| 1. |
- Alsved, Malin, et al.
(författare)
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Effect of Aerosolization and Drying on the Viability of Pseudomonas syringae Cells
- 2018
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Ingår i: Frontiers in Microbiology. - : Frontiers Media SA. - 1664-302X. ; 9
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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.
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| 2. |
- Andersen, Christina, et al.
(författare)
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Emissions of soot, PAHs, ultrafine particles, NOx, and other health relevant compounds from stressed burning of candles in indoor air
- 2021
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Ingår i: Indoor Air. - : Hindawi Limited. - 0905-6947 .- 1600-0668. ; 31:6, s. 2033-2048
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Tidskriftsartikel (refereegranskat)abstract
- Burning candles release a variety of pollutants to indoor air, some of which are of concern for human health. We studied emissions of particles and gases from the stressed burning of five types of pillar candles with different wax and wick compositions. The stressed burning was introduced by controlled fluctuating air velocities in a 21.6 m3 laboratory chamber. The aerosol physicochemical properties were measured both in well-mixed chamber air and directly above the candle flame with online and offline techniques. All candles showed different emission profiles over time with high repeatability among replicates. The particle mass emissions from stressed burning for all candle types were dominated by soot (black carbon; BC). The wax and wick composition strongly influenced emissions of BC, PM2.5 , and particle-phase polycyclic aromatic hydrocarbons (PAHs), and to lower degree ultrafine particles, inorganic and organic carbon fraction of PM, but did not influence NOx , formaldehyde, and gas-phase PAHs. Measurements directly above the flame showed empirical evidence of short-lived strong emission peaks of soot particles. The results show the importance of including the entire burn time of candles in exposure assessments, as their emissions can vary strongly over time. Preventing stressed burning of candles can reduce exposure to pollutants in indoor air.
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| 3. |
- Christiansen, Sigurd, et al.
(författare)
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Influence of Arctic Microlayers and Algal Cultures on Sea Spray Hygroscopicity and the Possible Implications for Mixed-Phase Clouds
- 2020
-
Ingår i: Journal of Geophysical Research: Atmospheres. - 2169-8996 .- 2169-897X. ; 125:19
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Tidskriftsartikel (refereegranskat)abstract
- As Arctic sea ice cover diminishes, sea spray aerosols (SSA) have a larger potential to be emitted into the Arctic atmosphere. Emitted SSA can contain organic material, but how it affects the ability of particles to act as cloud condensation nuclei (CCN) is still not well understood. Here we measure the CCN-derived hygroscopicity of three different types of aerosol particles: (1) Sea salt aerosols made from artificial seawater, (2) aerosol generated from artificial seawater spiked with diatom species cultured in the laboratory, and (3) aerosols made from samples of sea surface microlayer (SML) collected during field campaigns in the North Atlantic and Arctic Ocean. Samples are aerosolized using a sea spray simulation tank (plunging jet) or an atomizer. We show that SSA containing diatom and microlayer exhibit similar CCN activity to inorganic sea salt with a κ value of ∼1.0. Large-eddy simulation (LES) is then used to evaluate the general role of aerosol hygroscopicity in governing mixed-phase low-level cloud properties in the high Arctic. For accumulation mode aerosol, the simulated mixed-phase cloud properties do not depend strongly on κ, unless the values are lower than 0.4. For Aitken mode aerosol, the hygroscopicity is more important; the particles can sustain the cloud if the hygroscopicity is equal to or higher than 0.4, but not otherwise. The experimental and model results combined suggest that the internal mixing of biogenic organic components in SSA does not have a substantial impact on the cloud droplet activation process and the cloud lifetime in Arctic mixed-phase clouds.
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| 4. |
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| 5. |
- Christiansen, Sigurd, et al.
(författare)
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Sea Spray Aerosol Formation : Laboratory Results on the Role of Air Entrainment, Water Temperature, and Phytoplankton Biomass
- 2019
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 53:22, s. 13107-13116
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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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| 6. |
- Crljenica, Ivica, et al.
