| 1. |
- Baccarini, Andrea, et al.
(författare)
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Frequent new particle formation over the high Arctic pack ice by enhanced iodine emissions
- 2020
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- In the central Arctic Ocean the formation of clouds and their properties are sensitive to the availability of cloud condensation nuclei (CCN). The vapors responsible for new particle formation (NPF), potentially leading to CCN, have remained unidentified since the first aerosol measurements in 1991. Here, we report that all the observed NPF events from the Arctic Ocean 2018 expedition are driven by iodic acid with little contribution from sulfuric acid. Iodic acid largely explains the growth of ultrafine particles (UFP) in most events. The iodic acid concentration increases significantly from summer towards autumn, possibly linked to the ocean freeze-up and a seasonal rise in ozone. This leads to a one order of magnitude higher UFP concentration in autumn. Measurements of cloud residuals suggest that particles smaller than 30nm in diameter can activate as CCN. Therefore, iodine NPF has the potential to influence cloud properties over the Arctic Ocean. Which vapors are responsible for new particle formation in the Arctic is largely unknown. Here, the authors show that the formation of new particles at the central Arctic Ocean is mainly driven by iodic acid and that particles smaller than 30nm in diameter can activate as cloud condensation nuclei.
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| 2. |
- Christiansen, Sigurd, et al.
(författare)
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Influence of Arctic Microlayers and Algal Cultures on Sea Spray Hygroscopicity and the Possible Implications for Mixed-Phase Clouds
- 2020
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Ingår i: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 125:19
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Tidskriftsartikel (refereegranskat)abstract
- As Arctic sea ice cover diminishes, sea spray aerosols (SSA) have a larger potential to be emitted into the Arctic atmosphere. Emitted SSA can contain organic material, but how it affects the ability of particles to act as cloud condensation nuclei (CCN) is still not well understood. Here we measure the CCN-derived hygroscopicity of three different types of aerosol particles: (1) Sea salt aerosols made from artificial seawater, (2) aerosol generated from artificial seawater spiked with diatom species cultured in the laboratory, and (3) aerosols made from samples of sea surface microlayer (SML) collected during field campaigns in the North Atlantic and Arctic Ocean. Samples are aerosolized using a sea spray simulation tank (plunging jet) or an atomizer. We show that SSA containing diatom and microlayer exhibit similar CCN activity to inorganic sea salt with a κ value of ∼1.0. Large-eddy simulation (LES) is then used to evaluate the general role of aerosol hygroscopicity in governing mixed-phase low-level cloud properties in the high Arctic. For accumulation mode aerosol, the simulated mixed-phase cloud properties do not depend strongly on κ, unless the values are lower than 0.4. For Aitken mode aerosol, the hygroscopicity is more important; the particles can sustain the cloud if the hygroscopicity is equal to or higher than 0.4, but not otherwise. The experimental and model results combined suggest that the internal mixing of biogenic organic components in SSA does not have a substantial impact on the cloud droplet activation process and the cloud lifetime in Arctic mixed-phase clouds.
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| 3. |
- Cousins, Ian, et al.
(författare)
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Outside the Safe Operating Space of a New Planetary Boundary for Per- and Polyfluoroalkyl Substances (PFAS)
- 2022
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:16, s. 11172-11179
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Tidskriftsartikel (refereegranskat)abstract
- It is hypothesized that environmental contamination by per- and polyfluoroalkyl substances (PFAS) defines a separate planetary boundary and that this boundary has been exceeded. This hypothesis is tested by comparing the levels of four selected perfluoroalkyl acids (PFAAs) (i.e., perfluorooctanesulfonic acid (PFOS), perfluorooctanoic acid (PFOA), perfluorohexanesulfonic acid (PFHxS), and perfluorononanoic acid (PFNA)) in various global environmental media (i.e., rainwater, soils, and surface waters) with recently proposed guideline levels. On the basis of the four PFAAs considered, it is concluded that (1) levels of PFOA and PFOS in rainwater often greatly exceed US Environmental Protection Agency (EPA) Lifetime Drinking Water Health Advisory levels and the sum of the aforementioned four PFAAs (Σ4 PFAS) in rainwater is often above Danish drinking water limit values also based on Σ4 PFAS; (2) levels of PFOS in rainwater are often above Environmental Quality Standard for Inland European Union Surface Water; and (3) atmospheric deposition also leads to global soils being ubiquitously contaminated and to be often above proposed Dutch guideline values. It is, therefore, concluded that the global spread of these four PFAAs in the atmosphere has led to the planetary boundary for chemical pollution being exceeded. Levels of PFAAs in atmospheric deposition are especially poorly reversible because of the high persistence of PFAAs and their ability to continuously cycle in the hydrosphere, including on sea spray aerosols emitted from the oceans. Because of the poor reversibility of environmental exposure to PFAS and their associated effects, it is vitally important that PFAS uses and emissions are rapidly restricted.
