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Sökning: WFRF:(Salter Matthew)

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3.
  • Baccarini, Andrea, et al. (författare)
  • Frequent new particle formation over the high Arctic pack ice by enhanced iodine emissions
  • 2020
  • Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 11:1
  • 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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4.
  • Boy, M., et al. (författare)
  • Interactions between the atmosphere, cryosphere, and ecosystems at northern high latitudes
  • 2019
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:3, s. 2015-2061
  • Tidskriftsartikel (refereegranskat)abstract
    • The Nordic Centre of Excellence CRAICC (Cryosphere-Atmosphere Interactions in a Changing Arctic Climate), funded by NordForsk in the years 2011-2016, is the largest joint Nordic research and innovation initiative to date, aiming to strengthen research and innovation regarding climate change issues in the Nordic region. CRAICC gathered more than 100 scientists from all Nordic countries in a virtual centre with the objectives of identifying and quantifying the major processes controlling Arctic warming and related feedback mechanisms, outlining strategies to mitigate Arctic warming, and developing Nordic Earth system modelling with a focus on short-lived climate forcers (SLCFs), including natural and anthropogenic aerosols. The outcome of CRAICC is reflected in more than 150 peer-reviewed scientific publications, most of which are in the CRAICC special issue of the journal Atmospheric Chemistry and Physics. This paper presents an overview of the main scientific topics investigated in the centre and provides the reader with a state-of-the-art comprehensive summary of what has been achieved in CRAICC with links to the particular publications for further detail. Faced with a vast amount of scientific discovery, we do not claim to completely summarize the results from CRAICC within this paper, but rather concentrate here on the main results which are related to feedback loops in climate change-cryosphere interactions that affect Arctic amplification.
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5.
  • Christiansen, Sigurd, et al. (författare)
  • Influence of Arctic Microlayers and Algal Cultures on Sea Spray Hygroscopicity and the Possible Implications for Mixed-Phase Clouds
  • 2020
  • Ingår i: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 125:19
  • 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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6.
  • Christiansen, Sigurd, et al. (författare)
  • Sea Spray Aerosol Formation : Laboratory Results on the Role of Air Entrainment, Water Temperature, and Phytoplankton Biomass
  • 2019
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 53:22, s. 13107-13116
  • Tidskriftsartikel (refereegranskat)abstract
    • Sea spray aerosol (SSA) emission is a complex process affected by various controlling factors. This work seeks to deconvolute some of this complexity in a controlled laboratory setting using a plunging jet by varying three key parameters, one at a time: (1) air entrainment rate, (2) seawater temperature, and (3) biomass of phytoplankton. The production of SSA is found to vary linearly with air entrainment rate. By normalizing the production flux to air entrainment rate, we observe nonlinear variation of the production efficiency of SSA with seawater temperature with a minimum around 6-10 degrees C. For comparison, SSA was also generated by detraining air into artificial seawater using a diffuser demonstrating that the production efficiency of SSA generated using a diffuser decreases almost linearly with increasing seawater temperature, and the production efficiency is, significantly higher than that for SSA generated using a plunging jet. Finally, by varying the amount of phytoplankton biomass we demonstrate that SSA particle production varies nonlinearly with the amount of biomass in seawater.
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7.
  • Cousins, Ian, et al. (författare)
  • Outside the Safe Operating Space of a New Planetary Boundary for Per- and Polyfluoroalkyl Substances (PFAS)
  • 2022
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:16, s. 11172-11179
  • 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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8.
  • Cunliffe, Michael, et al. (författare)
  • Sea surface microlayers : A unified physicochemical and biological perspective of the air-ocean interface
  • 2013
  • Ingår i: Progress in Oceanography. - : Elsevier BV. - 0079-6611 .- 1873-4472. ; 109, s. 104-116
  • Forskningsöversikt (refereegranskat)abstract
    • The sea surface microlayer (SML) covers more than 70% of the Earth's surface and is the boundary layer interface between the ocean and the atmosphere. This important biogeochemical and ecological system is critical to a diverse range of Earth system processes, including the synthesis, transformation and cycling of organic material, and the air-sea exchange of gases, particles and aerosols. In this review we discuss the SML paradigm, taking into account physicochemical and biological characteristics that define SML structure and function. These include enrichments in biogenic molecules such as carbohydrates, lipids and proteinaceous material that contribute to organic carbon cycling, distinct microbial assemblages that participate in air-sea gas exchange, the generation of climate-active aerosols and the accumulation of anthropogenic pollutants with potentially serious implications for the health of the ocean. Characteristically large physical, chemical and biological gradients thus separate the SML from the underlying water and the available evidence implies that the SML retains its integrity over wide ranging environmental conditions. In support of this we present previously unpublished time series data on bacterioneuston composition and SML surfactant activity immediately following physical SML disruption; these imply timescales of the order of minutes for the reestablishment of the SML following disruption. A progressive approach to understanding the SML and hence its role in global biogeochemistry can only be achieved by considering as an integrated whole, all the key components of this complex environment.
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9.
  • Escobar, Matthew, et al. (författare)
  • Light regulation of the Arabidopsis respiratory chain. Multiple discrete photoreceptor responses contribute to induction of type II NAD(P)H dehydrogenase genes
  • 2004
  • Ingår i: Plant Physiology. - : Oxford University Press (OUP). - 1532-2548 .- 0032-0889. ; 136:1, s. 2710-2721
  • Tidskriftsartikel (refereegranskat)abstract
    • Controlled oxidation reactions catalyzed by the large, proton-pumping complexes of the respiratory chain generate an electrochemical gradient across the mitochondrial inner membrane that is harnessed for ATP production. However, several alternative respiratory pathways in plants allow the maintenance of substrate oxidation while minimizing the production of ATE We have investigated the role of light in the regulation of these energy-dissipating pathways by transcriptional profiling of the alternative oxidase, uncoupling protein, and type II NAD(P)H dehydrogenase gene families in etiolated Arabidopsis seedlings. Expression of the nda1 and ndc1 NAD(P)H dehydrogenase genes was rapidly up-regulated by a broad range of light intensities and qualities. For both genes, light induction appears to be a direct transcriptional effect that is independent of carbon status. Mutant analyses demonstrated the involvement of two separate photoreceptor families in nda1 and ndc1 light regulation: the phytochromes (phyA and phyB) and an undetermined blue light photoreceptor. In the case of the nda1 gene, the different photoreceptor systems generate distinct kinetic induction profiles that are integrated in white light response. Primary transcriptional control of light response was localized to a 99-bp region of the nda1 promoter, which contains an 1-box flanked by two GT-1 elements, an arrangement prevalent in the promoters of photosynthesis-associated genes. Light induction was specific to nda1 and ndc1. The only other substantial light effect observed was a decrease in aox2 expression. Overall, these results suggest that light directly influences the respiratory electron transport chain via photoreceptor-mediated transcriptional control, likely for supporting photosynthetic metabolism.
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10.