(författare)
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Determining the saturation vapour pressures of keto-dicarboxylic acids in aqueous solutions
- 2013
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Ingår i: NUCLEATION AND ATMOSPHERIC AEROSOLS. - : American Institute of Physics (AIP). - 9780735411524 ; , s. 468-471
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Konferensbidrag (refereegranskat)abstract
- A two-compartment binary mass transport model with group contribution methods parametrizations for the physical properties of the organic acids (UNIFAC Dortmund method for activity coefficients, GCVOL-OL-60 method for the pure liquid acid density, GC-MG method for the pure acid surface tension at room temperature, Fuller et al. method for the diffusion coefficients) was used to interpret the evaporation experiments of 100 nm sized keto-dicarboxylic acid aqueous solutions droplets at ambient temperature. The determined values for the saturation vapour pressure of liquid 2-keto-glutaric acid are in the order of 10(-5) Pa.
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| 7. |
- Elm, Jonas, et al.
(författare)
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Computational study of the Rayleigh light scattering properties of atmospheric pre-nucleation clusters
- 2014
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Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 16:22, s. 10883-10890
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Tidskriftsartikel (refereegranskat)abstract
- The Rayleigh and hyper Rayleigh scattering properties of the binary (H2SO4)(H2O)(n) and ternary (H2SO4)(NH3)(H2O) n clusters are investigated using a quantum mechanical response theory approach. The molecular Rayleigh scattering intensities are expressed using the dipole polarizability alpha and hyperpolarizability beta tensors. Using density functional theory, we elucidate the effect of cluster morphology on the scattering properties using a combinatorial sampling approach. We find that the Rayleigh scattering intensity depends quadratically on the number of water molecules in the cluster and that a single ammonia molecule is able to induce a high anisotropy, which further increases the scattering intensity. The hyper Rayleigh scattering activities are found to be extremely low. This study presents the first attempt to map the scattering of atmospheric molecular clusters using a bottom-up approach.
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| 8. |
- Ickes, Luisa, 1986, et al.
(författare)
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The ice-nucleating activity of Arctic sea surface microlayer samples and marine algal cultures
- 2020
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 20:18, s. 11089-11117
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Tidskriftsartikel (refereegranskat)abstract
- In recent years, sea spray as well as the biological material it contains has received increased attention as a source of ice-nucleating particles (INPs). Such INPs may play a role in remote marine regions, where other sources of INPs are scarce or absent. In the Arctic, these INPs can influence water-ice partitioning in low-level clouds and thereby the cloud lifetime, with consequences for the surface energy budget, sea ice formation and melt, and climate. Marine aerosol is of a diverse nature, so identifying sources of INPs is challenging. One fraction of marine bioaerosol (phytoplankton and their exudates) has been a particular focus of marine INP research. In our study we attempt to address three main questions. Firstly, we compare the ice-nucleating ability of two common phytoplankton species with Arctic seawater microlayer samples using the same instrumentation to see if these phytoplankton species produce ice-nucleating material with sufficient activity to account for the ice nucleation observed in Arctic microlayer samples. We present the first measurements of the ice-nucleating ability of two predominant phytoplankton species: Melosira arctica, a common Arctic diatom species, and Skeletonema marinoi, a ubiquitous diatom species across oceans worldwide. To determine the potential effect of nutrient conditions and characteristics of the algal culture, such as the amount of organic carbon associated with algal cells, on the ice nucleation activity, Skeletonema marinoi was grown under different nutrient regimes. From comparison of the ice nucleation data of the algal cultures to those obtained from a range of sea surface microlayer (SML) samples obtained during three different field expeditions to the Arctic (ACCACIA, NETCARE, and ASCOS), we found that they were not as ice active as the investigated microlayer samples, although these diatoms do produce ice-nucleating material. Secondly, to improve our understanding of local Arctic marine sources as atmospheric INPs we applied two aerosolization techniques to analyse the ice-nucleating ability of aerosolized microlayer and algal samples. The aerosols were generated either by direct nebulization of the undiluted bulk solutions or by the addition of the samples to a sea spray simulation chamber filled with artificial seawater. The latter method generates aerosol particles using a plunging jet to mimic the process of oceanic wave breaking. We observed that the aerosols produced using this approach can be ice active, indicating that the ice-nucleating material in seawater can indeed transfer to the aerosol phase. Thirdly, we attempted to measure ice nucleation activity across the entire temperature range relevant for mixed-phase clouds using a suite of ice nucleation measurement techniques - an expansion cloud chamber, a continuous-flow diffusion chamber, and a cold stage. In order to compare the measurements made using the different instruments, we have normalized the data in relation to the mass of salt present in the nascent sea spray aerosol. At temperatures above 248K some of the SML samples were very effective at nucleating ice, but there was substantial variability between the different samples. In contrast, there was much less variability between samples below 248 K. We discuss our results in the context of aerosol-cloud interactions in the Arctic with a focus on furthering our understanding of which INP types may be important in the Arctic atmosphere.