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| 4. |
- Ickes, Luisa, 1986, et al.
(författare)
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The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
- 2020
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:18, s. 11089-11117
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Tidskriftsartikel (refereegranskat)abstract
- In recent years, sea spray as well as the biological material it contains has received increased attention as a source of ice-nucleating particles (INPs). Such INPs may play a role in remote marine regions, where other sources of INPs are scarce or absent. In the Arctic, these INPs can influence water-ice partitioning in low-level clouds and thereby the cloud lifetime, with consequences for the surface energy budget, sea ice formation and melt, and climate. Marine aerosol is of a diverse nature, so identifying sources of INPs is challenging. One fraction of marine bioaerosol (phytoplankton and their exudates) has been a particular focus of marine INP research. In our study we attempt to address three main questions. Firstly, we compare the ice-nucleating ability of two common phytoplankton species with Arctic seawater microlayer samples using the same instrumentation to see if these phytoplankton species produce ice-nucleating material with sufficient activity to account for the ice nucleation observed in Arctic microlayer samples. We present the first measurements of the ice-nucleating ability of two predominant phytoplankton species: Melosira arctica, a common Arctic diatom species, and Skeletonema marinoi, a ubiquitous diatom species across oceans worldwide. To determine the potential effect of nutrient conditions and characteristics of the algal culture, such as the amount of organic carbon associated with algal cells, on the ice nucleation activity, Skeletonema marinoi was grown under different nutrient regimes. From comparison of the ice nucleation data of the algal cultures to those obtained from a range of sea surface microlayer (SML) samples obtained during three different field expeditions to the Arctic (ACCACIA, NETCARE, and ASCOS), we found that they were not as ice active as the investigated microlayer samples, although these diatoms do produce ice-nucleating material. Secondly, to improve our understanding of local Arctic marine sources as atmospheric INPs we applied two aerosolization techniques to analyse the ice-nucleating ability of aerosolized microlayer and algal samples. The aerosols were generated either by direct nebulization of the undiluted bulk solutions or by the addition of the samples to a sea spray simulation chamber filled with artificial seawater. The latter method generates aerosol particles using a plunging jet to mimic the process of oceanic wave breaking. We observed that the aerosols produced using this approach can be ice active, indicating that the ice-nucleating material in seawater can indeed transfer to the aerosol phase. Thirdly, we attempted to measure ice nucleation activity across the entire temperature range relevant for mixed-phase clouds using a suite of ice nucleation measurement techniques - an expansion cloud chamber, a continuous-flow diffusion chamber, and a cold stage. In order to compare the measurements made using the different instruments, we have normalized the data in relation to the mass of salt present in the nascent sea spray aerosol. At temperatures above 248K some of the SML samples were very effective at nucleating ice, but there was substantial variability between the different samples. In contrast, there was much less variability between samples below 248 K. We discuss our results in the context of aerosol-cloud interactions in the Arctic with a focus on furthering our understanding of which INP types may be important in the Arctic atmosphere.
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| 5. |
- Karlsson, Linn, et al.