  • Franke, Vera, et al. (författare)
  • Chemical composition and source analysis of carbonaceous aerosol particles at a mountaintop site in central Sweden
  • 2017
  • Ingår i: Tellus. Series B, Chemical and physical meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 69
  • Tidskriftsartikel (refereegranskat)abstract
    • The chemical composition of atmospheric particulate matter at Mt. angstrom reskutan, a mountaintop site in central Sweden, was analysed with a focus on its carbonaceous content. Filter samples taken during the Cloud and Aerosol Experiment at angstrom re (CAEsAR 2014) were analysed by means of a thermo-optical method and ion chromatography. Additionally, the particle light absorption and particle number size distribution measurements for the entire campaign were added to the analysis. Mean airborne concentrations of organic and elemental carbon during CAEsAR 2014 were OC= 0.85 +/- 0.8 mu gm(-3) and EC = 0.06 +/- 0.06 mu gm(-3), respectively. Elemental to organic carbon ratios varied between EC/OC = 0.02 and 0.19. During the study a large wildfire occurred in Vastmanland, Sweden, with the plume reaching our study site. This led to significant increases in OC and EC concentrations (OC = 3.04 +/- 0.03 mu gm(-3) and EC = 0.24 +/- 0.00 mu gm(-3)). The mean mass-specific absorption coefficient observed during the campaign was sigma(BC)(abs) = 9.1 +/- 7.3 m(2)g(-1) (at wavelength lambda= 637 nm). In comparison to similarly remote European sites, Mt. angstrom reskutan experienced significantly lower carbonaceous aerosol loadings with a clear dominance of organic carbon. A mass closure study revealed a missing chemical mass fraction that likely originated from mineral dust. Potential regional source contributions of the carbonaceous aerosol were investigated using modelled air mass back trajectories. This source apportionment pointed to a correlation between high EC concentrations and air originating from continental Europe. Particles rich in organic carbon most often arrived from highly vegetated continental areas. However, marine regions were also a source of these aerosol particles. The source contributions derived during this study were compared to emission inventories of an Earth system model. This comparison highlighted a lack of OC and EC point-sources in the model's emission inventory which could potentially lead to an underestimation of the carbonaceous aerosol reaching Mt. angstrom reskutan in the simulation of this Earth system model.
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11.
  • Ickes, Luisa, 1986, et al. (författare)
  • The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
  • 2020
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:18, s. 11089-11117
  • 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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13.
  • Johansson, Jana H., et al. (författare)
  • Global transport of perfluoroalkyl acids via sea spray aerosol
  • 2019
  • Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2050-7887 .- 2050-7895. ; 21:4, s. 635-649
  • Tidskriftsartikel (refereegranskat)abstract
    • Perfluoroalkyl acids (PFAAs) are persistent organic pollutants found throughout the world's oceans. Previous research suggests that long-range atmospheric transport of these substances may be substantial. However, it remains unclear what the main sources of PFAAs to the atmosphere are. We have used a laboratory sea spray chamber to study water-to-air transfer of 11 PFAAs via sea spray aerosol (SSA). We observed significant enrichment of all PFAAs relative to sodium in the SSA generated. The highest enrichment was observed in aerosols with aerodynamic diameter < 1.6 mm, which had aerosol PFAA concentrations up to similar to 62 000 times higher than the PFAA water concentrations in the chamber. In surface microlayer samples collected from the sea spray chamber, the enrichment of the substances investigated was orders of magnitude smaller than the enrichment observed in the aerosols. In experiments with mixtures of structural isomers, a lower contribution of branched PFAA isomers was observed in the surface microlayer compared to the bulk water. However, no clear trend was observed in the comparison of structural isomers in SSA and bulk water. Using the measured enrichment factors of perfluorooctanoic acid and perfluorooctane sulfonic acid versus sodium we have estimated global annual emissions of these substances to the atmosphere via SSA as well as their global annual deposition to land areas. Our experiments suggest that SSA may currently be an important source of these substances to the atmosphere and, over certain areas, to terrestrial environments.
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14.
  • Johansson, Jana H., et al. (författare)
  • Spatial variation in the atmospheric deposition of perfluoroalkyl acids : source elucidation through analysis of isomer patterns
  • 2018
  • Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2050-7887 .- 2050-7895. ; 20:7, s. 997-1006
  • Tidskriftsartikel (refereegranskat)abstract
    • To evaluate the relevance of different proposed sources of perfluoroalkyl acids (PFAAs) to air, their isomer patterns were analyzed in deposition samples collected from five geographical locations: two urban sites in China (>360 km from known operational fluorochemical manufacturing facilities), one remote marine site in the Azores archipelago and two Swedish sites representing urban and background conditions. Despite variable contributions from linear perfluorooctanoic acid (PFOA) in the samples, the pattern of branched PFOA isomers was similar to those of technical standards manufactured using electrochemical fluorination (ECF). This indicates that atmospheric fate processes have little influence on the isomer profiles of PFOA and that the relative contribution of PFOA manufactured using ECF (typically 20-26% branched isomers) and telomerization (typically one single linear isomer) can be determined in atmospheric deposition samples by analyzing the proportions of branched and linear isomers. In Chinese samples, branched isomers contributed 15-25% to the total loading of PFOA, indicating that the samples were dominated by ECF PFOA. Samples in the Azores had 8-10% contribution from branched PFOA isomers, indicating an approximately equal influence of ECF and telomer sources. Only three of the samples collected in Sweden displayed a quantifiable contribution from branched PFOA isomers (8-13% of overall PFOA loading in the samples). One branched PFNA isomer was observed in samples from the marine sites. Direct manufacturing discharges, transport of sea spray aerosols and degradation of precursors are all suggested to be contributing sources, albeit to different extents, to PFAAs in air at the different geographical locations where precipitation was sampled.
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15.
  • Karlsson, Linn, et al. (författare)
  • Physical and Chemical Properties of Cloud Droplet Residuals and Aerosol Particles During the Arctic Ocean 2018 Expedition
  • 2022
  • Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 127:11
  • 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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16.
  • Lapere, Rémy, et al. (författare)
  • The Representation of Sea Salt Aerosols and Their Role in Polar Climate Within CMIP6
  • 2023
  • Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 128:6
  • 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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17.
  • Lawler, M. J., et al. (författare)
  • New Insights Into the Composition and Origins of Ultrafine Aerosol in the Summertime High Arctic
  • 2021
  • Ingår i: Geophysical Research Letters. - 0094-8276 .- 1944-8007. ; 48:21
  • 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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18.
  • Mann, P. J., et al. (författare)
  • The biogeochemistry of carbon across a gradient of streams and rivers within the Congo Basin
  • 2014
  • Ingår i: Journal of Geophysical Research: Biogeosciences. - 2169-8953. ; 119:4, s. 687-702
  • Tidskriftsartikel (refereegranskat)abstract
    • Dissolved organic carbon (DOC) and inorganic carbon (DIC, pCO(2)), lignin biomarkers, and theoptical properties of dissolved organic matter (DOM) were measured in a gradient of streams and rivers within the Congo Basin, with the aim of examining how vegetation cover and hydrology influences the composition and concentration of fluvial carbon (C). Three sampling campaigns (February 2010, November 2010, and August 2011) spanning 56 sites are compared by subbasin watershed land cover type (savannah, tropical forest, and swamp) and hydrologic regime (high, intermediate, and low). Land cover properties predominately controlled the amount and quality of DOC, chromophoric DOM (CDOM) and lignin phenol concentrations (Sigma(8)) exported in streams and rivers throughout the Congo Basin. Higher DIC concentrations and changing DOM composition (lower molecular weight, less aromatic C) during periods of low hydrologic flow indicated shifting rapid overland supply pathways in wet conditions to deeper groundwater inputs during drier periods. Lower DOC concentrations in forest and swamp subbasins were apparent with increasing catchment area, indicating enhanced DOC loss with extended water residence time. Surface water pCO(2) in savannah and tropical forest catchments ranged between 2,600 and 11,922 mu atm, with swamp regions exhibiting extremely high pCO(2) (10,598-15,802 mu atm), highlighting their potential as significant pathways for water-air efflux. Our data suggest that the quantity and quality of DOM exported to streams and rivers are largely driven by terrestrial ecosystem structure and that anthropogenic land use or climate change may impact fluvial C composition and reactivity, with ramifications for regional C budgets and future climate scenarios.
