOS
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:20, s. 10619-10636
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Tidskriftsartikel (refereegranskat)abstract
- Measurements of submicron aerosol chemical composition were made over the central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.051 and 0.055 mu gm(-3), respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33% and 36% of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47% of the sulphate apportioned to marine biogenic sources and 48% to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25+/-0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it had a longer photochemical lifetime than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources. In particular, given that the factor does not correlate with common tracers of continental influence, we cannot rule out that the organic factor arises from a primary marine source.
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| 6. |
- Das, Ruby, et al.
(författare)
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Chemical composition of rainwater at Maldives Climate Observatory at Hanimaadhoo (MCOH)
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:8, s. 3743-3755
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Tidskriftsartikel (refereegranskat)abstract
- Water-soluble inorganic components in rain deposited at the Maldives Climate Observatory Hanimaadhoo (MCOH) were examined to determine seasonality and possible source regions. The study, which is part of the Atmospheric Brown Cloud (ABC) project, covers the period June 2005 to December 2007. Air mass trajectories were used to separate the data into situations with transport of air from India and adjacent parts of the Asian continent during the months December and January (Indian group) and those with southerly flow from the Indian Ocean during the summer monsoon season June to September (Marine group). A third trajectory group was identified with transport from the northern parts of the Arabian Sea and adjacent land areas during the months March, April and October (Arabian Sea group). The concentrations of nss-SO(4)(2-), NH(4)(+) and NO(3)(-) were more than a factor of 4 higher in the Indian group than in the Marine group. The average rainwater pH was significantly lower in the Indian group (4.7) than in the Marine group (6.0). This shows a pronounced influence of continental pollutants during December and January. The origin of the very high concentration of nss-Ca(2+) found in the Marine group - a factor of 7 higher than in the Indian group - is unclear. We discuss various possibilities including long-range transport from the African or Australian continents, local dust from nearby islands and calcareous plankton debris and exopolymer gels emitted from the ocean surface. The occurrence of NO(3)(-) and NH(4)(+) in the Marine group suggests emissions from the ocean surface. Part of the NO(3)(-) could also be associated with lightning over the ocean. Despite the fact that the concentrations of nss-SO(4)(2-), NO(3)(-), and NH(4)(+) were highest in the Indian group the wet deposition was at least as big in the Marine group reflecting the larger amount of rainfall during the monsoon season. The annual wet deposition of NO(3)(-), NH(4)(+) and nss-SO(4)(2-) at MCOH is about a factor of three lower than observed at rural sites in India.
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| 7. |
- Engström, Erik J., 1976-, et al.
(författare)
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Reducing uncertainties associated with filter-based optical measurements of soot aerosol particles with chemical information.
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Ingår i: Atmospheric Chemistry And Physics. - 1680-7316 .- 1680-7324.
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Tidskriftsartikel (refereegranskat)abstract
- Of the many identified and potential effects ofatmospheric aerosol particles on climate, those of soot particlesare the most uncertain, in that analytical techniques concerningsoot are far from satisfactory. One concern whenapplying filter-based optical measurements of soot is thatthey suffer from systematic errors due to the light scatteringof non-absorbing particles co-deposited on the filter, suchas inorganic salts and mineral dust. In addition to an opticalcorrection of the non-absorbing material this study providesa protocol for correction of light scattering based onthe chemical quantification of the material, which is a novelty.A newly designed Particle Soot Absorption Photometerwas constructed to measure light transmission on particleaccumulating filters, which includes an additional sensorrecording backscattered light. The choice of polycarbonatemembrane filters avoided high chemical blank values and reducederrors associated with length of the light path throughthe filter.Two protocols of corrections were applied to aerosol samplescollected at the Maldives Climate Observatory Hanimaadhooduring episodes with either continentally influencedair from the Indian/Arabian subcontinents (wintermonsoon) or pristine air from the Southern Indian Ocean(summer monsoon). The two ways of correction (optical andchemical) lowered the particle light absorption of soot by 63 to 61 %, respectively, for data from the Arabian Sea sourcedgroup, resulting in median soot absorption coefficients of 4.2 and 3.5 Mm-1. Corresponding values for the South IndianOcean data were 69 and 97 % (0.38 and 0.02 Mm-1). A comparison with other studies in the area indicated anoverestimation of their soot levels, by up to two orders ofmagnitude. This raises the necessity for chemical correctionprotocols on optical filter-based determinations of soot, before even the sign on the radiative forcing based on their effectscan be assessed.
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| 8. |
- Hamacher-Barth, Evelyne, et al.