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| 9. |
- King, Stephanie M., et al.
(författare)
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Investigating Primary Marine Aerosol Properties : CCN Activity of Sea Salt and Mixed Inorganic-Organic Particles
- 2012
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 46:19, s. 10405-10412
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Tidskriftsartikel (refereegranskat)abstract
- Sea spray particles ejected as a result of bubbles bursting from artificial seawater containing salt and organic matter in a stainless steel tank were sampled for size distribution, morphology, and cloud condensation nucleus (CCN) activity. Bubbles were generated either by aeration through a diffuser or by water jet impingement on the seawater surface. Three objectives were addressed in this study. First, CCN activities of NaCl and two types of artificial sea salt containing only inorganic components were measured to establish a baseline for further measurements of mixed organic inorganic particles. Second, the effect of varying bubble residence time in the bulk seawater solution on particle size and CCN activity was investigated and was found to be insignificant for the organic compounds studied. Finally, CCN activities of particles produced from jet impingement were compared with those produced from diffuser aeration. Analyses indicate a considerable amount of organic enrichment in the jet-produced particles relative to the bulk seawater composition when sodium laurate, an organic surfactant, is present in the seawater. In this case, the production of a thick foam layer during impingement may explain the difference in activation and supports hypotheses that particle production from the two methods of generating bubbles is not equal.
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| 10. |
- Krieger, Ulrich K., et al.
(författare)
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A reference data set for validating vapor pressure measurement techniques : homologous series of polyethylene glycols
- 2018
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Ingår i: Atmospheric Measurement Techniques. - : Copernicus GmbH. - 1867-1381 .- 1867-8548. ; 11:1, s. 49-63
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Tidskriftsartikel (refereegranskat)abstract
- To predict atmospheric partitioning of organic compounds between gas and aerosol particle phase based on explicit models for gas phase chemistry, saturation vapor pressures of the compounds need to be estimated. Estimation methods based on functional group contributions require training sets of compounds with well-established saturation vapor pressures. However, vapor pressures of semivolatile and low-volatility organic molecules at atmospheric temperatures reported in the literature often differ by several orders of magnitude between measurement techniques. These discrepancies exceed the stated uncertainty of each technique which is generally reported to be smaller than a factor of 2. At present, there is no general reference technique for measuring saturation vapor pressures of atmospherically relevant compounds with low vapor pressures at atmospheric temperatures. To address this problem, we measured vapor pressures with different techniques over a wide temperature range for intercomparison and to establish a reliable training set. We determined saturation vapor pressures for the homologous series of polyethylene glycols (H-(O-CH2-CH2)(n)-OH) for n = 3 to n = 8 ranging in vapor pressure at 298 K from 10(-7) to 5 x 10(-2) Pa and compare them with quantum chemistry calculations. Such a homologous series provides a reference set that covers several orders of magnitude in saturation vapor pressure, allowing a critical assessment of the lower limits of detection of vapor pressures for the different techniques as well as permitting the identification of potential sources of systematic error. Also, internal consistency within the series allows outlying data to be rejected more easily. Most of the measured vapor pressures agreed within the stated uncertainty range. Deviations mostly occurred for vapor pressure values approaching the lower detection limit of a technique. The good agreement between the measurement techniques (some of which are sensitive to the mass accommodation coefficient and some not) suggests that the mass accommodation coefficients of the studied compounds are close to unity. The quantum chemistry calculations were about 1 order of magnitude higher than the measurements. We find that extrapolation of vapor pressures from elevated to atmospheric temperatures is permissible over a range of about 100 K for these compounds, suggesting that measurements should be performed best at temperatures yielding the highest-accuracy data, allowing subsequent extrapolation to atmospheric temperatures.
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| 11. |
- Kristensen, Kasper, et al.