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19.
  • Patanen, Minna, et al. (författare)
  • 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
  • Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1032-1040
  • 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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20.
  • Pereira Freitas, Gabriel, 1993-, et al. (författare)
  • Emission of primary bioaerosol particles from Baltic seawater
  • 2022
  • Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1170-1182
  • 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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21.
  • Porter, Grace C.E., et al. (författare)
  • Highly Active Ice-Nucleating Particles at the Summer North Pole
  • 2022
  • Ingår i: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 127:6
  • 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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22.
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23.
  • Radoman, Nikola, 1985- (författare)
  • Enrichment of biogenic and anthropogenic organic substances on sea spray aerosols
  • 2022
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • The world’s oceans are the source of one of the most abundant types of natural aerosols, namely sea spray aerosols (SSA). By scattering solar radiation, SSA play a significant role in controlling the Earth’s radiation budget, while they are also involved in the formation of clouds, acting as cloud condensation nuclei (CCN). To understand the connection between biogeochemical processes occurring in the ocean and in the atmosphere, it is crucial to gain better insight into the detailed chemical composition of SSA, which broadly consists of sea salt and marine organic matter. The aim of this thesis is to (1) better understand the impact of ocean biological activity on the chemical composition of SSA and (2) improve the knowledge on the ability of SSA to transport different organic pollutants to the atmosphere. In Paper I it was shown that changes in the composition of marine organic matter during a phytoplankton bloom in the North Atlantic were clearly reflected in the composition of generated SSA. Increased chlorophyll a concentration in seawater was correlated with the presence of lipid-like compounds with high H/C and low O/C atomic ratios, and a consistent trend in chemical composition was observed for subsurface water, the surface microlayer, and generated SSA. Although the effect of biological processes on the composition of SSA organic matter was clear, in Paper II it was shown that during the phytoplankton bloom, the abundance of organic matter in SSA was fairly constant, without any significant influence on their CCN activity or the particle production flux. Paper III provided a mechanistic understanding of the enrichment of different cationic surfactants (CSs) in SSA through experiments conducted using a sea spray simulation chamber. It was shown that enrichment of the CSs was primarily driven by the alkyl chain length of the CSs but also affected by the different functional groups in the CSs. The highest enrichment of CSs on SSA was observed for quaternary amines followed by primary and tertiary amines. Interaction with dissolved humic acid was shown to decrease the enrichment of longer-chain amines while the enrichment was increased for shorter-chain ones. When the plunging jet flow rate was increased, enrichment in SSA was shown to increase, especially for lower water concentrations of surface-active compounds. The purpose of Paper IV was to improve the understanding of the enrichment behavior of perfluoroalkyl acids (PFAAs), which are strong anionic surfactants. Similar to CSs, it was shown that increasing the plunging jet flow increased the enrichment on SSA, from 43-88% for different PFAAs. The effect of different inorganic salts present in seawater on enrichment was also tested. Compared to chamber experiments prepared with ~35% NaCl water matrix, it was shown that the presence of other seawater ions, namely Ca2+ and Mg2+, increased the enrichment of some PFAAs, especially for those with longer perfluoroalkyl chains.
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24.
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25.
  • Radoman, Nikola, et al. (författare)
  • Probing the impact of a phytoplankton bloom on the chemistry of nascent sea spray aerosol using high-resolution mass spectrometry
  • 2022
  • Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1152-1169
  • Tidskriftsartikel (refereegranskat)abstract
    • Sea spray aerosol is the largest natural source of aerosol to Earth's atmosphere with significant impacts on climate. Despite this, estimates of the impact of sea spray aerosol on Earth's radiation budget are highly uncertain due to an overall lack of understanding of the physical and chemical factors controlling its composition. Critically, results from studies probing the importance of oceanic biological activity on the amount and type of organic matter present in nascent sea spray aerosol have been ambiguous. Some field studies have shown a relationship between the organic fraction of sea spray aerosol and oceanic primary productivity while others have reported no such relationships. Given this, we have probed the composition of seawater and nascent sea spray aerosol during a phytoplankton bloom in the North Atlantic using a novel liquid chromatography-mass spectrometry method. We observed that the composition of dissolved organic matter present in seawater changed as the phytoplankton bloom progressed over an 18 day period. Further, we observed changes to both the chemical composition of the organic matter present in seawater and the chemical composition of the organic matter present in the sea spray aerosol despite the organic matter mass fraction of the aerosol remaining unchanged. More specifically, we observed that the nascent sea spray aerosol became progressively more enriched in surface-active organic substances as the bloom progressed and that the sea spray aerosol had a distinct organic matter composition compared to the seawater. Thus, our work provides additional insight into the biological dependence of nascent sea spray aerosol composition.
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26.
  • Renard, Jean-Baptiste, et al. (författare)
  • LOAC : a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles - Part 1
  • 2016
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 9:4, s. 1721-1742
  • Tidskriftsartikel (refereegranskat)abstract
    • The study of aerosols in the troposphere and in the stratosphere is of major importance both for climate and air quality studies. Among the numerous instruments available, optical aerosol particles counters (OPCs) provide the size distribution in diameter range from about 100 nm to a few tens of mu m. Most of them are very sensitive to the nature of aerosols, and this can result in significant biases in the retrieved size distribution. We describe here a new versatile optical particle/sizer counter named LOAC (Light Optical Aerosol Counter), which is light and compact enough to perform measurements not only at the surface but under all kinds of balloons in the troposphere and in the stratosphere. LOAC is an original OPC performing observations at two scattering angles. The first one is around 12 degrees, and is almost insensitive to the refractive index of the particles; the second one is around 60 degrees and is strongly sensitive to the refractive index of the particles. By combining measurement at the two angles, it is possible to retrieve the size distribution between 0.2 and 100 mu m and to estimate the nature of the dominant particles (droplets, carbonaceous, salts and mineral particles) when the aerosol is relatively homogeneous. This typology is based on calibration charts obtained in the laboratory. The uncertainty for total concentrations measurements is +/- 20% when concentrations are higher than 1 particle cm 3 (for a 10 min integration time). For lower concentrations, the uncertainty is up to about +/- 60% for concentrations smaller than 10 2 particle cm(-3). Also, the uncertainties in size calibration are +/- 0.025 mu m for particles smaller than 0.6 mu m, 5% for particles in the 0.7-2 mu m range, and 10% for particles greater than 2 mu m. The measurement accuracy of sub-micronic particles could be reduced in a strongly turbid case when concentration of particles > 3 mu m exceeds a few particles cm(-3). Several campaigns of cross-comparison of LOAC with other particle counting instruments and remote sensing photometers have been conducted to validate both the size distribution derived by LOAC and the retrieved particle number density. The typology of the aerosols has been validated in well-defined conditions including urban pollution, desert dust episodes, sea spray, fog, and cloud. Comparison with reference aerosol mass monitoring instruments also shows that the LOAC measurements can be successfully converted to mass concentrations.
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27.