(författare)
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Size-resolved morphological properties of the high Arctic summer aerosol during ASCOS-2008
- 2016
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:10, s. 6577-6593
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Tidskriftsartikel (refereegranskat)abstract
- The representation of aerosol properties and processes in climate models is fraught with large uncertainties. Especially at high northern latitudes a strong underprediction of aerosol concentrations and nucleation events is observed and can only be constrained by in situ observations based on the analysis of individual aerosol particles. To further reduce the uncertainties surrounding aerosol properties and their potential role as cloud condensation nuclei this study provides observational data resolved over size on morphological and chemical properties of aerosol particles collected in the summer high Arctic, north of 80A degrees aEuro-N. Aerosol particles were imaged with scanning and transmission electron microscopy and further evaluated with digital image analysis. In total, 3909 aerosol particles were imaged and categorized according to morphological similarities into three gross morphological groups: single particles, gel particles, and halo particles. Single particles were observed between 15 and 800aEuro-nm in diameter and represent the dominating type of particles (82aEuro-%). The majority of particles appeared to be marine gels with a broad Aitken mode peaking at 70aEuro-nm and accompanied by a minor fraction of ammonium (bi)sulfate with a maximum at 170aEuro-nm in number concentration. Gel particles (11aEuro-% of all particles) were observed between 45 and 800aEuro-nm with a maximum at 154aEuro-nm in diameter. Imaging with transmission electron microscopy allowed further morphological discrimination of gel particles in 'aggregate' particles, 'aggregate with film' particles, and 'mucus-like' particles. Halo particles were observed above 75aEuro-nm and appeared to be ammonium (bi)sulfate (59aEuro-% of halo particles), gel matter (19aEuro-%), or decomposed gel matter (22aEuro-%), which were internally mixed with sulfuric acid, methane sulfonic acid, or ammonium (bi)sulfate with a maximum at 161aEuro-nm in diameter. Elemental dispersive X-ray spectroscopy analysis of individual particles revealed a prevalence of the monovalent ions Na+/K+ for single particles and aggregate particles and of the divalent ions Ca2+/Mg2+ for aggregate with film particles and mucus-like particles. According to these results and other model studies, we propose a relationship between the availability of Na+/K+ and Ca2+/Mg2+ and the length of the biopolymer molecules participating in the formation of the three-dimensional gel networks.
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| 9. |
- Hede, Thomas, 1975-, et al.
(författare)
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Model HULIS compounds in nanoaerosol clusters : investigations of surface tension and aggregate formation using molecular dynamics simulations
- 2011
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 11:13, s. 6549-6557
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Tidskriftsartikel (refereegranskat)abstract
- Cloud condensation nuclei act as cores for water vapour 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 model humic-like substances (HULIS) in systems containing 10 000 water molecules mimic experimental data well referring to reduction of surface tension. The model HULIS compounds investigated in this study are cis-pinonic acid (CPA), pinic acid (PAD) and pinonaldehyde (PAL). The structural properties examined show the ability for the model HULIS compounds to aggregate inside the nanoaerosol clusters.
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| 10. |
- Heintzenberg, Jost, et al.
(författare)
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New particle formation in the Svalbard region 2006-2015
- 2017
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:10, s. 6153-6175
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Tidskriftsartikel (refereegranskat)abstract
- Events of new particle formation (NPF) were analyzed in a 10-year data set of hourly particle size distributions recorded on Mt. Zeppelin, Spitsbergen, Svalbard. Three different types of NPF events were identified through objective search algorithms. The first and simplest algorithm utilizes short-term increases in particle concentrations below 25 nm (PCT (percentiles) events). The second one builds on the growth of the sub-50 nm diameter median (DGR (diameter growth) events) and is most closely related to the classical banana type of event. The third and most complex, multiple-size approach to identifying NPF events builds on a hypothesis suggesting the concurrent production of polymer gel particles at several sizes below ca. 60 nm (MEV (multisize growth) events). As a first and general conclusion, we can state that NPF events are a summer phenomenon and not related to Arctic haze, which is a late winter to early spring feature. The occurrence of NPF events appears to be somewhat sensitive to the available data on precipitation. The seasonal distribution of solar flux suggests some photochemical control that may affect marine biological processes generating particle precursors and/or atmospheric photochemical processes that generate condensable vapors from precursor gases. Notably, the seasonal distribution of the biogenic methanesulfonate (MSA) follows that of the solar flux although it peaks before the maxima in NPF occurrence. A host of ancillary data and findings point to varying and rather complex marine biological source processes. The potential source regions for all types of new particle formation appear to be restricted to the marginal-ice and open-water areas between northeastern Greenland and eastern Svalbard.Depending on conditions, yet to be clarified new particle formation may become visible as short bursts of particles around 20 nm (PCT events), longer events involving condensation growth (DGR events), or extended events with elevated concentrations of particles at several sizes below 100 nm (MEV events). The seasonal distribution of NPF events peaks later than that of MSA and DGR, and in particular than that of MEV events, which reach into late summer and early fall with open, warm, and biologically active waters around Svalbard. Consequently, a simple model to describe the seasonal distribution of the total number of NPF events can be based on solar flux and sea surface temperature, representing environmental conditions for marine biological activity and condensation sink, controlling the balance between new particle nucleation and their condensational growth. Based on the sparse knowledge about the seasonal cycle of gel-forming marine microorganisms and their controlling factors, we hypothesize that the seasonal distribution of DGR and, more so, MEV events reflect the seasonal cycle of the gel-forming phytoplankton.
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