| 1. |
|
|
| 2. |
- Alsved, Malin, et al.
(författare)
-
Effect of Aerosolization and Drying on the Viability of Pseudomonas syringae Cells
- 2018
-
Ingår i: Frontiers in Microbiology. - : Frontiers Media SA. - 1664-302X. ; 9
-
Tidskriftsartikel (refereegranskat)abstract
- Airborne dispersal of microorganisms influences their biogeography, gene flow, atmospheric processes, human health and transmission of pathogens that affect humans, plants and animals. The extent of their impact depends essentially on cell-survival rates during the process of aerosolization. A central factor for cell-survival is water availability prior to and upon aerosolization. Also, the ability of cells to successfully cope with stress induced by drying determines their chances of survival. In this study, we used the ice-nucleation active, plant pathogenic Pseudomonas syringae strain R10.79 as a model organism to investigate the effect of drying on cell survival. Two forms of drying were simulated: drying of cells in small droplets aerosolized from a wet environment by bubble bursting and drying of cells in large droplets deposited on a surface. For drying of cells both in aerosol and surface droplets, the relative humidity (RH) was varied in the range between 10 and 90%. The fraction of surviving cells was determined by live/dead staining followed by flow cytometry. We also evaluated the effect of salt concentration in the water droplets on the survival of drying cells by varying the ionic strength between 0 and 700 mM using NaCl and sea salt. For both aerosol and surface drying, cell survival increased with decreasing RH (p < 0.01), and for surface drying, survival was correlated with increasing salt concentration (p < 0.001). Imaging cells with TEM showed shrunk cytoplasm and cell wall damage for a large fraction of aerosolized cells. Ultimately, we observed a 10-fold higher fraction of surviving cells when dried as aerosol compared to when dried on a surface. We conclude that the conditions, under which cells dry, significantly affect their survival and thus their success to spread through the atmosphere and colonize new environments as well as their ability to affect atmospheric processes.
|
|
| 3. |
- 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.
|
|
| 4. |
|
|
| 5. |
- 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.
|
|
| 6. |
- 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.
|
|
| 7. |
- 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.
|
|
| 8. |
- Rosati, Bernadette, et al.
(författare)
-
Hygroscopicity and CCN potential of DMS-derived aerosol particles
- 2022
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:20, s. 13449-13466
-
Tidskriftsartikel (refereegranskat)abstract
- Dimethyl sulfide (DMS) is emitted by phytoplankton species in the oceans and constitutes the largest source of naturally emitted sulfur to the atmosphere. The climate impact of secondary particles, formed through the oxidation of DMS by hydroxyl radicals, is still elusive. This study investigates the hygroscopicity and cloud condensation nuclei activity of such particles and discusses the results in relation to their chemical composition. We show that mean hygroscopicity parameters, κ, during an experiment for particles of 80 nm in diameter range from 0.46 to 0.52 or higher, as measured at both sub- and supersaturated water vapour conditions. Ageing of the particles leads to an increase in κ from, for example, 0.50 to 0.58 over the course of 3 h (Exp. 7). Aerosol mass spectrometer measurements from this study indicate that this change most probably stems from a change in chemical composition leading to slightly higher fractions of ammonium sulfate compared to methanesulfonic acid (MSA) within the particles with ageing time. Lowering the temperature to 258 K increases κ slightly, particularly for small particles. These κ values are well comparable to previously reported model values for MSA or mixtures between MSA and ammonium sulfate. Particle nucleation and growth rates suggest a clear temperature dependence, with slower rates at cold temperatures. Quantum chemical calculations show that gas-phase MSA clusters are predominantly not hydrated, even at high humidity conditions, indicating that their gas-phase chemistry should be independent of relative humidity.
|
|
| 9. |
- Rosati, Bernadette, et al.
(författare)
-
New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals
- 2021
-
Ingår i: ACS Earth and Space Chemistry. - : American Chemical Society (ACS). - 2472-3452. ; 5:4, s. 801-811
-
Tidskriftsartikel (refereegranskat)abstract
- Dimethyl sulfide (DMS) is produced by plankton in oceans and constitutes the largest natural emission of sulfur to the atmosphere. In this work, we examine new particle formation from the primary pathway of oxidation of gas-phase DMS by OH radicals. We particularly focus on particle growth and mass yield as studied experimentally under dry conditions using the atmospheric simulation chamber AURA. Experimentally, we show that aerosol mass yields from oxidation of 50-200 ppb of DMS are low (2-7%) and that particle growth rates (8.2-24.4 nm/h) are comparable with ambient observations. An HR-ToF-AMS was calibrated using methanesulfonic acid (MSA) to account for fragments distributed across both the organic and sulfate fragmentation table. AMS-derived chemical compositions revealed that MSA was always more dominant than sulfate in the secondary aerosols formed. Modeling using the Aerosol Dynamics, gas- and particle-phase chemistry kinetic multilayer model for laboratory CHAMber studies (ADCHAM) indicates that the Master Chemical Mechanism gas-phase chemistry alone underestimates experimentally observed particle formation and that DMS multiphase and autoxidation chemistry is needed to explain observations. Based on quantum chemical calculations, we conclude that particle formation from DMS oxidation in the ambient atmosphere will most likely be driven by mixed sulfuric acid/MSA clusters clustering with both amines and ammonia.
|
|
| 10. |
- Rosati, Bernadette, et al.