(författare)
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High-Molecular Weight Dimer Esters Are Major Products in Aerosols from α-Pinene Ozonolysis and the Boreal Forest
- 2016
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 3:8, s. 280-285
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Tidskriftsartikel (refereegranskat)abstract
- This study investigates the contribution of high-molecular weight dimer esters to laboratory-generated α-pinene gas- and particle-phase secondary organic aerosol (SOA) and particulate matter (PM) collected at the Nordic boreal forest site of Hyytiälä, Finland. Laboratory flow reactor experiments (25 °C) show that dimer esters from ozonolysis of α-pinene contribute between 5 and 16% of the freshly formed α-pinene particle-phase SOA mass. An increased level of formation is observed at a higher relative humidity of ∼40%, and the presence of a hydroxyl radical (OH) scavenger is shown to affect the formation of dimer esters. Of the 28 dimer esters identified in laboratory α-pinene SOA, 15 are also observed in ambient PM samples, contributing between 0.5 and 1.6% of the total PM1. The observed esters show good correlation with known α-pinene SOA tracers in collected PM samples. This work reveals an, until now, unrecognized contribution of dimer esters from α-pinene oxidation to boreal forest PM.
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| 12. |
- Kristensson, Adam, et al.
(författare)
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Cloud Droplet Activation of Amino Acid Aerosol Particles.
- 2010
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Ingår i: Journal of physical chemistry. A. - : American Chemical Society (ACS). - 1520-5215 .- 1089-5639. ; 114:1, s. 379-386
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Tidskriftsartikel (refereegranskat)abstract
- In this work we investigated the ability of a series of amino acids to act as cloud condensation nuclei using a static thermal gradient diffusion type cloud condensation nucleus counter. Particles of pure dry l-glycine, glycyl-glycine, l-serine, l-methionine, l-glutamic acid, l-aspartic acid, and l-tyrosine were studied as well as internally mixed dry particles containing ammonium sulfate and one or two of the following amino acids: l-methionine, l-aspartic acid, or l-tyrosine. The amino acids ranged in water solubility from high (>100 g/L), intermediate (10-100 g/L), low (3-10 g/L), to very low (<3 g/L). With the exception of l-methionine and l-tyrosine, all the studied pure amino acid particles activated as though they were fully soluble, although Kohler theory modified to account for limited solubility suggests that the activation of the intermediate and low solubility amino acids l-serine, l-glutamic acid, and l-aspartic acid should be limited by solubility. Activation of mixed particles containing at least 60% dry mass of l-tyrosine was limited by solubility, but the activation of the other investigated mixed particles behaved as if fully soluble. In general, the results show that particles containing amino acids at atmospherically relevant mixture ratios are good cloud condensation nuclei.
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| 13. |
- Kulmala, Markku, et al.
(författare)
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Overview of the biosphere-aerosol-cloud-climate interactions (BACCI) studies
- 2008
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Ingår i: Tellus. Series B: Chemical and Physical Meteorology. - : Stockholm University Press. - 0280-6509 .- 1600-0889. ; 60:3, s. 300-317
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Forskningsöversikt (refereegranskat)abstract
- Here we present research methods and results obtained by the Nordic Centre of Excellence Biosphere-Aerosol-Cloud-Climate Interactions (BACCI) between 1 January 2003 and 31 December 2007. The centre formed an integrated attempt to understand multiple, but interlinked, biosphere-atmosphere interactions applying inter and multidisciplinary approaches in a coherent manner. The main objective was to study the life cycle of aerosol particles and their importance on climate change. The foundation in BACCI was a thorough understanding of physical, meteorological, chemical and ecophysiological processes, providing a unique possibility to study biosphere-aerosol-cloud-climate interactions. Continuous measurements of atmospheric concentrations and fluxes of aerosol particles and precursors and, CO2/aerosol trace gas interactions in different field stations (e.g. SMEAR) were supported by models of particle thermodynamics, transport and dynamics, atmospheric chemistry, boundary layer meteorology and forest growth. The main progress was related to atmospheric new particle formation, existence of clusters, composition of nucleation mode aerosol particles, chemical precursors of fresh aerosol particles, the contribution of biogenic aerosol particles on the global aerosol load, transport, transformation and deposition of aerosol particles, thermodynamics related to aerosol particles and cloud droplets, and the microphysics and chemistry of cloud droplet formation.
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| 14. |
- Li, Linjie, et al.