  • Renard, Jean-Baptiste, et al. (författare)
  • LOAC : a small aerosol optical counter/sizer for ground-based and balloon measurements of the size distribution and nature of atmospheric particles - Part 2
  • 2016
  • Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 9:8, s. 3673-3686
  • Tidskriftsartikel (refereegranskat)abstract
    • In the companion (Part I) paper, we have described and evaluated a new versatile optical particle counter/sizer named LOAC (Light Optical Aerosol Counter), based on scattering measurements at angles of 12 and 60A degrees. That allows for some typology identification of particles (droplets, carbonaceous, salts, and mineral dust) in addition to size-segregated counting in a large diameter range from 0.2aEuro-A mu m up to possibly more than 100aEuro-A mu m depending on sampling conditions (Renard et al., 2016). Its capabilities overpass those of preceding optical particle counters (OPCs) allowing the characterization of all kind of aerosols from submicronic-sized absorbing carbonaceous particles in polluted air to very coarse particles (> 10-20aEuro-A mu m in diameter) in desert dust plumes or fog and clouds. LOAC's light and compact design allows measurements under all kinds of balloons, on-board unmanned aerial vehicles (UAVs) and at ground level. We illustrate here the first LOAC airborne results obtained from a UAV and a variety of scientific balloons. The UAV was deployed in a peri-urban environment near Bordeaux in France. Balloon operations include (i) tethered balloons deployed in urban environments in Vienna (Austria) and Paris (France), (ii) pressurized balloons drifting in the lower troposphere over the western Mediterranean (during the Chemistry-Aerosol Mediterranean Experiment - ChArMEx campaigns), (iii) meteorological sounding balloons launched in the western Mediterranean region (ChArMEx) and from Aire-sur-l'Adour in south-western France (VOLTAIRE-LOAC campaign). More focus is put on measurements performed in the Mediterranean during (ChArMEx) and especially during African dust transport events to illustrate the original capability of balloon-borne LOAC to monitor in situ coarse mineral dust particles. In particular, LOAC has detected unexpected large particles in desert sand plumes.
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28.
  • Salter, Matthew E., et al. (författare)
  • An empirically derived inorganic sea spray source function incorporating sea surface temperature
  • 2015
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:19, s. 11047-11066
  • Tidskriftsartikel (refereegranskat)abstract
    • We have developed an inorganic sea spray source function that is based upon state-of-the-art measurements of sea spray aerosol production using a temperature-controlled plunging jet sea spray aerosol chamber. The size-resolved particle production was measured between 0.01 and 10 mu m dry diameter. Particle production decreased non-linearly with increasing seawater temperature (between -1 and 30 degrees C) similar to previous findings. In addition, we observed that the particle effective radius, as well as the particle surface, particle volume and particle mass, increased with increasing seawater temperature due to increased production of particles with dry diameters greater than 1 mu m. By combining these measurements with the volume of air entrained by the plunging jet we have determined the size-resolved particle flux as a function of air entrainment. Through the use of existing parameterisations of air entrainment as a function of wind speed, we were subsequently able to scale our laboratory measurements of particle production to wind speed. By scaling in this way we avoid some of the difficulties associated with defining the white area of the laboratory whitecap - a contentious issue when relating laboratory measurements of particle production to oceanic whitecaps using the more frequently applied whitecap method. The here-derived inorganic sea spray source function was implemented in a Lagrangian particle dispersion model (FLEXPART - FLEXible PARTicle dispersion model). An estimated annual global flux of inorganic sea spray aerosol of 5.9 +/- 0.2 Pg yr(-1) was derived that is close to the median of estimates from the same model using a wide range of existing sea spray source functions. When using the source function derived here, the model also showed good skill in predicting measurements of Na+ concentration at a number of field sites further underlining the validity of our source function. In a final step, the sensitivity of a large-scale model (NorESM - the Norwegian Earth System Model) to our new source function was tested. Compared to the previously implemented parameterisation, a clear decrease of sea spray aerosol number flux and increase in aerosol residence time was observed, especially over the Southern Ocean. At the same time an increase in aerosol optical depth due to an increase in the number of particles with optically relevant sizes was found. That there were noticeable regional differences may have important implications for aerosol optical properties and number concentrations, subsequently also affecting the indirect radiative forcing by non-sea spray anthropogenic aerosols.
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29.
  • Salter, Matthew E., et al. (författare)
  • Calcium enrichment in sea spray aerosol particles
  • 2016
  • Ingår i: Geophysical Research Letters. - : Blackwell Publishing. - 0094-8276 .- 1944-8007. ; 43:15, s. 8277-8285
  • Tidskriftsartikel (refereegranskat)abstract
    • Sea spray aerosol particles are an integral part of the Earth's radiation budget. To date, the inorganic composition of nascent sea spray aerosol particles has widely been assumed to be equivalent to the inorganic composition of seawater. Here we challenge this assumption using a laboratory sea spray chamber containing both natural and artificial seawater, as well as with ambient aerosol samples collected over the central Arctic Ocean during summer. We observe significant enrichment of calcium in submicrometer (<1 μm in diameter) sea spray aerosol particles when particles are generated from both seawater sources in the laboratory as well as in the ambient aerosols samples. We also observe a tendency for increasing calcium enrichment with decreasing particle size. Our results suggest that calcium enrichment in sea spray aerosol particles may be environmentally significant with implications for our understanding of sea spray aerosol, its impact on Earth's climate, as well as the chemistry of the marine atmosphere.
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30.
  • Salter, Matthew E., et al. (författare)
  • On the seawater temperature dependence of the sea spray aerosol generated by a continuous plunging jet
  • 2014
  • Ingår i: Journal of Geophysical Research - Atmospheres. - 2169-897X .- 2169-8996. ; 119:14, s. 9052-9072
  • Tidskriftsartikel (refereegranskat)abstract
    • Breaking waves on the ocean surface produce bubbles which, upon bursting, deliver seawater constituents into the atmosphere as sea spray aerosol particles. One way of investigating this process in the laboratory is to generate a bubble plume by a continuous plunging jet. We performed a series of laboratory experiments to elucidate the role of seawater temperature on aerosol production from artificial seawater free from organic contamination using a plunging jet. The seawater temperature was varied from -1.3 degrees C to 30.1 degrees C, while the volume of air entrained by the jet, surface bubble size distributions, and size distribution of the aerosol particles produced was monitored. We observed that the volume of air entrained decreased as the seawater temperature was increased. The number of surface bubbles with film radius smaller than 2 mm decreased nonlinearly with seawater temperature. This decrease was coincident with a substantial reduction in particle production. The number concentrations of particles with dry diameter less than similar to 1 mu m decreased substantially as the seawater temperature was increased from -1.3 degrees C to similar to 9 degrees C. With further increase in seawater temperature (up to 30 degrees C), a small increase in the number concentration of larger particles (dry diameter >similar to 0.3 mu m) was observed. Based on these observations, we infer that as seawater temperature increases, the process of bubble fragmentation changes, resulting in decreased air entrainment by the plunging jet, as well as the number of bubbles with film radius smaller than 2 mm. This again results in decreased particle production with increasing seawater temperature.
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31.
  • Savvidou, Eleni Konstantina, 1994-, et al. (författare)
  • Horizontal and Vertical Distribution of Perfluoroalkyl Acids (PFAAs) in the Water Column of the Atlantic Ocean
  • 2023
  • Ingår i: Environmental Science and Technology Letters. - : AMER CHEMICAL SOC. - 2328-8930. ; 10:5, s. 418-424
  • Tidskriftsartikel (refereegranskat)abstract
    • Perfluoroalkyl acids (PFAAs) are widely distributed in the oceans which are their largest global reservoir, but knowledge is limited about their vertical distribution and fate. This study measured the concentrations of PFAAs (perfluoroalkyl carboxylic acids (PFCAs) with 6 to 11 carbons and perfluoroalkanesulfonic acids (PFSAs) with 6 and 8 carbons) in the surface and deep ocean. Seawater depth profiles from the surface to a 5000 m depth at 28 sampling stations were collected in the Atlantic Ocean from similar to 50 degrees N to similar to 50 degrees S. The results demonstrated PFAA input from the Mediterranean Sea and the English Channel. Elevated PFAA concentrations were observed at the eastern edge of the Northern Atlantic Subtropical Gyre, suggesting that persistent contaminants may accumulate in ocean gyres. The median sigma PFAA surface concentration in the Northern Hemisphere (n = 17) was 105 pg L-1, while for the Southern Hemisphere (n = 11) it was 28 pg L-1. Generally, PFAA concentrations decreased with increasing distance to the coast and increasing depth. The C6-C9 PFCAs and C6 and C8 PFSAs dominated in surface waters, while longer-chain PFAAs (C10-C11 PFCAs) peaked at intermediate depths (500-1500 m). This profile may be explained by stronger sedimentation of longer-chain PFAAs, as they sorb more strongly to particulate organic matter.