(författare)
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Physical and Chemical Properties of Cloud Droplet Residuals and Aerosol Particles During the Arctic Ocean 2018 Expedition
- 2022
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Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 127:11
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Tidskriftsartikel (refereegranskat)abstract
- Detailed knowledge of the physical and chemical properties and sources of particles that form clouds is especially important in pristine areas like the Arctic, where particle concentrations are often low and observations are sparse. Here, we present in situ cloud and aerosol measurements from the central Arctic Ocean in August–September 2018 combined with air parcel source analysis. We provide direct experimental evidence that Aitken mode particles (particles with diameters ≲70 nm) significantly contribute to cloud condensation nuclei (CCN) or cloud droplet residuals, especially after the freeze-up of the sea ice in the transition toward fall. These Aitken mode particles were associated with air that spent more time over the pack ice, while size distributions dominated by accumulation mode particles (particles with diameters ≳70 nm) showed a stronger contribution of oceanic air and slightly different source regions. This was accompanied by changes in the average chemical composition of the accumulation mode aerosol with an increased relative contribution of organic material toward fall. Addition of aerosol mass due to aqueous-phase chemistry during in-cloud processing was probably small over the pack ice given the fact that we observed very similar particle size distributions in both the whole-air and cloud droplet residual data. These aerosol–cloud interaction observations provide valuable insight into the origin and physical and chemical properties of CCN over the pristine central Arctic Ocean.
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| 6. |
- Lapere, Rémy, et al.
(författare)
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The Representation of Sea Salt Aerosols and Their Role in Polar Climate Within CMIP6
- 2023
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Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 128:6
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Tidskriftsartikel (refereegranskat)abstract
- Natural aerosols and their interactions with clouds remain an important uncertainty within climate models, especially at the poles. Here, we study the behavior of sea salt aerosols (SSaer) in the Arctic and Antarctic within 12 climate models from CMIP6. We investigate the driving factors that control SSaer abundances and show large differences based on the choice of the source function, and the representation of aerosol processes in the atmosphere. Close to the poles, the CMIP6 models do not match observed seasonal cycles of surface concentrations, likely due to the absence of wintertime SSaer sources such as blowing snow. Further away from the poles, simulated concentrations have the correct seasonality, but have a positive mean bias of up to one order of magnitude. SSaer optical depth is derived from the MODIS data and compared to modeled values, revealing good agreement, except for winter months. Better agreement for aerosol optical depth than surface concentration may indicate a need for improving the vertical distribution, the size distribution and/or hygroscopicity of modeled polar SSaer. Source functions used in CMIP6 emit very different numbers of small SSaer, potentially exacerbating cloud-aerosol interaction uncertainties in these remote regions. For future climate scenarios SSP126 and SSP585, we show that SSaer concentrations increase at both poles at the end of the 21st century, with more than two times mid-20th century values in the Arctic. The pre-industrial climate CMIP6 experiments suggest there is a large uncertainty in the polar radiative budget due to SSaer.Plain Language Summary Aerosols emitted from the ocean, such as sea salt particles (aerosols), are critical for the climate of polar regions. However, there is still uncertainty in their representation in climate models. The purpose of this work is to evaluate the representation of sea salt aerosols (SSaer) in the Arctic and Antarctic in a recent model inter-comparison initiative, and to assess the consequences for our understanding of present-day and future polar climate. We find that the models disagree between them and with observations from ground stations and from space. This suggests that the formulation of sea salt emissions in global models is not adapted for polar regions. With sea ice retreat, SSaer will most likely increase in the future, which makes addressing the current uncertainty an important next step for the scientific community.
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| 7. |
- Lawler, M. J., et al.
(författare)
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New Insights Into the Composition and Origins of Ultrafine Aerosol in the Summertime High Arctic
- 2021
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Ingår i: Geophysical Research Letters. - 0094-8276 .- 1944-8007. ; 48:21
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Tidskriftsartikel (refereegranskat)abstract
- The summertime high Arctic atmosphere is characterized by extremely low aerosol abundance, such that small natural aerosol inputs have a strong influence on cloud formation and surface temperature. The physical sources and the mechanisms responsible for aerosol formation and development in this climate-critical and changing region are still uncertain. We report time-resolved measurements of high Arctic Aitken mode (∼20–60 nm diameter) aerosol composition during August–September 2018. During a significant Aitken mode formation event, the particles were composed of a combination of primary and secondary materials. These results highlight the importance of primary aerosol sources for high Arctic cloud formation, and they imply the action of a poorly understood atmospheric mechanism separating larger particles into multiple sub-particles.
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| 8. |
- Patanen, Minna, et al.