(författare)
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Gas-to-Particle Partitioning of Products from Ozonolysis of Δ3-Carene and the Effect of Temperature and Relative Humidity
- 2024
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Ingår i: JOURNAL OF PHYSICAL CHEMISTRY A. - 1089-5639 .- 1520-5215. ; 128:5, s. 918-928
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Tidskriftsartikel (refereegranskat)abstract
- Formation of oxidized products from Delta(3)-carene (C10H16) ozonolysis and their gas-to-particle partitioning at three temperatures (0, 10, and 20 degrees C) under dry conditions (<2% RH) and also at 10 degrees C under humid (78% RH) conditions were studied using a time-of-flight chemical ionization mass spectrometer (ToF-CIMS) combined with a filter inlet for gases and aerosols (FIGAERO). The Delta(3)-carene ozonolysis products detected by the FIGAERO-ToF-CIMS were dominated by semivolatile organic compounds (SVOCs). The main effect of increasing temperature or RH on the product distribution was an increase in fragmentation of monomer compounds (from C-10 to C-7 compounds), potentially via alkoxy scission losing a C-3 group. The equilibrium partitioning coefficient estimated according to equilibrium partitioning theory shows that the measured SVOC products distribute more into the SOA phase as the temperature decreases from 20 to 10 and 0 degrees C and for most products as the RH increases from <2 to 78%. The temperature dependency of the saturation vapor pressure (above an assumed liquid state), derived from the partitioning method, also allows for a direct way to obtain enthalpy of vaporization for the detected species without accessibility of authentic standards of the pure substances. This method can provide physical properties, beneficial for, e.g., atmospheric modeling, of complex multifunctional oxidation products.
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| 15. |
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| 16. |
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| 17. |
- Quelever, Lauriane L.J., et al.
(författare)
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Effect of temperature on the formation of highly oxygenated organic molecules (HOMs) from alpha-pinene ozonolysis
- 2019
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 19:11, s. 7609-7625
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Tidskriftsartikel (refereegranskat)abstract
- Highly oxygenated organic molecules (HOMs) are important contributors to secondary organic aerosol (SOA) and new-particle formation (NPF) in the boreal atmosphere. This newly discovered class of molecules is efficiently formed from atmospheric oxidation of biogenic volatile organic compounds (VOCs), such as monoterpenes, through a process called autoxidation. This process, in which peroxy-radical intermediates isomerize to allow addition of molecular oxygen, is expected to be highly temperature-dependent. Here, we studied the dynamics of HOM formation during α-pinene ozonolysis experiments performed at three different temperatures, 20, 0 and -15 ĝC, in the Aarhus University Research on Aerosol (AURA) chamber. We found that the HOM formation, under our experimental conditions (50 ppb α-pinene and 100 ppb ozone), decreased considerably at lower temperature, with molar yields dropping by around a factor of 50 when experiments were performed at 0 ĝC, compared to 20 ĝC. At -15 ĝC, the HOM signals were already close to the detection limit of the nitrate-based chemical ionization atmospheric pressure interface time-of-flight (CI-APi-TOF) mass spectrometer used for measuring gas-phase HOMs. Surprisingly, comparing spectra measured at 0 and 20 ĝC, ratios between HOMs of different oxidation levels, e.g., the typical HOM products C10H14O7, C10H14O9, and C10H14O11, changed considerably less than the total HOM yields. More oxidized species have undergone more isomerization steps; yet, at lower temperature, they did not decrease more than the less oxidized species. One possible explanation is that the primary rate-limiting steps forming these HOMs occur before the products become oxygenated enough to be detected by our CI-APi-TOF (i.e., typically seven or more oxygen atoms). The strong temperature dependence of HOM formation was observed under temperatures highly relevant to the boreal forest, but the exact magnitude of this effect in the atmosphere will be much more complex: the fate of peroxy radicals is a competition between autoxidation (influenced by temperature and VOC type) and bimolecular termination pathways (influenced mainly by concentration of reaction partners). While the temperature influence is likely smaller in the boreal atmosphere than in our chamber, both the magnitude and complexity of this effect clearly deserve more consideration in future studies in order to estimate the ultimate role of HOMs on SOA and NPF under different atmospheric conditions.
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| 18. |
- Radoman, Nikola, et al.