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32.
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33.
  • Schneider-Zapp, K., et al. (författare)
  • An automated gas exchange tank for determining gas transfer velocities in natural seawater samples
  • 2014
  • Ingår i: Ocean Science. - : Copernicus GmbH. - 1812-0784 .- 1812-0792. ; 10:4, s. 587-600
  • Tidskriftsartikel (refereegranskat)abstract
    • In order to advance understanding of the role of seawater surfactants in the air-sea exchange of climatically active trace gases via suppression of the gas transfer velocity (k(w)), we constructed a fully automated, closed air-water gas exchange tank and coupled analytical system. The system allows water-side turbulence in the tank to be precisely controlled with an electronically operated baffle. Two coupled gas chromatographs and an integral equilibrator, connected to the tank in a continuous gas-tight system, allow temporal changes in the partial pressures of SF6, CH4 and N2O to be measured simultaneously in the tank water and headspace at multiple turbulence settings, during a typical experimental run of 3.25 h. PC software developed by the authors controls all operations and data acquisition, enabling the optimisation of experimental conditions with high reproducibility. The use of three gases allows three independent estimates of k(w) for each turbulence setting; these values are subsequently normalised to a constant Schmidt number for direct comparison. The normalised k(w) estimates show close agreement. Repeated experiments with Milli-Q water demonstrate a typical measurement accuracy of 4% for k(w). Experiments with natural seawater show that the system clearly resolves the effects on k(w) of spatial and temporal trends in natural surfactant activity. The system is an effective tool with which to probe the relationships between k(w), surfactant activity and biogeochemical indices of primary productivity, and should assist in providing valuable new insights into the air-sea gas exchange process.
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34.
  • Sha, Bo, et al. (författare)
  • Constraining global transport of perfluoroalkyl acids on sea spray aerosol using field measurements
  • 2024
  • Ingår i: Science Advances. - : AMER ASSOC ADVANCEMENT SCIENCE. - 2375-2548. ; 10:14
  • Tidskriftsartikel (refereegranskat)abstract
    • Perfluoroalkyl acids (PFAAs) are highly persistent anthropogenic pollutants that have been detected in the global oceans. Our previous laboratory studies demonstrated that PFAAs in seawater are remobilized to the air in sea spray aerosols (SSAs). Here, we conducted field experiments along a north-south transect of the Atlantic Ocean to study the enrichment of PFAAs in SSA. We show that in some cases PFAAs were enriched >100,000 times in the SSA relative to seawater concentrations. On the basis of the results of the field experiments, we estimate that the secondary emission of certain PFAAs from the global oceans via SSA emission is comparable to or greater than estimates for the other known global sources of PFAAs to the atmosphere from manufacturing emissions and precursor degradation.
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35.
  • Sha, Bo, 1987-, et al. (författare)
  • Enrichment of Perfluoroalkyl Acids on Sea Spray Aerosol in Laboratory Experiments : The Role of Dissolved Organic Matter, Air Entrainment Rate and Inorganic Ion Composition
  • 2024
  • Ingår i: Environmental Science and Technology Letters. - 2328-8930.
  • Tidskriftsartikel (refereegranskat)abstract
    • The process by which perfluoroalkyl acids (PFAAs) become enriched on sea spray aerosol (SSA) is complex and likely influenced by several factors. In this study, we utilized a plunging water jet in a controlled laboratory setup to generate SSA. We investigated the enrichment process of PFAAs on nascent SSA by systematically varying three key parameters: 1) total organic carbon (TOC), 2) water jet flow rate, and 3) inorganic ion composition. The results showed a significant enhancement in enrichment when organic matter was introduced into artificial seawater. However, this enhancement did not exhibit a consistent trend when increasing the TOC from 1 to 2 mg L-1. The enrichment was increased at higher water jet flow rates (3.2 L min(-1)) compared to lower flow rates (1.6 and 2.4 L min(-1)), and the effect was particularly pronounced for submicrometer SSA particles. There was minimal difference in the enrichment of PFAAs when SSA was generated using sodium chloride solution instead of artificial seawater at the same salinity. Overall, these findings shed light on the complex process of PFAA enrichment on SSA and improved our understanding of the uncertainties associated with varying dissolved organic matter, water jet flow rate, and inorganic ion composition.
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36.
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37.
  • Sha, Bo, et al. (författare)
  • Influence of Water Concentrations of Perfluoroalkyl Acids (PFAAs) on Their Size-Resolved Enrichment in Nascent Sea Spray Aerosols
  • 2021
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 55:14, s. 9489-9497
  • Tidskriftsartikel (refereegranskat)abstract
    • Perfluoroalkyl acids (PFAAs) are persistent organic substances that have been widely detected in the global oceans. Previous laboratory experiments have demonstrated effective enrichment of PFAAs in nascent sea spray aerosols (SSA), suggesting that SSA are an important source of PFAAs to the atmosphere. In the present study, the effects of the water concentration of PFAAs on their size-resolved enrichment in SSA were examined using a sea spray simulation chamber. Aerosolization of the target compounds in almost all sizes of SSA revealed a strong linear relationship with their water concentrations (p < 0.05, r(2) > 0.9). The enrichment factors (EF) of the target compounds showed no correlation with their concentrations in the chamber water, despite the concentrations varying by a factor of 500 (similar to 0.3 to similar to 150 ng L-1). The particle surface-area-to-volume ratio appeared to be a key predictor of the enrichment of perfluoroalkyl carboxylic acids (PFCAs) with >= 7 perfluorinated carbons and perfluoroalkanesulfonic acids (PFSAs) with >= 6 perfluorinated carbons in supermicron particles (p < 0.05, r(2) > 0.8), but not in submicron particles. The different enrichment behaviors of PFAAs in submicron and supermicron particles might be a result of the different production mechanisms of film droplets and jet droplets. The results suggest that the variability in seawater concentrations of PFAAs has little influence on EFs and that modeling studies designed to quantify the source of PFAAs via SSA emissions do not need to consider this factor.
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38.
  • Sha, Bo, et al. (författare)
  • Sea Spray Aerosol (SSA) as a Source of Perfluoroalkyl Acids (PFAAs) to the Atmosphere : Field Evidence from Long-Term Air Monitoring
  • 2022
  • Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 56:1, s. 228-238
  • Tidskriftsartikel (refereegranskat)abstract
    • The effective enrichment of perfluoroalkyl acids (PFAAs) in sea spray aerosols (SSA) demonstrated in previous laboratory studies suggests that SSA is a potential source of PFAAs to the atmosphere. In order to investigate the influence of SSA on atmospheric PFAAs in the field, 48 h aerosol samples were collected regularly between 2018 and 2020 at two Norwegian coastal locations, Andoya and Birkenes. Significant correlations (p < 0.05) between the SSA tracer ion, Na+, and PFAA concentrations were observed in the samples from both locations, with Pearson's correlation coefficients (r) between 0.4-0.8. Such significant correlations indicate SSA to be an important source of atmospheric PFAAs to coastal areas. The correlations in the samples from Andoya were observed for more PFAA species and were generally stronger than in the samples from Birkenes, which is located further away from the coast and closer to urban areas than Andøya. Factors such as the origin of the SSA, the distance of the sampling site to open water, and the presence of other PFAA sources (e.g., volatile precursor compounds) can have influence on the contribution of SSA to PFAA in air at the sampling sites and therefore affect the observed correlations between PFAAs and Na+.