(författare)
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Surface composition of size-selected sea salt particles under the influence of organic acids studied in situ using synchrotron radiation X-ray photoelectron spectroscopy
- 2022
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Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1032-1040
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Tidskriftsartikel (refereegranskat)abstract
- Sea spray aerosols play a key role in the climate system by scattering solar radiation and by serving as cloud condensation nuclei. Despite their importance, the impact of sea spray aerosols on global climate remains highly uncertain. One of the key knowledge gaps in our understanding of sea spray aerosol is the chemical composition of the particle surface, important for various atmospheric chemical processes, as a function of size and bulk composition. Here, we have applied X-ray photoelectron spectroscopy (XPS) to determine the surface composition of both pure inorganic sea salt aerosols and sea salt aerosols spiked with an amino acid (phenylalanine) and a straight chain fatty acid (octanoic acid). Importantly, the use of a differential mobility analyser allowed size-selection of 150, 250 and 350 nm monodisperse aerosol particles for comparison to polydisperse aerosol particles. We observed enrichment of magnesium at the particle surfaces relative to chloride in all aerosols tested, across all particle sizes. Interestingly, the magnitude of this enrichment was dependent on the type of organic present in the solution as well as the particle size. Our results suggest that the observed enrichment in magnesium is an inorganic effect which can be either enhanced or diminished by the addition of organic substances.
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| 9. |
- Pereira Freitas, Gabriel, 1993-, et al.
(författare)
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Emission of primary bioaerosol particles from Baltic seawater
- 2022
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Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1170-1182
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Tidskriftsartikel (refereegranskat)abstract
- Bioaerosols are particles of biological origin with various important atmospheric implications, for example, within cloud formation where bioaerosols can act as cloud condensation or ice nuclei. Their sources and properties, however, are poorly understood. We conducted a controlled sea spray experiment to determine the properties and emission of primary biological aerosol particles (PBAP) originating from Baltic seawater. Using a single-particle fluorescence and light-scattering instrument, the Multiparameter Bioaerosol Spectrometer (MBS), we differentiated PBAP within sea spray aerosol (SSA). Overall, approximately 1 in 104 particles larger than 0.8 μm in diameter were classified as PBAP. The optically-determined morphology of the nascent and fluorescent SSA particles showed a clear transition in symmetry and elongation most likely due to changes in the biogeochemical properties of the surface water. These shifts were also reflected in a clear change of the bacterial community composition of the aerosol and seawater as determined by 16S rRNA-gene analysis, which were significantly distinct from each other, suggesting a preferential emission of specific bacteria to the atmosphere. Our results demonstrate the capability of the MBS to identify and count PBAP within SSA on a single-particle basis and will help to better constrain the emission of marine PBAP and their dependence on the seawater's biogeochemical properties.
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| 10. |
- Porter, Grace C.E., et al.
(författare)
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Highly Active Ice-Nucleating Particles at the Summer North Pole
- 2022
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Ingår i: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 127:6
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Tidskriftsartikel (refereegranskat)abstract
- The amount of ice versus supercooled water in clouds is important for their radiative properties and role in climate feedbacks. Hence, knowledge of the concentration of ice-nucleating particles (INPs) is needed. Generally, the concentrations of INPs are found to be very low in remote marine locations allowing cloud water to persist in a supercooled state. We had expected the concentrations of INPs at the North Pole to be very low given the distance from open ocean and terrestrial sources coupled with effective wet scavenging processes. Here we show that during summer 2018 (August and September) high concentrations of biological INPs (active at >−20°C) were sporadically present at the North Pole. In fact, INP concentrations were sometimes as high as those recorded at mid-latitude locations strongly impacted by highly active biological INPs, in strong contrast to the Southern Ocean. Furthermore, using a balloon borne sampler we demonstrated that INP concentrations were often different at the surface versus higher in the boundary layer where clouds form. Back trajectory analysis suggests strong sources of INPs near the Russian coast, possibly associated with wind-driven sea spray production, whereas the pack ice, open leads, and the marginal ice zone were not sources of highly active INPs. These findings suggest that primary ice production, and therefore Arctic climate, is sensitive to transport from locations such as the Russian coast that are already experiencing marked climate change.
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