(författare)
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Probing the impact of a phytoplankton bloom on the chemistry of nascent sea spray aerosol using high-resolution mass spectrometry
- 2022
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Ingår i: Environmental Science. - : Royal Society of Chemistry (RSC). - 2634-3606. ; 2:5, s. 1152-1169
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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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| 19. |
- Rasmussen, Berit B, et al.
(författare)
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Emissions of ultrafine particles from five types of candles during steady burn conditions
- 2021
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Ingår i: Indoor Air. - : Hindawi Limited. - 0905-6947 .- 1600-0668. ; 31:4, s. 1084-1094
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Tidskriftsartikel (refereegranskat)abstract
- Emissions from candles are of concern for indoor air quality. In this work, five different types of pillar candles were burned under steady burn conditions in a new laboratory scale system for repeatable and controlled comparison of candle emissions (temperature ~25°C, relative humidity ~13%, O2 >18%, air exchange rate 1.9 h-1 ). Burn rate, particle number concentrations, mass concentrations, and mode diameters varied between candle types. Based on the results, the burning period was divided in two phases: initial (0-1 h) and stable (1-6 h). Burn rates were in the range 4.4-7.3 and 4.7-7.1 g/h during initial and stable phase, respectively. Relative particle number emissions, mode diameters, and mass concentrations were higher during the initial phase compared to the stable phase for a majority of the candles. We hypothesize that this is due to elevated emissions of wick additives upon ignition of the candle together with a slightly higher burn rate in the initial phase. Experiments at higher relative humidity (~40%) gave similar results with a tendency toward larger particle sizes at the higher relative humidity. Chemical composition with respect to inorganic salts was similar in the emitted particles (dry conditions) compared to the candlewicks, but with variations between different candles.
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| 20. |
- Rissler, Jenny, et al.
(författare)
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An evaluation and comparison of cloud condensation nucleus activity models: Predicting particle critical saturation from growth at subsaturation
- 2010
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Ingår i: Journal of Geophysical Research. - 2156-2202. ; 115
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Tidskriftsartikel (refereegranskat)abstract
- The ability of particles to activate and form cloud droplets influences the functioning of the Earth's hydrological cycle. This work links the particle water uptake at subsaturation to the critical supersaturation ratio needed for particles to become cloud condensation nuclei (CCN). Five models using the particle hygroscopic growth at subsaturation for predicting the critical supersaturation needed for droplet activation were applied to a laboratory data set of inorganic and organic compounds and mixtures of them. The data set consisted of hygroscopicity tandem differential mobility analyzer measurements and CCN counter measurements. No chemical composition information was used when applying the models. All models tested were based on modifications of Kohler theory and gave similar results. The agreement between predicted and measured critical supersaturations was good, considering the relatively simple models used. A trend of overestimating the critical supersaturations was observed, typically by similar to 15%. The best performing model gave on average only a 4% offset from experimental values; the model with the largest deviation was offset by 20%. A comparison was made between the number of soluble entities (ions or nondissociating molecules) estimated from the particle hygroscopic growth at 90% relative humidity (RH) and the number estimated from the particle critical supersaturation; a similar to 35% increase was observed in the effective number of entities in solution when going from 90% RH to activation. For many types of aerosols, differences in the model approaches tested do not induce large differences in the predicted critical supersaturation. However, it is most important to follow the recommendations published with the respective models and not use them indiscriminately.
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| 21. |
- Rosati, Bernadette, et al.
(författare)
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Hygroscopicity and CCN potential of DMS-derived aerosol particles
- 2022
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Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 22:20, s. 13449-13466
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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.
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| 22. |
- Rosati, Bernadette, et al.
(författare)
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New Particle Formation and Growth from Dimethyl Sulfide Oxidation by Hydroxyl Radicals
- 2021
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Ingår i: ACS Earth and Space Chemistry. - : American Chemical Society (ACS). - 2472-3452. ; 5:4, s. 801-811
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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.
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| 23. |
- Rosati, Bernadette, et al.
(författare)
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The impact of atmospheric oxidation on hygroscopicity and cloud droplet activation of inorganic sea spray aerosol
- 2021
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 11:1
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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.
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| 24. |
- Svenningsson, Birgitta, et al.