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39.
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40.
  • Sha, Bo, 1987- (författare)
  • Transport of perfluoroalkyl acids from the ocean to the atmosphere via sea spray aerosol
  • 2022
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • Perfluoroalkyl acids (PFAAs) are a subgroup of per- and polyfluoroalkyl substances (PFAS) that have been widely used in commercial and industrial applications. PFAAs are very persistent in the environment and some can bioaccumulate and have adverse health effects on human health. They have been detected ubiquitously in the abiotic environment, in biota and in humans. Long-range atmospheric transport (LRAT) is considered important for their global distribution. PFAAs are detected in the global oceans and they can be enriched in sea spray aerosol (SSA) due to their high surface activity. Thus, ocean-to-atmosphere transfer via sea spray aerosol emission is suggested to be one of the major sources of PFAAs to the atmosphere, yet the contribution of this source to PFAAs in air is not well-understood. The aim of this thesis is to improve the knowledge regarding the importance of SSA as a global source of PFAAs in the atmosphere. In Paper I, PFAA enrichment on SSA particles of different sizes was investigated via a series of laboratory experiments. A sea spray simulation chamber filled with sodium chloride solution (~35 g L-1) was used to generate SSA. The results showed that variation in PFAA water concentrations had little impact on the SSA enrichment factors (EFs). Furthermore, the results suggested that SSA production mechanisms result in different enrichment behaviors of individual PFAAs on <1 µm and >1µm SSA particles. Paper II provided clear field evidence that SSA can be an important source of PFAAs in the atmosphere. Significant positive correlations (p<0.05) were identified between the concentrations of PFAAs and SSA tracer ion (i.e. Na+) in aerosol samples collected at two Norwegian coastal sites during long-term air monitoring. Such correlations suggested that PFAAs transported via SSA can have a significant influence on their air concentrations in coastal areas. Aiming at bridging the gap between the lab and the field, in Paper III, a series of field experiments were conducted along a transect from ~50°N to ~50°S on the Atlantic Ocean. Changes in surface seawater temperature, salinity, conductivity and fluorescence during the field experiments revealed minor influences on EFs. However, the EFs derived from the field experiments were higher than the lab experiments in Paper I, which may be due to the different composition and properties of the chamber water in the two studies. It was concluded, however, that the variation of PFAA concentrations in the global oceans is the major contributor to the uncertainty in the estimation of PFAA ocean-to-air flux via SSA emission. Paper IV investigated mass-size distributions of PFAAs in aerosol samples collected near an industrial source and the associated LRAT potential of the PFAAs emitted. The results suggested that industrial sources can have regional influence on PFAA concentration in air. The information in Paper IV will help evaluate the relative importance of atmospheric sources of PFAAs at certain locations. This thesis contributes to a better understanding on the transport of PFAAs via SSA emission and on the sources of PFAAs to air in general.
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41.
  • Siegel, Karolina, et al. (författare)
  • Insights into the molecular composition of semi-volatile aerosols in the summertime central Arctic Ocean using FIGAERO-CIMS
  • 2021
  • Ingår i: Environmental Science. - 2634-3606. ; 1:4, s. 161-175
  • Tidskriftsartikel (refereegranskat)abstract
    • The remote central Arctic during summertime has a pristine atmosphere with very low aerosol particle concentrations. As the region becomes increasingly ice-free during summer, enhanced ocean-atmosphere fluxes of aerosol particles and precursor gases may therefore have impacts on the climate. However, large knowledge gaps remain regarding the sources and physicochemical properties of aerosols in this region. Here, we present insights into the molecular composition of semi-volatile aerosol components collected in September 2018 during the MOCCHA (Microbiology-Ocean-Cloud-Coupling in the High Arctic) campaign as part of the Arctic Ocean 2018 expedition with the Swedish Icebreaker Oden. Analysis was performed offline in the laboratory using an iodide High Resolution Time-of-Flight Chemical Ionization Mass Spectrometer with a Filter Inlet for Gases and AEROsols (FIGAERO-HRToF-CIMS). Our analysis revealed significant signal from organic and sulfur-containing compounds, indicative of marine aerosol sources, with a wide range of carbon numbers and O : C ratios. Several of the sulfur-containing compounds are oxidation products of dimethyl sulfide (DMS), a gas released by phytoplankton and ice algae. Comparison of the time series of particulate and gas-phase DMS oxidation products did not reveal a significant correlation, indicative of the different lifetimes of precursor and oxidation products in the different phases. This is the first time the FIGAERO-HRToF-CIMS was used to investigate the composition of aerosols in the central Arctic. The detailed information on the molecular composition of Arctic aerosols presented here can be used for the assessment of aerosol solubility and volatility, which is relevant for understanding aerosol-cloud interactions.
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42.
  • Stolle, Christian, et al. (författare)
  • The MILAN Campaign : Studying Diel Light Effects on the Air–Sea Interface
  • 2020
  • Ingår i: Bulletin of The American Meteorological Society - (BAMS). - 0003-0007 .- 1520-0477. ; 101:2, s. E146-E166
  • Tidskriftsartikel (refereegranskat)abstract
    • The sea surface microlayer (SML) at the air–sea interface is <1 mm thick, but it is physically, chemically, and biologically distinct from the underlying water and the atmosphere above. Wind-driven turbulence and solar radiation are important drivers of SML physical and biogeochemical properties. Given that the SML is involved in all air–sea exchanges of mass and energy, its response to solar radiation, especially in relation to how it regulates the air–sea exchange of climate-relevant gases and aerosols, is surprisingly poorly characterized. MILAN (Sea Surface Microlayer at Night) was an international, multidisciplinary campaign designed to specifically address this issue. In spring 2017, we deployed diverse sampling platforms (research vessels, radio-controlled catamaran, free-drifting buoy) to study full diel cycles in the coastal North Sea SML and in underlying water, and installed a land-based aerosol sampler. We also carried out concurrent ex situ experiments using several microsensors, a laboratory gas exchange tank, a solar simulator, and a sea spray simulation chamber. In this paper we outline the diversity of approaches employed and some initial results obtained during MILAN. Our observations of diel SML variability show, for example, an influence of (i) changing solar radiation on the quantity and quality of organic material and (ii) diel changes in wind intensity primarily forcing air–sea CO2 exchange. Thus, MILAN underlines the value and the need of multidiciplinary campaigns for integrating SML complexity into the context of air–sea interaction.
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43.