(författare)
-
The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol
- 2021
-
Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 11:1
-
Tidskriftsartikel (refereegranskat)abstract
- Sea spray aerosol (SSA) contributes significantly to natural aerosol particle concentrations globally, in marine areas even dominantly. The potential changes of the omnipresent inorganic fraction of SSA due to atmospheric ageing is largely unexplored. In the atmosphere, SSA may exist as aqueous phase solution droplets or as dried solid or amorphous particles. We demonstrate that ageing of liquid NaCl and artificial sea salt aerosol by exposure to ozone and UV light leads to a substantial decrease in hygroscopicity and cloud activation potential of the dried particles of the same size. The results point towards surface reactions on the liquid aerosols that are more crucial for small particles and the formation of salt structures with water bound within the dried aerosols, termed hydrates. Our findings suggest an increased formation of hydrate forming salts during ageing and the presence of hydrates in dried SSA. Field observations indicate a reduced hygroscopic growth factor of sub-micrometre SSA in the marine atmosphere compared to fresh laboratory generated NaCl or sea salt of the same dry size, which is typically attributed to organic matter or sulphates. Aged inorganic sea salt offers an additional explanation for such a measured reduced hygroscopic growth factor and cloud activation potential.
|
|
| 11. |
- Wollesen De Jonge, Robin, et al.
(författare)
-
Secondary aerosol formation from dimethyl sulfide-improved mechanistic understanding based on smog chamber experiments and modelling
- 2021
-
Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:13, s. 9955-9976
-
Tidskriftsartikel (refereegranskat)abstract
- Dimethyl sulfide (DMS) is the dominant biogenic sulfur compound in the ambient marine atmosphere. Low-volatility acids from DMS oxidation promote the formation and growth of sulfur aerosols and ultimately alter cloud properties and Earth's climate. We studied the OH-initiated oxidation of DMS in the Aarhus University Research on Aerosol (AURA) smog chamber and the marine boundary layer (MBL) with the aerosol dynamics and gas-and particle-phase chemistry kinetic multilayer model ADCHAM. Our work involved the development of a revised and comprehensive multiphase DMS oxidation mechanism, capable of both reproducing smog chamber and atmospheric relevant conditions. The secondary aerosol mass yield in the AURA chamber was found to have a strong dependence on the reaction of methyl sulfinic acid (MSIA) and OH, causing a 82.8% increase in the total PM at low relative humidity (RH), while the autoxidation of the intermediate radical CH3SCH2OO forming hydroperoxymethyl thioformate (HPMTF) proved important at high temperature and RH, decreasing the total PM by 55.8%. The observations and modelling strongly support the finding that a liquid water film existed on the Teflon surface of the chamber bag, which enhanced the wall loss of water-soluble intermediates and oxidants dimethyl sulfoxide (DMSO), MSIA, HPMTF, SO2, methanesulfonic acid (MSA), sulfuric acid (SA) and H2O2. The effect caused a 64.8% and 91.7% decrease in the secondary aerosol mass yield obtained at both dry (0%RH-12%RH) and humid (50%RH-80%RH) conditions, respectively. Model runs reproducing the ambient marine atmosphere indicate that OH comprises a strong sink of DMS in the MBL (accounting for 31.1% of the total sink flux of DMS) although less important than the combined effect of halogen species Cl and BrO (accounting for 24.3% and 38.7%, respectively). Cloudy conditions promote the production of SO42-particular mass (PM) from SO2 accumulated in the gas phase, while cloud-free periods facilitate MSA formation in the deliquesced particles. The exclusion of aqueous-phase chemistry lowers the DMS sink as no halogens are activated in the sea spray particles and underestimates the secondary aerosol mass yield by neglecting SO42-and MSA PM production in the particle phase. Overall, this study demonstrated that the current DMS oxidation mechanisms reported in literature are inadequate in reproducing the results obtained in the AURA chamber, whereas the revised chemistry captured the formation, growth and chemical composition of the formed aerosol particles well. Furthermore, we emphasize the importance of OH-initiated oxidation of DMS in the ambient marine atmosphere during conditions with low sea spray emissions.
|
|