(författare)
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Relaxed step functions for evaluation of CCN counter data on size-separated aerosol particles
- 2008
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Ingår i: Journal of Aerosol Science. - : Elsevier BV. - 0021-8502. ; 39:7, s. 592-608
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Tidskriftsartikel (refereegranskat)abstract
- tmospherically important data are gained from cloud condensation nucleus counter (CCNC) analysis of aerosols that are particle mobility separated using differential mobility analysers (I)MA). We present relaxed step functions that can be fitted to these data to obtain critical diameters or critical supersaturations. The step functions are based on the DMA transfer function. We treat the case with fixed supersaturation and varied particle diameter as well as fixed particle size and varied supersaturation. Comparison with experimental data shows that the width of the DMA transfer function controls the steepness of the relaxed step function. The less steep slope in the activation curve caused by the presence of a slightly soluble compound in the particle is discussed. Also in this case, the DMA transfer function width influences the steepness of the activation curve. Finally we demonstrate the errors made if doubly charged particles are not accounted for and a wide DMA transfer function is used.
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| 25. |
- Thomsen, Ditte, et al.
(författare)
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The effect of temperature and relative humidity on secondary organic aerosol formation from ozonolysis of Δ3-carene
- 2024
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Ingår i: Environmental Science: Atmospheres. - 2634-3606. ; 4:1, s. 88-103
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Tidskriftsartikel (refereegranskat)abstract
- This study investigates the effects of temperature and relative humidity (RH) on the formation of secondary organic aerosol (SOA) from Δ3-carene, a prevalent monoterpene in boreal forests. Dark ozonolysis experiments of 10 ppb Δ3-carene were conducted in the Aarhus University Research on Aerosol (AURA) atmospheric simulation chamber at temperatures of 0, 10, and 20 °C. Under dry conditions (RH < 2%), the SOA formation in terms of both particle number and mass concentration shows minimal temperature dependence. This is in contrast to previous findings at higher initial concentrations and suggests an effect of VOC loading for Δ3-carene. Interestingly, the mass fraction of key oxidation products (cis-3-caric acid, cis-3-caronic acid) exhibit a temperature dependence suggesting continuous condensation at lower temperatures, while evaporation and further reactions over time become more favourable at higher temperatures. The oxygen-to-carbon ratios in the particle phase and the occurrence of highly oxygenated organic molecules (HOM) in the gas phase show modest increases with higher temperatures. Predictions from the Aerosol Dynamics and Gas- and Particle-Phase Chemistry Kinetic Multilayer Model (ADCHAM) agrees with the experimental results regarding both physical particle properties and aerosol composition considering the experimental uncertainties. At high RH (∼80%, 10 °C), a considerable increase in the particle nucleation rate and particle number concentration is observed compared to experiments under dry conditions. This is likely due to enhanced particle nucleation resulting from more stable cluster formation of water and inorganics at increased RH. However, RH does not affect the particle mass concentration.
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| 26. |
- Wollesen De Jonge, Robin, et al.
(författare)
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Secondary aerosol formation from dimethyl sulfide-improved mechanistic understanding based on smog chamber experiments and modelling
- 2021
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Ingår i: Atmospheric Chemistry and Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 21:13, s. 9955-9976
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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.
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| 27. |
- Yli-Juuti, Taina, et al.
(författare)
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Volatility of Organic Aerosol : Evaporation of Ammonium Sulfate/Succinic Acid Aqueous Solution Droplets
- 2013
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 47:21, s. 12123-12130
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Tidskriftsartikel (refereegranskat)abstract
- Condensation and evaporation modify the properties and effects of atmospheric aerosol particles. We studied the evaporation of aqueous succinic acid and succinic acid/ammonium sulfate droplets to obtain insights on the effect of ammonium sulfate on the gas/particle partitioning of atmospheric organic acids. Droplet evaporation in a laminar flow tube was measured in a Tandem Differential Mobility Analyzer setup. A wide range of droplet compositions was investigated, and for some of the experiments the composition was tracked using an Aerosol Mass Spectrometer. The measured evaporation was compared to model predictions where the ammonium sulfate was assumed not to directly affect succinic acid evaporation. The model captured the evaporation rates for droplets with large organic content but overestimated the droplet size change when the molar concentration of succinic acid was similar to or lower than that of ammonium sulfate, suggesting that ammonium sulfate enhances the partitioning of dicarboxylic acids to aqueous particles more than currently expected from simple mixture thermodynamics. If extrapolated to the real atmosphere, these results imply enhanced partitioning of secondary organic compounds to particulate phase in environments dominated by inorganic aerosol.
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