  • Triesch, Nadja, et al. (författare)
  • Sea Spray Aerosol Chamber Study on Selective Transfer and Enrichment of Free and Combined Amino Acids
  • 2021
  • Ingår i: ACS Earth and Space Chemistry. - : American Chemical Society (ACS). - 2472-3452. ; 5:6, s. 1564-1574
  • Tidskriftsartikel (refereegranskat)abstract
    • Free (FAAs) and combined amino acids (CAAs) were investigated on size-resolved samples of nascent sea spray aerosol (SSA) particles generated during controlled laboratory experiments. Compared to seawater, the amino acids were strongly enriched on the SSA particles. The enrichment factors (EFaer) on submicron SSA particles (EFaer Sigma(FAA): 2.5 x 10(6) and EFaer Sigma CAA: 7.9 x 10(5)) were 1-2 orders of magnitude higher than on supermicron ones (EFaerSFAA: 1.0 x 105 and EFaer Sigma(CAA): 7.3 x 10(4)) and continuously increased toward smaller SSA particles. Molecular-level analysis showed that the more polar the FAAs, the more they are enriched on the SSA particles (especially FAAs with polar acid side chains, e.g., aspartic acid: EFaer of 5.8 x 10(6)). Comparison of the amino acids present on nascent SSA with those present on ambient marine aerosol particles revealed a higher complexity of the amino acids of the nascent SSA, suggesting that atmospheric processes likely reduce the amino acid diversity. In addition, our results highlight that although almost all the amino acids studied are transferred to the atmosphere via bubble bursting under controlled conditions, two amino acids, gamma-aminobutyric acid (GABA) and glycine likely have additional sources to the atmosphere. GABA is likely formed on ambient marine submicron aerosol particles to a large extent (35-47% of Sigma FAA). Glycine likely originates from long-range transport processes or photochemical reactions, as discussed in the literature; however, our results highlight the potential for a direct oceanic source via bubble bursting (similar to 20% of Sigma FAA). Overall, bubble-bursting-derived total amino acids made up 11-18% of the mass of dissolved organic carbon on the submicron SSA particles.
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44.
  • Unger, Isaak, et al. (författare)
  • Influence of Organic Acids on the Surface Composition of Sea Spray Aerosol
  • 2020
  • Ingår i: Journal of Physical Chemistry A. - : American Chemical Society (ACS). - 1089-5639 .- 1520-5215. ; 124:2, s. 422-429
  • Tidskriftsartikel (refereegranskat)abstract
    • Recent studies on sea spray aerosol indicate an enrichment of Ca2+ in small particles, which are often thought to originate from the very surface of a water body when bubbles burst. One model to explain this observation is the formation of ion pairs between Ca2+(aq) and surface-active organic species. In this study, we have used X-ray photoelectron spectroscopy to probe aqueous salt solutions and artificial sea spray aerosol to study whether ion pairing in the liquid environment also affects the surface composition of dry aerosol. Carboxylic acids were added to the sample solutions to mimic some of the organic compounds present in natural seawater. Our results show that the formation of a core-shell structure governs the surface composition of the aerosol. The core-shell structure contrasts previous observations of the dry sea spray aerosol on substrates. As such, this may indicate that substrates can impact the morphology of the dried aerosol.
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45.
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46.
  • Upstill-Goddard, Robert C., et al. (författare)
  • The riverine source of CH4 and N2O from the Republic of Congo, western Congo Basin
  • 2017
  • Ingår i: Biogeosciences. - : Copernicus GmbH. - 1726-4170 .- 1726-4189. ; 14:9, s. 2267-2281
  • Tidskriftsartikel (refereegranskat)abstract
    • We discuss concentrations of dissolved CH4, N2O, O-2, NO(3)(-)and NH4-, and emission fluxes of CH4 and N2O for river sites in the western Congo Basin, Republic of Congo (ROC). Savannah, swamp forest and tropical forest samples were collected from the Congo main stem and seven of its tributaries during November 2010 (41 samples; wet season) and August 2011 (25 samples; dry season; CH4 and N2O only). Dissolved inorganic nitrogen (DIN: NH4- + NO3-; wet season) was dominated by NO3- (63 +/- 19% of DIN). Total DIN concentrations (1.545.3 mu mol L-1) were consistent with the near absence of agricultural, domestic and industrial sources for all three land types. Dissolved O-2 (wet season) was mostly undersaturated in swamp forest (36 +/- 29 %) and tropical forest (77 +/- 36 %) rivers but predominantly supersaturated in savannah rivers (100 +/- 17 %). The dissolved concentrations of CH4 and N2O were within the range of values reported earlier for sub-Saharan African rivers. Dissolved CH4 was found to be supersaturated (11.2-9553 nmol L-1; 440-354 444 %), whereas N2O ranged from strong undersaturation to supersaturation (3.2-20.6 nmol L-1; 47-205 %). Evidently, rivers of the ROC are persistent local sources of CH4 and can be minor sources or sinks for N2O. During the dry season the mean and range of CH4 and N2O concentrations were quite similar for the three land types. Wet and dry season mean concentrations and ranges were not significant for N2O for any land type or for CH4 in savannah rivers. The latter observation is consistent with seasonal buffering of river discharge by an underlying sandstone aquifer. Significantly higher wet season CH4 concentrations in swamp and forest rivers suggest that CH4 can be derived from floating macrophytes during flooding and/or enhanced methanogenesis in adjacent flooded soils. Swamp rivers also exhibited both low (47 %) and high (205 %) N2O saturation but wet season values were overall significantly lower than in either tropical forest or savannah rivers, which were always supersaturated (103-266 %) and for which the overall means and ranges of N2O were not significantly different. In swamp and forest rivers O-2 saturation co-varied inversely with CH4 saturation (log %) and positively with % N2O. A significant positive correlation between N2O and O-2 saturation in swamp rivers was coincident with strong N2O and O-2 undersaturation, indicating N2O consumption during denitrification in the sediments. In savannah rivers persistent N2O supersaturation and a negative correlation between N2O and O-2 suggest N2O production mainly by nitrification. This is consistent with a stronger correlation between N2O and NH4+ than between N2O and NO3-. Our ranges of values for CH4 and N2O emission fluxes (33-48 705 mu mol CH4 m(-2) d(-1); 1-67 mu mol N(2)Om(2)(-) d(-1)) are within the ranges previously estimated for sub-Saharan African rivers but they include uncertainties deriving from our use of basin-wide values for CH4 and N2O gas transfer velocities. Even so, because we did not account for any contribution from ebullition, which is quite likely for CH4 (at least 20 %), we consider our emission fluxes for CH4 to be conservative.
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47.
  • Wagner, Robert, et al. (författare)
  • Heterogeneous ice nucleation ability of aerosol particles generated from Arctic sea surface microlayer and surface seawater samples at cirrus temperatures
  • 2021
  • Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:18, s. 13903-13930
  • Tidskriftsartikel (refereegranskat)abstract
    • Sea spray aerosol particles are a recognised type of ice-nucleating particles under mixed-phase cloud conditions. Entities that are responsible for the heterogeneous ice nucleation ability include intact or fragmented cells of marine microorganisms as well as organic matter released by cell exudation. Only a small fraction of sea spray aerosol is transported to the upper troposphere, but there are indications from mass-spectrometric analyses of the residuals of sublimated cirrus particles that sea salt could also contribute to heterogeneous ice nucleation under cirrus conditions. Experimental studies on the heterogeneous ice nucleation ability of sea spray aerosol particles and their proxies at temperatures below 235K are still scarce. In our article, we summarise previous measurements and present a new set of ice nucleation experiments at cirrus temperatures with particles generated from sea surface microlayer and surface seawater samples collected in three different regions of the Arctic and from a laboratory-grown diatom culture (Skeletonema marinoi). The particles were suspended in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) cloud chamber and ice formation was induced by expansion cooling. We confirmed that under cirrus conditions, apart from the ice-nucleating entities mentioned above, also crystalline inorganic salt constituents can contribute to heterogeneous ice formation. This takes place at temperatures below 220 K, where we observed in all experiments a strong immersion freezing mode due to the only partially deliquesced inorganic salts. The inferred ice nucleation active surface site densities for this nucleation mode reached a maximum of about 5 x 10(10) m(-2) at an ice saturation ratio of 1.3. Much smaller densities in the range of 10(8)-10(9) m(-2) were observed at temperatures between 220 and 235 K, where the inorganic salts fully deliquesced and only the organic matter and/or algal cells and cell debris could contribute to heterogeneous ice formation. These values are 2 orders of magnitude smaller than those previously reported for particles generated from microlayer suspensions collected in temperate and subtropical zones. While this difference might simply underline the strong variability of the number of ice-nucleating entities in the sea surface microlayer across different geographical regions, we also discuss how instrumental parameters like the aerosolisation method and the ice nucleation measurement technique might affect the comparability of the results amongst different studies.
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48.
  • Zabori, Julia, et al. (författare)
  • Comparison between summertime and wintertime Arctic Ocean primary marine aerosol properties
  • 2013
  • Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 13:9, s. 4783-4799
  • Tidskriftsartikel (refereegranskat)abstract
    • Primary marine aerosols (PMAs) are an important source of cloud condensation nuclei, and one of the key elements of the remote marine radiative budget. Changes occurring in the rapidly warming Arctic, most importantly the decreasing sea ice extent, will alter PMA production and hence the Arctic climate through a set of feedback processes. In light of this, laboratory experiments with Arctic Ocean water during both Arctic winter and summer were conducted and focused on PMA emissions as a function of season and water properties. Total particle number concentrations and particle number size distributions were used to characterize the PMA population. A comprehensive data set from the Arctic summer and winter showed a decrease in PMA concentrations for the covered water temperature (T-w) range between - 1 degrees C and 15 degrees C. A sharp decrease in PMA emissions for a T-w increase from -1 degrees C to 4 degrees C was followed by a lower rate of change in PMA emissions for T-w up to about 6 degrees C. Near constant number concentrations for water temperatures between 6 degrees C to 10 degrees C and higher were recorded. Even though the total particle number concentration changes for overlapping T-w ranges were consistent between the summer and winter measurements, the distribution of particle number concentrations among the different sizes varied between the seasons. Median particle number concentrations for a dry diameter (D-p) < 0.125 mu m measured during winter conditions were similar (deviation of up to 3 %), or lower (up to 70 %) than the ones measured during summer conditions (for the same water temperature range). For D-p > 0.125 mu m, the particle number concentrations during winter were mostly higher than in summer (up to 50 %). The normalized particle number size distribution as a function of water temperature was examined for both winter and summer measurements. An increase in T-w from -1 degrees C to 10 degrees C during winter measurements showed a decrease in the peak of relative particle number concentration at about a D-p of 0.180 mu m, while an increase was observed for particles with D-p > 1 mu m. Summer measurements exhibited a relative shift to smaller particle sizes for an increase of T-w in the range 7-11 degrees C. The differences in the shape of the number size distributions between winter and summer may be caused by different production of organic material in water, different local processes modifying the water masses within the fjord (for example sea ice production in winter and increased glacial meltwater inflow during summer) and different origin of the dominant sea water mass. Further research is needed regarding the contribution of these factors to the PMA production.
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49.
  • Zieger, Paul, et al. (författare)
  • Revising the hygroscopicity of inorganic sea salt particles
  • 2017
  • Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 8
  • Tidskriftsartikel (refereegranskat)abstract
    • Sea spray is one of the largest natural aerosol sources and plays an important role in the Earth's radiative budget. These particles are inherently hygroscopic, that is, they take-up moisture from the air, which affects the extent to which they interact with solar radiation. We demonstrate that the hygroscopic growth of inorganic sea salt is 8-15% lower than pure sodium chloride, most likely due to the presence of hydrates. We observe an increase in hygroscopic growth with decreasing particle size (for particle diameters <150 nm) that is independent of the particle generation method. We vary the hygroscopic growth of the inorganic sea salt within a general circulation model and show that a reduced hygroscopicity leads to a reduction in aerosol-radiation interactions, manifested by a latitudinal-dependent reduction of the aerosol optical depth by up to 15%, while cloud-related parameters are unaffected. We propose that a value of kappa(s) = 1.1 (at RH = 90%) is used to represent the hygroscopicity of inorganic sea salt particles in numerical models.
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50.
  • Zinke, Julika, 1995- (författare)
  • Factors influencing emission fluxes and bacterial enrichment in sea spray aerosols : Insights from laboratory and field studies
  • 2023
  • Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
    • Sea spray aerosol (SSA) is one of the major natural aerosol sources and is produced when wave breaking entrains air into ocean surface water, which subsequently breaks up into bubbles. These bubbles rise to the surface and can scavenge biogenic material. Once they reach the surface, they burst and produce both a large number of relatively small film drops that result from the disintegration of the bubble film cap and a smaller number of jet drops that result from the collapse of the bubble cavity and are typically larger in size than the film drops. The production of SSA is influenced by several factors, including wind speed, sea state, seawater temperature, salinity, and the physicochemical and biological condition of the ocean. SSA can significantly impact Earth's radiation budget by scattering incoming solar radiation directly and by acting as cloud condensation nuclei. To improve our understanding of the impact of sea spray aerosols on the Earth’s climate, it is critical to understand the physical mechanisms which determine the size-resolved SSA production flux. Furthermore, SSA can be a vector for the emission of primary biological airborne particles (PBAP) from the oceans to the atmosphere. PBAP encompass bacteria, viruses, pollen and spores and can be present in the atmosphere in form of agglomerates, single particles or cell fractions.  Although, the abundance of PBAP typically only make up < 0.1% of the number of aerosols, this does not imply their insignificance. On the contrary, PBAP are known to be very efficient cloud- and ice condensation nuclei and thus can influence cloud properties such as cloud phase, albedo and lifetime, thereby affecting the Earth’s climate as well as biogeochemical cycles. As the Earth is 70% covered by oceans, of which most could be characterized as remote, quantifying the PBAP emissions over these waters are important for the enhancement of climate models.The goal of this thesis was to study the factors impacting SSA emissions and the emission of primary biological particles with SSA with particular focus on bacteria emissions. This was done both through laboratory and field experiments in the Baltic Sea and in the Azores archipelago using a plunging jet sea spray simulation chamber and various techniques to characterize aerosol emissions. More specifically, a parameterization for the SSA production flux as a function of salinity and temperature was derived from laboratory experiments and a wind speed and sea state dependent parameterization were derived from ambient eddy covariance (EC) flux measurements in the Baltic Sea. The combination of EC flux measurements and laboratory generated SSA allowed to derive a chamber specific scaling factor that could be applied to derive bacteria emission fluxes ranging between 16-63 cells m−2 s−1 from the Baltic Sea. Bacteria were found to be 13-488 and 9-148 times enriched in SSA compared to the underlying seawater from mesocosm experiments in the Baltic Sea and Azores, respectively. A comparison of single cell abundance estimates from fluorescence microscopy and real-time measurements of PBAP with diameters > 0.8 µm using a bioaerosol sensor revealed that the latter yielded consistently lower concentrations. The discrepancy was explained by differences in the sampling approach and size cut-offs (i.e. single cells versus agglomerates or particle-attached cells). As such, both methods are applicable to different research questions and should be considered complementary.An analysis of the microbial community composition in the aerosols and underlying seawater showed selective aerosolization of certain bacteria taxa. Furthermore, selective growth and a decrease in alpha diversity in the seawater was observed when the mesocosm experiments were operated in a closed mode (meaning that the seawater was not exchanged over the duration of each experiment), which can however be circumvented by continuously replacing the water in the mesocosm.Ambient measurements of PBAP revealed diurnal variations with a peak during the early morning hours that was correlated to changes wind speed, wave height, air temperature, relative humidity, latent and sensitive heat flux.
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